Nanocrystalline High-Dimensional Nb2O5 for Efficient Electroreductive Dicarboxylation of CO2 with Cycloalkane
Yuanming Xie, Xinlin Wang, Junjun Mao, Chenchen Zhang, Qingqing Song, Toru Murayama, Mingyue Lin, Jiawei Zhang, Yang Lou, Chengsi Pan, Ying Zhang, Yongfa Zhu
ACS Catalysis, 2024年12月06日
研究論文（学術雑誌）

Preparation and Catalytic Properties of Gold Single‐Atom and Cluster Catalysts Utilizing Nanoparticulate Mg‐Al Layered Double Hydroxides
Tamao Ishida, Akihiro Nakayama, Ayano Yoshida, Chika Aono, Tetsuo Honma, Norihito Sakaguchi, Ayako Taketoshi, Takashi Fujita, Toru Murayama, Tetsuya Shimada, Shinsuke Takagi
ChemPlusChem, Wiley, 2024年10月11日
研究論文（学術雑誌）, Au single atoms and clusters were stabilized on Mg‐Al layered double hydroxide nanoparticles (LDH NPs), and the obtained Au@LDH NPs were supported on SiO2 and CeO2. After hydrogen reduction, Au single atoms were found together with Au clusters on LDH/SiO2. In contrast to Au single‐atom catalysts which are deposited in metal vacancies of oxide supports, the LDH NPs stabilize small Au species despite the absence of metal vacancies. The obtained Au(0)@LDH/SiO2 catalyzed aerobic oxidation of alcohols, and Au single atoms maintained after the reaction. Given that only Au NPs were observed on bulk LDH, the abundant surface OH group of LDH NPs would contribute to stabilize Au, resulting in higher activity than Au/LDH‐bulk. After calcination to transform LDH to mixed metal oxide (MMO), the obtained Au(0)@MMO/SiO2 also exhibited high catalytic activity. Moreover, Au(0)@LDH/CeO2 exhibited higher activity and excellent selectivity for hydrogenation of 4‐nitrostyrene to 4‐aminostyrene than conventional Au catalysts such as Au/CeO2 and Au/TiO2 even though only Au NPs were present. We demonstrated that Au size can be minimized using LDH NPs, exhibiting in high catalytic performance. The basic surface OH groups of LDH would be also beneficial for deprotonation of alcohols and heterolytic H2 dissociation in the catalytic reactions.

CO Oxidation at Low Temperatures over the Au Cluster Supported on Crystalline Silicotitanate
Miyu Muraoka, Takuto Miyatani, Akihiro Sembuku, Tamao Ishida, Toru Murayama, Yoshihiro Kubota, Satoshi Inagaki
ACS Omega, 2024年10月08日
研究論文（学術雑誌）

Theoretical investigation of CO oxidation over polyoxometalate-supported Au cluster catalyst
Tomohisa Yonemori, Yasutaka Hamada, Tamao Ishida, Toru Murayama, Takashi Kawakami, Shusuke Yamanaka, Mitsutaka Okumura
Journal of Catalysis, 438, 2024年10月
研究論文（学術雑誌）, A polyoxometalate-supported Au cluster catalyst (Au/POM) exhibited high catalytic activity for CO oxidation at room temperature; however, its activity decreased at the reaction temperature above 60 ℃. Density functional theory calculations were performed to elucidate the unique catalytic activities. Our calculations show that the interactions between water molecules accommodated within the defect site of the support and the O2 adsorbed on the Au cluster generate active OOH− species. This OOH− species reacts readily with CO, resulting in high CO oxidation catalytic activity between −40 and 40 degrees Celsius. The activation barrier of CO oxidation over Au/POM in the presence of H2O is much lower than that in the absence of H2O. This is in good agreement with the experimental results, indicating that surface-adsorbed water allows for high CO oxidation catalytic activity around room temperature, whereas the activity decreases at higher temperatures owing to the desorption of surface-adsorbed water molecules.

High-Dimensional Nb2O5 with NbO6 Octahedra for Efficient Electrocatalytic Upgrading of Methanol to Formate
Xinlin Wang, Chuqian Xiao, Yuanming Xie, Chunqi Yang, Yuhang Li, Ying Zhang, Toru Murayama, Tamao Ishida, Mingyue Lin, Guangli Xiu
ACS Applied Materials & Interfaces, 2024年08月28日
研究論文（学術雑誌）

Efficient formation of propylene oxide under low hydrogen concentration in propylene epoxidation over Au nanoparticles supported on V-doped TS-1
Caixia Qi, Yanan Cheng, Zixuan Yang, Tamao Ishida, Huijuan Su, Jingzhou Zhang, Xun Sun, Libo Sun, Lijun Zhao, Toru Murayama
Journal of Catalysis, 436, 2024年08月
研究論文（学術雑誌）, The direct epoxidation of propylene to propylene oxide (PO) represents a unique feature of gold nanoparticle catalysts. Different amounts of vanadium were introduced into TS-1 using a hydrothermal method to give V-TS-1, and the effect of various vanadium loadings on the catalytic performance of Au/V-TS-1 was investigated in the epoxidation of propylene under different reaction conditions. The obtained characterization results indicate that the molecular sieve pore structure and crystalline phase structure of TS-1 were maintained after vanadium incorporation, and vanadium was incorporated into the molecular sieve framework. The introduction of an appropriate amount of vanadium resulted in the homogeneous dispersion of gold particles with a small average particle size, which facilitated the epoxidation reaction. When V was introduced into TS-1, the propylene conversion decreased under the condition of 10 % H2 concentration (C3H6/H2 = 1/1) in the reaction atmosphere, but the PO selectivity was maintained. Interestingly, when the H2 concentration in the reaction atmosphere was lowered to 2 % (C3H6/H2 = 3/1), the propylene conversion in Au/TS-1 was significantly decreased compared to 10 % H2 concentration condition, while in Au/V-TS-1, the propylene conversion was maintained in 2 % H2 concentration condition compared to 10 % H2. Au/V-TS-1 also maintained its selectivity for PO even when the H2 concentration was lowered. Therefore, under low hydrogen concentration conditions, the PO formation rate of Au/V-TS-1 was much higher than that of Au/TS-1. More, the same trend was observed when Mo was added in place of V. Our strategy will guide the design of future catalysts as a way to utilize hydrogen more effectively while maintaining PO productivity.

Ring–Opening Mechanism of O-heterocycles into α,ω-Diols over Ni−La(OH)3: C−O Bond Hydrogenolysis of THFA to 1,5-Pentanediol as a Case Study
Mohammed Al-Yusufi, Dirk Michalik, Christoph Kubis, Toru Murayama, Tamao Ishida, Ali M. Abdel-Mageed, Angela Köckritz
ChemCatChem, 16, 13, 2024年07月08日
研究論文（学術雑誌）, The elucidation of the ring–opening reaction mechanism is a critical step towards improving the catalytic performance for the conversion of biomass into value–added chemicals. Herein, we focused on the stepwise C−O bond hydrogenolysis mechanism of oxygen–containing heterocycles (O-heterocycles) into α,ω-diols, in particular THFA to 1,5-PeD, over selective Ni−La(OH)3 in hydrogen–donor isopropanol. A mechanistic study was carried out on a structurally well–defined Ni−La(OH)3, where the mechanism was elucidated using a combination of kinetic and 13C NMR isotope labeling experiments. It was suggested that both Ni nanoparticles and La(OH)3 support play a critical role in the reaction mechanism, where basic hydroxide species of the support initially deprotonate the CH2OH and −OH modified furan, tetrahydrofuran and tetrahydropyran rings, adsorbing them chemically on the catalyst surface. This step is followed by a direct hydride attack on the second carbon atom of these rings, which is proposed to be the key step for ring cleavage, as indicated by the increased deuteration at this position. In addition to the direct hydrogenolysis using gaseous H2, it is assumed that a catalytic transfer hydrogenolysis reaction (CTH) reaction of THFA is proposed to proceed via the dehydrogenation of isopropanol over isolated Ni species, forming hydrogen species that can be adsorbed on the Ni surface or desorb as H2 molecules.

In situ/operando spectroscopic evidence on associative redox mechanism for periodic unsteady-state water–gas shift reaction on Au/CeO2 catalyst
Ningqiang Zhang, Lingcong Li, Yuan Jing, Yucheng Qian, Duotian Chen, Nobutaka Maeda, Toru Murayama, Takashi Toyao, Ken-ichi Shimizu
Journal of Catalysis, 433, 115500, 115500, Elsevier BV, 2024年05月
研究論文（学術雑誌）

Highly Active and Sintering-Resistant Pt Clusters Supported on FeOx–Hydroxyapatite Achieved by Tailoring Strong Metal–Support Interactions
Yunxia Liu, Guandong Wu, Rile Ge, Xunzhu Jiang, Lin Li, Tamao Ishida, Toru Murayama, Botao Qiao, Junhu Wang
ACS Applied Materials & Interfaces, 16, 17, 22007, 22015, 2024年05月01日, ［国際誌］
英語, 研究論文（学術雑誌）, The catalytic performance of supported metal catalysts is closely related to their structure. While Pt-based catalysts are widely used in many catalytic reactions because of their exceptional intrinsic activity, they tend to deactivate in high-temperature reactions, requiring a tedious and expensive regeneration process. The strong metal-support interaction (SMSI) is a promising strategy to improve the stability of supported metal nanoparticles, but often at the price of the activity due to either the coverage of the active sites by support overlay and/or the too-strong metal-support bonding. Herein, we newly constructed a supported Pt cluster catalyst by introducing FeOx into hydroxyapatite (HAP) support to fine-tune the SMSIs. The catalyst exhibited not only high catalytic activity but also sintering resistance, without deactivation in a 100 h test for catalytic CO oxidation. Detailed characterizations reveal that FeOx introduced into HAP weaken the strong covalent metal-support interaction (CMSI) between Pt and FeOx while simultaneously inhibiting the oxidative strong metal-support interaction (OMSI) between Pt and HAP, giving rise to both high activity and thermal stability of the supported Pt clusters.

The Development of the Regenerable Catalytic System in Selective Catalytic Oxidation of Ammonia with High N2 Selectivity
Haifeng Wang, Toru Murayama, Tamao Ishida, Ken-ichi Shimizu, Norihito Sakaguchi, Kazuya Yamaguchi, Hiroki Miura, Tetsuya Shishido
ACS Applied Materials & Interfaces, 16, 15, 18693, 18702, 2024年04月17日, ［国際誌］
英語, 研究論文（学術雑誌）, Supported particulate noble-metal catalysts are widely used in industrial catalytic reactions. However, these metal species, whether in the form of nanoparticles or highly dispersed entities, tend to aggregate during reactions, leading to a reduced activity or selectivity. Addressing the frequent necessity for the replacement of industrial catalysts remains a significant challenge. Herein, we demonstrate the feasibility of the 'regenerable catalytic system' exemplified by selective catalytic oxidation of ammonia (NH3-SCO) employing Ag/Al2O3 catalysts. Results demonstrate that our highly dispersed Ag catalyst (Ag HD) maintains >90% N2 selectivity at 80% NH3 conversion and >80% N2 selectivity at 100% NH3 conversion after enduring 5 cycles of reducible aggregation and oxidative dispersion. Moreover, it consistently upholds over 98% N2 selectivity at 100% NH3 conversion after 10 cycles of Ar treatment. During the aggregation-dispersion process, the Ag HD catalyst intentionally aggregated into Ag nanoparticles (Ag NP) after H2 reduction and exhibited remarkable regenerable capabilities, returning to the Ag HD state after calcination in the air. This structural evolution was characterized through in situ transmission electron microscopy, atomically resolved high-angle annular dark-field scanning transmission electron microscopy, and X-ray absorption spectroscopy, revealing the on-site oxidative dispersion of Ag NP. Additionally, in situ diffuse reflectance infrared Fourier transform spectroscopy provided insights into the exceptional N2 selectivity on Ag HD catalysts, elucidating the critical role of NO+ intermediates. Our findings suggest a sustainable and cost-effective solution for various industry applications.

Manipulation of the electronic state of Au to boost the catalytic efficiency of Au/polyaniline by doping engineering
Libo Sun, Heshun Jing, Shuo Zhou, Wenyu Tan, Xinyuan Ren, Miao Zhang, Xun Sun, Haifeng Wang, Toru Murayama, Caixia Qi
Molecular Catalysis, 2024年03月
研究論文（学術雑誌）

Decoration of Gold and Platinum Nanoparticle Catalysts by 1 nm Thick Metal Oxide Overlayer and Its Effect on the CO Oxidation Activity
Kaho Okayama, Akihiro Nakayama, Toru Murayama, Norihito Sakaguchi, Feng Hong, Botao Qiao, Junhu Wang, Tetsuya Shimada, Shinsuke Takagi, Tamao Ishida
ACS Applied Materials & Interfaces, 16, 4, 4570, 4580, American Chemical Society (ACS), 2024年01月19日, ［国際誌］
英語, 研究論文（学術雑誌）, Exfoliated M-Al layered double hydroxide (M-Al LDH; M = Mg, Co, Ni, and Zn) nanosheets were adsorbed on Au/SiO2 and calcined to transform LDH into mixed metal oxides (MMOs) and yield Au/SiO2 coated with a thin MMO overlayer. These catalysts showed a higher catalytic activity than pristine Au/SiO2. In particular, the 50% CO conversion temperature decreased by more than 250 °C for Co-Al MMO-coated Au/SiO2. In contrast, the deposition of CoAlOx on Au/SiO2 by impregnation or the deposition of Au on Co-Al MMO-coated SiO2 resulted in a worse catalytic activity. Moreover, the presence of a thick MMO overlayer decreased the catalytic activity, suggesting that the control of the overlayer thickness to less than 1 nm is a requisite for obtaining a high catalytic activity. Moreover, the thin Co-Al MMO overlayer on Au/SiO2 possessed abundant oxygen vacancies, which would play an important role in O2 activation, resulting in a highly active interface between Au and the defect-rich MMO on the Au NP surface. Finally, this can be applied to Pt/SiO2, and the obtained Co-Al MMO-coated Pt/SiO2 also exhibited a much improved catalytic activity for CO oxidation.

Role of the heptagonal channel of crystalline Mo3VOx catalyst for the selective oxidation of acrolein and methacrolein
Satoshi Ishikawa, Nagisa Noda, Kosuke Shimoda, Toru Murayama, Wataru Ueda
Catalysis Science & Technology, 2024年
研究論文（学術雑誌）

Prolonging the n-type conduction of thermoelectric carbon nanotubes exposed to warm air by mixing hydrated water into the adsorbed dopant layers composed of Li⁺-receptor molecules
Shinichi Hata, Chika Nakagawa, Ayako Taketoshi, Toru Murayama, Tamao Ishida, Yukou Du, Yukihide Shiraishi, Naoki Toshima
RSC Applied Interfaces, Royal Society of Chemistry (RSC), 2024年
研究論文（学術雑誌）, The n-type properties of carbon nanotubes are stabilized in the ambient atmosphere by hydrated water on a cationic molecular adsorption layer supplemented with Li⁺, which slows the diffusion of thermally active oxygen molecules.

Niedrige Temperatur Hydrierung von CO2 zu Methanol in Wasser auf ZnO‐geträgerten CuAu‐Nanolegierungen
Jawaher Mosrati, Tamao Ishida, Hung Mac, Mohammed Al‐Yusufi, Tetsuo Honma, Magdalena Parliniska‐Wojtan, Yasuhiro Kobayashi, Alexander Klyushin, Toru Murayama, Ali M. Abdel‐Mageed
Angewandte Chemie, 2023年12月18日
研究論文（学術雑誌）

Low‐Temperature Hydrogenation of CO2 to Methanol in Water on ZnO‐Supported CuAu Nanoalloys
Jawaher Mosrati, Tamao Ishida, Hung Mac, Mohammed Al‐Yusufi, Tetsuo Honma, Magdalena Parliniska‐Wojtan, Yasuhiro Kobayashi, Alexander Klyushin, Toru Murayama, Ali M. Abdel‐Mageed
Angewandte Chemie International Edition, 62, 51, e202311340, 2023年12月18日, ［国際誌］
英語, 研究論文（学術雑誌）, Optimizing processes and materials for the valorization of CO2 to hydrogen carriers or platform chemicals is a key step for mitigating global warming and for the sustainable use of renewables. We report here on the hydrogenation of CO2 in water on ZnO-supported CuAu nanoalloys, based on ≤7 mol % Au. Cux Auy /ZnO catalysts were characterized using 197 Au Mössbauer, in situ X-ray absorption (Au LIII - and Cu K-edges), and ambient pressure X-ray photoelectron (APXP) spectroscopic methods together with X-ray diffraction and high-resolution electron microscopy. At 200 °C, the conversion of CO2 showed a significant increase by 34 times (from 0.1 to 3.4 %) upon increasing Cu93 Au7 loading from 1 to 10 wt %, while maintaining methanol selectivity at 100 %. Limited CO selectivity (4-6 %) was observed upon increasing temperature up to 240 °C but associated with a ≈3-fold increase in CO2 conversion. Based on APXPS during CO2 hydrogenation in an H2 O-rich mixture, Cu segregates preferentially to the surface in a mainly metallic state, while slightly charged Au submerges deeper into the subsurface region. These results and detailed structural analyses are topics of the present contribution.

Dual-core drive hydrogen transfer heterogeneous catalysts based on iridium-enzyme co-modified carbon nanotubes for aromatic aldehyde hydrogenation
Li-Jun Zhao, Caimei Zhang, Shixin Zhang, Jiayang Chen, Xiaoyi Lv, Huijuan Su, Xun Sun, Toru Murayama, Caixia Qi
Journal of Catalysis, 2023年12月
研究論文（学術雑誌）

High Selectivity Cofactor NADH Regeneration Organic Iridium Complexes Used for High-Efficiency Chem-Enzyme Cascade Catalytic Hydrogen Transfer
Li-Jun Zhao, Caimei Zhang, Shixin Zhang, Xiaoyi Lv, Jiayang Chen, Xun Sun, Huijuan Su, Toru Murayama, Caixia Qi
Inorganic Chemistry, 62, 43, 17577, 17582, 2023年10月30日, ［国際誌］
英語, 研究論文（学術雑誌）, Our research demonstrated that novel pentamethylcyclopentadienyl (Cp*) iridium pyridine sulfonamide complex PySO2NPh-Ir (7) could highly specifically catalyze nicotinamide adenine dinucleotide (NAD+) into the corresponding reducing cofactor NADH in cell growth media containing various biomolecules. The structures and catalytic mechanism of 7 were studied by single-crystal X-ray, NMR, electrochemical, and kinetic methods, and the formation of iridium hydride species Ir-H was confirmed to be the plausible hydride-transfer intermediate of 7. Moreover, benefiting from its high hydrogen-transfer activity and selectivity for NADH regeneration, 7 was used as an optimal metal catalyst to establish a chem-enzyme cascade catalytic hydrogen-transfer system, which realized the high-efficiency preparation of l-glutamic acid by combining with l-glutamate dehydrogenase (GLDH).

In-situ Raman unveiled Nb-O-bond-dependency selectivity for methanol electro-oxidation at high current density
Xinlin Wang, Chuqian Xiao, Yuhang Li, Toru Murayama, Tamao Ishida, Mingyue Lin, Guangli Xiu
Applied Catalysis A: General, 2023年08月
研究論文（学術雑誌）

Au Clusters Supported on Defect-Rich Ni-Ti Oxides Derived from Ultrafine Layered Double Hydroxides (LDHs) for CO Oxidation at Ambient Temperature
Ayu Takahashi, Akihiro Nakayama, Toru Murayama, Norihito Sakaguchi, Tetsuya Shimada, Shinsuke Takagi, Tamao Ishida
Catalysts, 13, 8, 1155, 1155, MDPI AG, 2023年07月26日
研究論文（学術雑誌）, Ultrafine layered double hydroxides (LDHs) have abundant hydroxy groups at their edge sites, serving as anchor sites for metal NPs. Furthermore, transformation of ultrafine LDHs into mixed metal oxides (MMOs) generates abundant oxygen vacancies, which are advantageous for O2 activation during Au-catalyzed CO oxidation. We used ultrafine Ni-Ti LDHs with low crystallinity or Ni-Ti MMOs supported on SiO2 onto which Au NPs were deposited by deposition–precipitation (DP) and DP–urea (DPU). The catalytic activity of the Au catalysts was significantly affected by the preparation method, with the highest activity obtained by depositing Au onto LDH/SiO2 by DPU, followed by transformation of LDH to MMO (Au/Ni-Ti MMO/SiO2 (LDH-DPU)). The presence of Au on LDHs affected the transformation of LDHs into MMOs, resulting in LDH-DPU having the greatest number of oxygen vacancies in the TiO2 domain in MMOs. Consequently, the adsorbed or the lattice oxygen on the surface of LDH-DPU can be easily utilized for CO oxidation at low temperatures. Moreover, the catalytic activity of LDH-DPU increased with water vapor concentration up to 100% relative humidity at room temperature, suggesting the potential of Au/Ni-Ti MMO/SiO2 as an air purification catalyst.

Metal–Support Interaction in Gold Zeolitic Octahedral Metal Oxide and the Catalytic Activity for Low-Temperature Alcohol Oxidation
Yukang Wang, Guijin Zheng, Qianqian Zhu, Qiangqiang Tong, Bolun Yu, Tamao Ishida, Toru Murayama, Yanshuo Li, Wataru Ueda, Zhenxin Zhang
Langmuir, 39, 29, 10163, 10177, 2023年07月25日, ［国際誌］
英語, 研究論文（学術雑誌）, Au nanoparticles are efficient catalysts for selective oxidations. The interaction between Au nanoparticles and supports is critical for achieving high catalytic activity. Herein, Au nanoparticles are supported on a zeolitic octahedral metal oxide based on Mo and V. The charge of Au is controlled by the surface oxygen vacancies of the supports, and the redox property of the zeolitic vanadomolybdate is highly dependent on Au loading. The Au-supported zeolitic vanadomolybdate is used as a heterogeneous catalyst for alcohol oxidation under mild conditions with molecular oxygen as an oxidant. The supported Au catalyst can be recovered and reused without the loss of activity.

Gold/Substituted Hydroxyapatites for Oxidative Esterification: Control of Thin Apatite Layer on Gold Based on Strong Metal-Support Interaction (SMSI) Results in High Activity.
Ayako Taketoshi, Yuvaraj Gangarajula, Ryusei Sodenaga, Akihiro Nakayama, Mitsutaka Okumura, Norihito Sakaguchi, Toru Murayama, Tetsuya Shimada, Shinsuke Takagi, Masatake Haruta, Botao Qiao, Junhu Wang, Tamao Ishida
ACS applied materials & interfaces, 15, 28, 34290, 34302, 2023年07月19日, ［国際誌］
英語, 研究論文（学術雑誌）, Gold nanoparticles (Au NPs) deposited on various cation- and anion-substituted hydroxyapatites (Au/sHAPs) show oxidative strong metal-support interaction (SMSI), wherein a thin layer of the sHAP covered the surface of the Au NPs by heat treatment in an oxidative atmosphere. Calcination of Au/sHAPs at 300 °C caused a partial SMSI and that at 500 °C gave fully encapsulated Au NPs. We investigated the influence of the substituted ions in sHAP and the degree of the oxidative SMSI on the catalytic performance of Au/sHAPs for oxidative esterification of octanal or 1-octanol with ethanol to obtain ethyl octanoate. The catalytic activity depends on the size of the Au NPs but not on the support used, owing to the similarity of the acid and base properties of sHAPs except for Au/CaFAP. The presence of a large number of acidic sites on CaFAP lowered the product selectivity, but all other sHAPs exhibited similar activity when the Au particle size was almost the same, owing to the similarity of the acid and base properties. Au/sHAPs_O2 with SMSI exhibited higher catalytic activity than Au/sHAPs_H2 without SMSI despite the fact that the number of exposed surface Au atoms was decreased by the SMSI. In addition, the oxidative esterification reaction proceeded even though the Au NPs were fully covered by the sHAP layer when the thickness of the layer was controlled to be less than 1 nm. The substrate can access the surfaces of the Au NPs covered by the thin sHAP layer (<1 nm), and the presence of the sHAP structure in close contact with the Au NPs resulted in significantly higher catalytic activity compared with that for fully exposed Au NPs deposited on the sHAPs. This result suggests that maximizing the contact area between the Au NPs and the sHAP support based on the SMSI enhances the catalytic activity of Au.

Sodium ion intercalation in vanadium oxide promotes low-temperature NH3-SCR activity: Sodium vanadium bronzes (Na0.33V2O5) for NOx removal
Yusuke Inomata, Hiroe Kubota, Yoshinori Honmatsu, Hiroaki Takamitsu, Sosuke Sakotami, Kazuhiro Yoshida, Takashi Toyao, Ken-ichi Shimizu, Toru Murayama
APPLIED CATALYSIS B-ENVIRONMENTAL, 328, ELSEVIER, 2023年07月
英語, 研究論文（学術雑誌）, NH3-SCR (selective catalytic reduction) is a key technique for converting harmful NOx to harmless N2 and H2O in exhaust gases. Herein, V2O5, Na0.33V2O5 and Na1.2V3O8 are synthesized by a simple chemical process (the oxalate method) as examples of Na-intercalated vanadium oxide (sodium vanadium oxide bronze) for low-temperature NH3-SCR less than 150 degrees C. Among them, Na0.33V2O5 shows 92% (dry) and 86% (in the presence of 10 vol% water) NO conversions at 150 degrees C. The reaction rate of Na0.33V2O5 is 6.1-times higher than that of V2O5, indi-cating that Na intercalation accelerates NH3-SCR cycles. Mechanistic analysis suggests that the reaction mech-anism of Na0.33V2O5 is different from those of other V-based catalysts. Although it has been believed that alkali ions inhibit catalytic cycles of NH3-SCR, the results of this study suggest that alkali ions affect the structural, redox and adsorption properties of bulk V2O5, leading to an increase in NH3-SCR activity.

Selective formation of acetate intermediate prolongs robust ethylene removal at 0 degrees C for 15 days
Mingyue Lin, Haifeng Wang, Takashi Takei, Hiroki Miura, Tetsuya Shishido, Yuhang Li, Jinneng Hu, Yusuke Inomata, Tamao Ishida, Masatake Haruta, Guangli Xiu, Toru Murayama
NATURE COMMUNICATIONS, 14, 1, 2885, 2885, NATURE PORTFOLIO, 2023年05月20日, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, Efficient ethylene removal below room temperatures is of great importance to food transportation and storage. Here the authors have developed an efficient gold-platinum nanoalloy catalyst for trace ethylene removal at 0 degrees C for 15 days.Efficient ethylene (C2H4) removal below room temperatures, especially near 0 degrees C, is of great importance to suppress that the vegetables and fruits spoil during cold-chain transportation and storage. However, no catalysts have been developed to fulfill the longer-than-2-h C2H4 removal at this low temperature effectively. Here we prepare gold-platinum (Au-Pt) nanoalloy catalysts that show robust C2H4 (of 50 ppm) removal capacity at 0 degrees C for 15 days (360 h). We find, by virtue of operando Fourier transformed infrared spectroscopy and online temperature-programmed desorption equipped mass spectrometry, that the Au-Pt nanoalloys favor the formation of acetate from selective C2H4 oxidation. And this on-site-formed acetate intermediate would partially cover the catalyst surface at 0 degrees C, thus exposing active sites to prolong the continuous and effective C2H4 removal. We also demonstrate, by heat treatment, that the performance of the used catalysts will be fully recovered for at least two times.

Long-Alkyl-Chain Phosphonium Surfactant Molecular Wrapping to Block Oxygen Impurities in n-Type Carbon Nanotubes for Thermoelectric Applications
Shinichi Hata, Fumiya Kitano, Hiroki Ihara, Toru Murayama, Yukou Du, Yukihide Shiraishi, Naoki Toshima
ACS Applied Engineering Materials, American Chemical Society (ACS), 2023年02月23日
研究論文（学術雑誌）

Pd-Rh Alloyed Nanoparticles on Zeolite Imidazolide Framework-67 for Methyl Orange Degradation
Shinichi Hata, Yuki Sakai, Nanami Tani, Sho Kitano, Hiroki Habazaki, Akari Hirakawa, Hinako Tanaka, Yusuke Inomata, Toru Murayama, Masatake Haruta, Yukou Du, Yukihide Shiraishi, Naoki Toshima
ACS Applied Nano Materials, 5, 11, 16231, 16241, 2022年11月25日
研究論文（学術雑誌）, Bimetallic or alloyed nanoparticles (NPs) are important materials that often exhibit chemical properties different from those of their monometallic counterparts. However, access to uniformly alloyed bimetallic particles, particularly in the Pd-Rh system, is difficult because of the thermodynamic immiscibility of the individual metals. Herein, we propose a method for accumulating Pd-Rh alloy particles on the surface of zeolite imidazolide framework-67 (ZIF-67), a chemically stable metal-organic framework, under mild conditions at 25 °C. The degradation of methyl orange was used to test the applicability of the resultant material as a heterogeneous catalyst. A turnover frequency of 38.5 h-1 was recorded for Pd0.12Rh0.88/ZIF-67, which is higher than that of catalysts with either Pd (17.2 h-1) or Rh (16.5 h-1). The acceleration of methyl orange decomposition was attributed to electron transfer from Pd to Rh in the alloy particles due to the differences in Pauling electronegativity and an increase in metallic Rh on the catalyst surface. No metal leakage or structural degradation of the ZIF-67 support was observed during the catalytic reaction. Pd0.12Rh0.88/ZIF-67 could actively degrade methyl orange, congo red, and methylene blue. The structure of the catalyst remained intact even when a mixed solution of all three dyes was circulated for 60 min in a fixed-bed system, and the catalyst conversion rate exceeded 99.7%. Our results collectively demonstrate the successful preparation of Pd-Rh-supported catalysts and their application to the continuous reduction of multicomponent dye mixtures. The metal NP-MOF composites prepared using the proposed approach are free from MOF pore damage and can maintain their specific surface area. Therefore, this strategy could give impetus to research on catalytic applications of NP-MOF composites.

Obituary for Masatake Haruta (1947–2022)
Toru Murayama, Tamao Ishida
Gold Bulletin, 2022年10月
研究論文（学術雑誌）

Enhancement effect of strong metal-support interaction (SMSI) on the catalytic activity of substituted-hydroxyapatite supported Au clusters
Akihiro Nakayama, Ryusei Sodenaga, Yuvaraj Gangarajula, Ayako Taketoshi, Toru Murayama, Tetsuo Honma, Norihito Sakaguchi, Tetsuya Shimada, Shinsuke Takagi, Masatake Haruta, Botao Qiao, Junhu Wang, Tamao Ishida
Journal of Catalysis, 410, 194, 205, Elsevier BV, 2022年06月
研究論文（学術雑誌）

Understanding the Distinct Effects of Ag Nanoparticles and Highly Dispersed Ag Species on N₂ Selectivity in NH₃–SCO Reaction
Haifeng Wang, Toru Murayama, Mingyue Lin, Norihito Sakaguchi, Masatake Haruta, Hiroki Miura, Tetsuya Shishido
ACS Catalysis, 6108, 6118, American Chemical Society (ACS), 2022年05月09日
研究論文（学術雑誌）

Defective NiO as a Stabilizer for Au Single-Atom Catalysts
Chihiro Mochizuki, Yusuke Inomata, Shunsaku Yasumura, Mingyue Lin, Ayako Taketoshi, Tetsuo Honma, Norihito Sakaguchi, Masatake Haruta, Ken-ichi Shimizu, Tamao Ishida, Toru Murayama
ACS Catalysis, 6149, 6158, American Chemical Society (ACS), 2022年05月09日
研究論文（学術雑誌）

Effect of poly(N-vinylpyrrolidone) ligand on catalytic activities of Au nanoparticles supported on Nb2O5 for CO oxidation and furfural oxidation
Mingyue Lin, Chihiro Mochizuki, Tamao Ishida, Ying Zhang, Masatake Haruta, Toru Murayama
Catalysis Today, Elsevier BV, 2022年04月
研究論文（学術雑誌）

Efficient non-volatile organogold complex for TiO2-supported gold cluster catalysts: Preparation and catalytic activity for CO oxidation
Luong Xuan Dien, Toru Murayama, Nguyen Tuan Hung, Quang Duc Truong, Huynh Dang Chinh, Masamichi Yoshimura, Masatake Haruta, Tamao Ishida
Journal of Catalysis, 408, 236, 244, 2022年04月
研究論文（学術雑誌）, Gold nanoparticles supported on titania (Au/TiO2) catalysts were prepared by solid grinding (SG) method using a halide-free nonvolatile organogold complex, bis(phenyl)boroxinato(4-tolylpyridyl)gold(III), abbreviated as AuBO, followed by calcination. Density functional theory (DFT) calculation revealed that AuBO was adsorbed on TiO2 by hydrogen bonding with the surface hydroxy group of TiO2 and that the adsorption energy was lower than those of other gold precursors. The obtained catalyst (AuBO/TiO2) showed higher catalytic activity for CO oxidation than did Au/TiO2 prepared by conventional deposition–precipitation method and by SG using other organogold complexes. Furthermore, grinding of the gold precursor with potassium tert-butoxide followed by calcination (AuBO/K-TiO2) improved the catalytic activity and 100% CO conversion reached at − 23 °C (temperature at which 50% CO conversion occurs, T1/2 = − 39 °C) as compared to AuBO/TiO2 (T1/2 = − 28 °C). Potassium tert-butoxide facilitated the decomposition of AuBO adsorbed on TiO2, and increased surface basicity contributed to the improved catalytic activity. AuBO/K-TiO2 also exhibited high catalyst stability for CO oxidation at room temperature.

Transesterification of Ethyl-10-undecenoate Using a Cu-Deposited V2O5 Catalyst as a Model Reaction for Efficient Conversion of Plant Oils to Monomers and Fine Chemicals
Swetha Sudhakaran, Ayako Taketoshi, S. M. A. Hakim Siddiki, Toru Murayama, Kotohiro Nomura
ACS Omega, 7, 5, 4372, 4380, American Chemical Society ({ACS}), 2022年02月08日, ［国際誌］
英語, 研究論文（学術雑誌）, Transesterification of ethyl-10-undecenoate (derived from castor oil) with 1,4-cyclohexanedimethanol over a recyclable Cu-deposited V2O5 catalyst afforded 1,ω-diene, the corresponding cyclohexane-1,4-diylbis(methylene) bis(undec-10-enoate), a promising monomer for the synthesis of biobased polyesters, in an efficient manner. Deposition of Cu plays an important role in proceeding the reaction with high selectivity, and both the activity and the selectivity are preserved for five recycled runs by the addition of the substrates. The present catalyst was effective for transesterification with other alcohols, especially primary alcohols, demonstrating a possibility of using this catalyst for efficient conversion of plant oil to various fine chemicals.

Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides
Weixuan Zhao, Junjie Shi, Mingyue Lin, Libo Sun, Huijuan Su, Xun Sun, Toru Murayama, Caixia Qi
RSC Advances, 12, 9, 5374, 5385, 2022年, ［国際誌］
英語, 研究論文（学術雑誌）, Modulating the active sites for controllable tuning of the catalytic activity has been the goal of much research, however, this remains challenging. The O vacancy is well known as an active site in reducible oxides. To modify the activity of O vacancies in praseodymia, we synthesized a series of praseodymia-titania mixed oxides. Varying the Pr : Ti mole ratio (2 : 1, 1 : 2, 1 : 1, 1 : 4) allows us to control the electronic interactions between Au, Pr and Ti cations and the local chemical environment of the O vacancies. These effects have been studied study by X-ray photoelectron spectroscopy (XPS), CO diffuse reflectance Fourier transform infrared spectroscopy (CO-DRIFTS) and temperature-programmed reduction (CO-TPR, H2-TPR). The water gas shift reaction (WGSR) was used as a benchmark reaction to test the catalytic performance of different praseodymia-titania supported Au. Among them, Au/Pr1Ti2O x was identified to exhibit the highest activity, with a CO conversion of 75% at 300 °C, which is about 3.7 times that of Au/TiO2 and Au/PrO x . The Au/Pr1Ti2O x also exhibited excellent stability, with the conversion after 40 h time-on-stream at 300 °C still being 67%. An optimal ratio of Pr content (Pr : Ti 1 : 2) is necessary for improving the surface oxygen mobility and oxygen exchange capability, a higher Pr content leads to more O vacancies, however with lower activity. This study presents a new route for modulating the active defect sites in mixed oxides which could also be extended to other heterogeneous catalysis systems.

Anti-inflammatory effect of gold nanoparticles supported on metal oxides
Takashi Fujita, Maeva Zysman, Dan Elgrabli, Toru Murayama, Masatake Haruta, Sophie Lanone, Tamao Ishida, Jorge Boczkowski
Scientific Reports, 11, 1, 23129, 23129, Springer Science and Business Media LLC, 2021年12月, ［国際誌］
英語, 研究論文（学術雑誌）, Gold (Au) can be deposited as nanoparticles (NPs) smaller than 10 nm in diameter on a variety of metal oxide (MOx) NPs. Au/MOx have high catalytic performance and selective oxidation capacity which could have implications in terms of biological activity, and more specifically in modulation of the inflammatory reaction. Therefore, the aim of this study was to examine the effect of Au/TiO₂, Au/ZrO₂ and Au/CeO₂ on viability, phagocytic capacity and inflammatory profile (TNF-α and IL-1β secretion) of murine macrophages. The most important result of this study is an anti-inflammatory effect of Au/MOx depending on the MOx nature with particle internalization and no alteration of cell viability and phagocytosis. The effect was dependent on the MOx NPs chemical nature (Au/TiO₂ > Au/ZrO₂ > Au/CeO₂ if we consider the number of cytokines whose concentration was reduced by the NPs), and on the inflammatory mediator considered. The effect of Au/TiO₂ NPs was not related to Au NPs size (at least in the case of Au/TiO₂ NPs in the range of 3–8 nm). To the best of our knowledge, this is the first demonstration of an anti-inflammatory effect of Au/MOx.

Bulk tungsten-substituted vanadium oxide for low-temperature NOx removal in the presence of water
Yusuke Inomata, Hiroe Kubota, Shinichi Hata, Eiji Kiyonaga, Keiichiro Morita, Kazuhiro Yoshida, Norihito Sakaguchi, Takashi Toyao, Ken-ichi Shimizu, Satoshi Ishikawa, Wataru Ueda, Masatake Haruta, Toru Murayama
Nature Communications, 12, 1, 557, 557, Springer Science and Business Media LLC, 2021年12月, ［国際誌］
英語, 研究論文（学術雑誌）, NH₃-SCR (selective catalytic reduction) is important process for removal of NOx. However, water vapor included in exhaust gases critically inhibits the reaction in a low temperature range. Here, we report bulk W-substituted vanadium oxide catalysts for NH₃-SCR at a low temperature (100–150 °C) and in the presence of water (~20 vol%). The 3.5 mol% W-substituted vanadium oxide shows >99% (dry) and ~93% (wet, 5–20 vol% water) NO conversion at 150 °C (250 ppm NO, 250 ppm NH₃, 4% O₂, SV = 40000 mL h⁻¹ g_cat⁻¹). Lewis acid sites of W-substituted vanadium oxide are converted to Brønsted acid sites under a wet condition while the distribution of Brønsted and Lewis acid sites does not change without tungsten. NH₄⁺ species adsorbed on Brønsted acid sites react with NO accompanied by the reduction of V⁵⁺ sites at 150 °C. The high redox ability and reactivity of Brønsted acid sites are observed for bulk W-substituted vanadium oxide at a low temperature in the presence of water, and thus the catalytic cycle is less affected by water vapor.

Synthesis of Zeolitic Ti, Zr-Substituted Vanadotungstates and Investigation of Their Catalytic Activities for Low Temperature NH3-SCR
Meilin Tao, Satoshi Ishikawa, Zhenxin Zhang, Toru Murayama, Yusuke Inomata, Akiho Kamiyama, Ichika Nakaima, Yuan Jing, Shinya Mine, Kosuke Shimoda, Takashi Toyao, Ken Ichi Shimizu, Wataru Ueda
ACS Catalysis, 11, 22, 14016, 14025, 2021年11月19日
研究論文（学術雑誌）, Microporous vanadotungstate (W4V3O19, VT-1) was constructed via the connection of [W4O16]8- cubane units with VO2+ linkers to form an LTA-zeolite-type crystal structure. We found that the VO2+ sites connecting the cubane units of VT-1 could be partially removed by an appropriate acid treatment without destroying its crystal structure. This process involved a redox reaction between the [W4O16]8- cubane units and VO2+ linkers, and V was removed as V5+ during the acid treatment. TiO2+ or ZrO2+ could be introduced into the VO2+ vacancies. The introduction of Ti or Zr substantially improved the thermal stability of VT-1 under oxidizing conditions. The catalytic activity toward the selective catalytic reduction of NOx with NH3 (NH3-SCR) was improved by the introduction of Ti or Zr.

Catalytic Activities of Various Niobium Oxides for Hydrogen Absorption/Desorption Reactions of Magnesium
Keita Shinzato, Hiroyuki Gi, Toru Murayama, Masahiro Sadakane, Yongming Wang, Shigehito Isobe, Takayuki Ichikawa, Hiroki Miyaoka
ACS Omega, 6, 36, 23564, 23569, American Chemical Society (ACS), 2021年09月14日, ［国際誌］
英語, 研究論文（学術雑誌）, Five types of niobium(V) oxides (Nb2O5) were synthesized by hydrothermal and heat treatment processes, and their structural properties and catalytic activities for the hydrogen absorption/desorption reactions of magnesium were characterized. The synthesized Nb oxides were dispersed on magnesium hydride (MgH2), a typical hydrogen storage material, using the ball-milling method. All the synthesized Nb oxides improved the reaction kinetics of the hydrogen desorption/absorption reactions. The catalytic activities for the hydrogen desorption were comparable, while the hydrogen absorption rates were significantly different for each synthesized Nb oxide. This difference can be explained by the structural stability of Nb2O5, which is related to the formation of a catalytically active state by the reduction of Nb2O5 during the ball-milling process. Notably, the highest catalytic effect was observed for Nb2O5 with a highly crystalline pyrochlore structure and a low specific surface area, suggesting that pyrochlore Nb2O5 is a metastable phase. However, only the amorphous Nb oxide was out of order, even though there is a report on the high catalytic activity of amorphous Nb oxide. This is attributed to the initial condensed state of amorphous Nb oxide, because particle size affects the dispersion state on the MgH2 surface, which is also important for obtaining high catalytic activity. Thus, it is concluded that Nb2O5 with lower stability of the crystal structure and smaller particle size shows better catalysis for both hydrogen desorption and absorption reactions.

Analogous Mechanistic Features of NH3-SCR over Vanadium Oxide and Copper Zeolite Catalysts
Hiroe Kubota, Takashi Toyao, Zen Maeno, Yusuke Inomata, Toru Murayama, Naoto Nakazawa, Satoshi Inagaki, Yoshihiro Kubota, Ken Ichi Shimizu
ACS Catalysis, 11, 17, 11180, 11192, 2021年09月03日
研究論文（学術雑誌）, Reduction/oxidation half-cycles of the selective catalytic reduction of NO with NH3(NH3-SCR) at 200 °C were investigated usingin situandoperandospectroscopies to propose a general mechanism for four different catalysts (TiO2-supported and bulk vanadium oxides and Cu-AFX and Cu-CHA zeolites). The reduction half-cycle is initiated by the reaction of NH3on Lewis acid sites [V(V) or Cu(II); L-NH3] and NO, followed by the gradual reaction of NH3on Brønsted acid sites (B-NH3) and NO; this results in the formation of V(IV) or Cu(I) and protons (H+) on the surface, along with N2and H2O. The UV-vis measurements for the reduction half-cycle indicate that N2is continuously generated until the surface V(V) or Cu(II) species is depleted. The subsequent reoxidation of the reduced catalysts under O2leads to the regeneration of V(V) or Cu(II) and the reaction of surface H+, yielding H2O (oxidation half-cycle). The higher consumption rates of B-NH3and L-NH3under NO + O2than those under NO, which has been previously reported in the literature, were explained based on the continuous reduction/oxidation of V(V)/V(IV) or Cu(II)/Cu(I) where the regenerated V(V) or Cu(II) site is reused in the subsequent (second) reduction half-cycle. Namely, upon the recovery of V(V) or Cu(II)viareoxidation, the leftover B-NH3species react with the supplied NO to yield N2; this suggests that B-NH3is not a spectator but a reservoir of NH3to participate in the second reduction half-cycle possiblyviathe migration of NH3or HONO species. These results provide comprehensive evidence of the general mechanism of NH3-SCR, which was found to be applicable to both V and Cu catalysts.

Synthesis of bulk vanadium oxide with a large surface area using organic acids and its low-temperature NH3-SCR activity
Yusuke Inomata, Shinichi Hata, Eiji Kiyonaga, Keiichiro Morita, Kazuhiro Yoshida, Masatake Haruta, Toru Murayama
CATALYSIS TODAY, 376, 188, 196, ELSEVIER, 2021年09月, ［査読有り］
英語, 研究論文（学術雑誌）, Selective catalytic reduction using NH3 (NH3-SCR) is a chemical process that is used for the elimination of NOx (NO and NO2). Although current vanadia-based catalysts need a high reaction temperature, which leads to deactivation of the catalysts, bulk vanadium oxide showed the potential for NH3-SCR at a low temperature below 150 degrees C. We investigated a method for synthesis of vanadium oxide with a large surface area using an organic acid to enhance its NH3-SCR activity. Vanadium oxide catalysts were synthesized from ammonium metavanadate (NH4VO3) and organic acids (oxalic acid, succinic acid, malic acid and citric acid). When carboxylic acids (oxalic acid and succinic acid) were used as the organic acid source, the surface area of the catalysts increased up to 41 cm2 g-1, which was larger than that of vanadium oxide synthesized without an organic acid and with hydroxy acid. SEM and TEM measurements showed that vanadium oxide catalysts synthesized by the calcination of vanadyl oxalate at 300 degrees C (V2O5-OX_300) formed a pore structure that contributed to the increase in surface area. An increase in the number of acid sites and redox sites, which is important for NH3-SCR to proceed, was confirmed from NH3-TPD and H2-TPR measurements for V2O5-OX_300. The NO conversion of V2O5-OX_300 (47 % at 100 degrees C) was higher than that of the catalysts synthesized from only NH4VO3 (19 % at 100 degrees C), indicating that vanadium oxide catalysts synthesized using carboxylic acid have the low-temperature NH3-SCR activity due to the increase in their surface area.

Performance of Au/ZnO catalysts in CO2 reduction to methanol: Varying the Au loading / Au particle size
Shilong Chen, Ali M. Abdel-Mageed, Ashlee Hauble, Tamao Ishida, Toru Murayama, Magdalena Parlinska-Wojtan, R. Jürgen Behm
Applied Catalysis A: General, 624, Elsevier B.V., 2021年08月25日
英語, 研究論文（学術雑誌）, Methanol synthesis by CO2 reduction is an important approach for energy storage. Aiming at a reduction of the catalyst mass in technical applications, we have investigated the influence of increasing Au loading on the performance of Au/ZnO in methanol and CO formation from CO2 reduction. Using the same type of ZnO support, increased Au loading resulted also in a pronounced increase in Au particle size. The Au-mass-normalized reaction rate for methanol formation and TOF decrease with increasing Au loading/particle size, while the selectivity for methanol formation increases. CO adsorption monitored by in situ FTIR revealed a pronounced decrease of the accessible Au surface area during reaction, independent of the Au loading, pointing to a partial encapsulation of the Au nanoparticles by a partly reduced ZnOx, as described by SMSI effects. Possible reasons responsible for these effects and Au loading/size effects therein are discussed, strategies for future work are outlined.

True Catalytically Active Structure in Mo-V-Based Mixed Oxide Catalysts for Selective Oxidation of Acrolein
Satoshi Ishikawa, Yudai Yamada, Naoki Kashio, Nagisa Noda, Kosuke Shimoda, Mio Hayashi, Toru Murayama, Wataru Ueda
ACS Catalysis, 11, 16, 10294, 10307, American Chemical Society, 2021年08月20日
英語, 研究論文（学術雑誌）, Crystalline trigonal Mo3VOx (Tri-MoVO) catalyst is constructed of {Mo6O21}6- pentagonal units and octahedral {MO6} units that form hexagonal and heptagonal channels in the crystal structure. Tri-MoVO is an extremely active catalyst for selective oxidation of acrolein (ACR) to form acrylic acid (AA), with the local structure around the heptagonal channel responsible for the catalysis. Here, promoter elements that are widely used in industrial Mo-V-based mixed oxide catalysts (W and Cu) were introduced without altering the crystal structure of Tri-MoVO. W was located at the pentagonal unit sites by replacing Mo, and Cu was located in the interstitial spaces of lattice oxygens in the corner of the heptagonal channel micropore, forming a sophisticated crystal structure involving the four constituent elements. Introduction of W improved the ACR conversion without altering AA selectivity even when the water pressure in the reaction gas was decreased, owing to the promotion of the dissociative adsorption of water. The introduction of Cu resulted in improvement of the AA selectivity from ca. 93-94% to ca. 97%. Based on the structural and elemental similarities between Tri-MoVWCuO and industrially utilized Mo-V-based mixed oxide catalysts synthesized according to the patented procedure, we concluded that Tri-MoVWCuO is the true catalytically active structure for selective oxidation of ACR.

Controlling the O-Vacancy Formation and Performance of Au/ZnO Catalysts in CO2 Reduction to Methanol by the ZnO Particle Size
Shilong Chen, Ali M. Abdel-Mageed, Chihiro Mochizuki, Tamao Ishida, Toru Murayama, Jabor Rabeah, Magdalena Parlinska-Wojtan, Angelika Brückner, R. Jürgen Behm
ACS Catalysis, 11, 15, 9022, 9033, American Chemical Society (ACS), 2021年08月06日
研究論文（学術雑誌）

Selective catalytic oxidation of ammonia to nitrogen over zeolite-supported Pt-Au catalysts: Effects of alloy formation and acid sites
Haifeng Wang, Mingyue Lin, Toru Murayama, Shixiang Feng, Masatake Haruta, Hiroki Miura, Tetsuya Shishido
Journal of Catalysis, Elsevier BV, 2021年08月
研究論文（学術雑誌）

Insights into Au Nanoparticle Size and Chemical State of Au/ZSM-5 Catalyst for Catalytic Cracking of n-Octane to Increase Propylene Production
Miao Zhang, Qi Liu, Houang Long, Libo Sun, Toru Murayama, Caixia Qi
Journal of Physical Chemistry C, 125, 29, 16013, 16023, American Chemical Society, 2021年07月29日
英語, 研究論文（学術雑誌）, The cracking of n-octane to propylene was chosen as a model reaction over gold catalysts supported on ZSM-5. Au/ZSM-5 catalysts with a series of Au particle sizes (6.9-10.6 nm) were prepared through deposition-precipitation in which the catalysts were distinguishable and had uniform-sized Au particles. Au/ZSM-5 catalysts with different Au species were obtained by changing the reduction temperature. The crystallinity, textural parameters, and acidity of Au/ZSM-5 were not destroyed compared with those of virgin ZSM-5 through this preparation approach. The influences of Au particle size and Au species are linked to the catalytic activity and selectivity in catalytic cracking reactions to increase propylene production. Metallic gold was found to be dominant for the cracking reaction, and the Au particle size played an important role in the dehydrogenation reaction to produce propylene. The reaction results of real light diesel oil are consistent with octane cracking where a smaller gold particle size provides a better catalytic activity. The effects of the Au chemical state on the catalytic activity and selectivity were also researched, and the Au0 species was the dominant Au active site for the cracking reaction. A similar conclusion was also verified in the light diesel oil cracking reaction.

Ag Size/Structure-Dependent Effect on Low-Temperature Selective Catalytic Oxidation of NH3 over Ag/MnO2
Haifeng Wang, Mingyue Lin, Toru Murayama, Shixiang Feng, Masatake Haruta, Hiroki Miura, Tetsuya Shishido
ACS Catalysis, 11, 14, 8576, 8584, American Chemical Society (ACS), 2021年07月16日
研究論文（学術雑誌）

Synthesis of Zeolitic Mo-Doped Vanadotungstates and Their Catalytic Activity for Low-Temperature NH3-SCR
Meilin Tao, Satoshi Ishikawa, Toru Murayama, Yusuke Inomata, Akiho Kamiyama, Wataru Ueda
INORGANIC CHEMISTRY, 60, 7, 5081, 5086, AMER CHEMICAL SOC, 2021年04月, ［国際誌］
英語, 研究論文（学術雑誌）, Mo was successfully introduced into a vanadotungstate (VT-1), which is a crystalline microporous zeolitic transition-metal oxide based on cubane clusters [W4O16](8-) and VO2+ linkers (MoxW4-x. x: number of Mo in VT-1 unit cell determined by inductively coupled plasma-atomic emission spectroscopy (ICP-AES)). It was confirmed that W in the cubane units was substituted by Mo. The resulting materials showed higher microporosity compared with VT-1. The surface area and the micropore volume increased to 296 m(2).g(-1) and 0.097 cm(3).g(-1), respectively, for Mo0.6W3.4 compared with the those values for VT-1 (249 m(2).g(-1) and 0.078 cm(3).g(-1), respectively). The introduction of Mo changed the acid properties including the acid amount (VT-1: 1.06 mmol g(-1), Mo0.6W3.4: 2.18 mmol.g(-1)) and its strength because of the changes of the chemical bonding in the framework structure. MoxW4-x showed substantial catalytic activity for the selective catalytic reduction of NO with NH3 (NH3-selective catalytic reduction (SCR)) at a temperature as low as 150 degrees C.

Gold Nanoparticles Supported on Ce-Zr Oxides for Selective Hydrogenation of Acetylene
Xiaoyue Hua, Yuhua Zheng, Zixuan Yang, Libo Sun, Huijuan Su, Toru Murayama, Caixia Qi
TOPICS IN CATALYSIS, 64, 3-4, 206, 214, SPRINGER/PLENUM PUBLISHERS, 2021年03月
英語, 研究論文（学術雑誌）, Gold nanocatalysts have been reported to be active in the selective hydrogenation of acetylene. In this paper, a series of Au/Ce1-xZrxO2(x = 0.03 to 0.5) supported catalysts with different ratios of Ce to Zr were prepared and their catalytic performance for selective hydrogenation of acetylene was investigated. The structure and surface defects of the catalyst can be changed by altering the amount of Zr incorporation. Compared to both Au/CeO(2)and Au/ZrO2, the synthesized Au/Ce(1-x)Zr(x)O(2)showed the higher catalytic activity with keeping almost 100% ethylene selectivity at 300 degrees C. The TEM observation indicated that the incorporation of Zr led to the formation of hollow spherical solid solutions. The specific surface area also has a certain influence on the catalytic activity. Considering the catalytic activity of Au/Ce(1-x)Zr(x)O(2)and their characterizations by XPS and Raman, the concentration of Ce(4+)and the oxygen vacancy of the Ce(1-x)Zr(x)O(2)support play an important role in the selective hydrogenation of acetylene.

High dimensionally structured W-V oxides as highly effective catalysts for selective oxidation of toluene
Toru Murayama, Satoshi Ishikawa, Norihito Hiyoshi, Yoshinori Goto, Zhenxin Zhang, Takashi Toyao, Ken-ichi Shimizu, Shutoku Lee, Wataru Ueda
CATALYSIS TODAY, 363, 60, 66, ELSEVIER, 2021年03月
英語, 研究論文（学術雑誌）, High dimensionally structured W-V-O catalysts (HDS-WVO) were synthesized by hydrothermal method and catalyst structures were investigated by HAADF-STEM analysis. HDS-WVO were rod-shaped crystals and the cross-sections were constituted by W6O21 pentagonal units and MO6 octahedra (M = V, W), forming heptagonal and hexagonal channels. HDS-WVO catalysts showed excellent catalytic performance for selective oxidation of toluene to benzoic acid, and the activity and the selectivity to benzoic acid were superior to those of state-of-theart catalysts. After the ion exchange using Cs+, the catalytic activity over HDS-WVO was significantly decreased. Since HAADF-STEM analysis and N-2 adsorption revealed that Cs+ was located mainly at the heptagonal channel of HDS-WVO, it can be concluded that toluene oxidation takes place at the heptagonal channel site of HDS-WVO.

Preparation of Polyaniline Microtubes as the Gold Catalyst Support with Improved Catalytic Performances for the Reduction of Nitrophenols
Libo Sun, Lin Jiang, Jie Zhang, Toru Murayama, Miao Zhang, Yuhua Zheng, Huijuan Su, Caixia Qi
TOPICS IN CATALYSIS, 64, 3-4, 215, 223, SPRINGER/PLENUM PUBLISHERS, 2021年03月
英語, 研究論文（学術雑誌）, Polyaniline (PANI) microtubes supported Au catalysts were prepared and evaluated in the catalytic reduction of nitrophenols to aminophenols with NaBH(4)as the reductant. PANI microtubes were prepared through a template-free method with salicylic acid as the dopant. HAuCl(4)was used as a gold precursor. Au nanoparticles were loaded on PANI microtubes by an in situ redox reaction between PANI and HAuCl4. The morphology and structure of the as-prepared PANI/Au composite catalyst were investigated using SEM, TEM, FT-IR, XRD and Raman spectra. We found that the metallic Au nanoparticles were loaded on PANI through the in situ redox reaction and located closer to the imine nitrogens of PANI. And the interaction between PANI and Au nanoparticles led the metallic Au negatively charged and favored the improvement of catalytic activities in the reduction of 4-nitrophenol (4-NP). A comparative study for the catalytic reduction of 3-nitrophenol (3-NP) and 2-nitrophenol (2-NP) showed that the activity sequence of PANI/Au was 3-NP > 2-NP > 4-NP.

C, N Co-Decorated Alumina-Supported Au Nanoparticles:Enhanced Catalytic Performance for Selective Hydrogenation of Acetylene
Yuan Zhang, Xun Sun, Yali Zhao, Huijuan Su, Toru Murayama, Caixia Qi
TOPICS IN CATALYSIS, 64, 3-4, 197, 205, SPRINGER/PLENUM PUBLISHERS, 2021年03月
英語, 研究論文（学術雑誌）, The modifications of support for the dispersion and immobilization of gold nanoparticles were examined for the selective hydrogenation of acetylene to ethylene. The catalyst, denoted as Au/CNA, was prepared by the carbonization of C and N atom-containing organic precursors on Al2O3, which were subsequently used as supports for gold nanoparticles. The TOF value of Au/CNA was five times higher than that of Au/Al(2)O(3)at 250 degrees C. The carbonization modification of Al(2)O(3)support without N species showed almost no change in catalytic activity. Therefore, the improved catalytic performance of Au/CNA is related to the interactions of the N species on the CNA support with nano-gold particles. From the XPS analysis, electron transfer between gold and C, N co-doped species may play an important role in the high levels of Au active site utilization. This study may provide new avenues for the construction of organic/inorganic composite materials for efficient catalytic hydrogenation applications.

Influence of the support in aqueous phase oxidation of ethanol on gold/metal oxide catalysts studied by ATR-IR spectroscopy under working conditions
Ammara Waheed, Xianwei Wang, Nobutaka Maeda, Daniel M. Meier, Tamao Ishida, Toru Murayama, Masatake Haruta, Alfons Baiker
CATALYSIS COMMUNICATIONS, 148, ELSEVIER, 2021年01月
英語, 研究論文（学術雑誌）, Effects of supports (Co3O4, CeO2, NiO) in the gold-catalyzed aqueous phase oxidation of ethanol (EtOH) to acetic acid (AcOH) were examined. ATR-IR spectroscopy under working conditions of the catalysts uncovered on gold particles bidentate ethoxy, and on supports monodentate ethoxy species, multi-layered ethanol, and acetate. Preferential formation of bidentate ethoxy species and adsorbed EtOH were identified as key factors for high activity and selectivity to AcOH. These requirements were best matched with Au/Co3O4. On NiO, monodentate ethoxy species on the support deteriorated the catalytic performance due to consecutive esterification of AcOH and/or acetate species with EtOH producing undesirable ethyl acetate.

Features of Nb2O5 as a metal oxide support of Pt and Pd catalysts for selective catalytic oxidation of NH3 with high N-2 selectivity
Mingyue Lin, Baoxiang An, Takashi Takei, Tetsuya Shishido, Tamao Ishida, Masatake Haruta, Toru Murayama
JOURNAL OF CATALYSIS, 389, 366, 374, ACADEMIC PRESS INC ELSEVIER SCIENCE, 2020年09月
英語, 研究論文（学術雑誌）, Selective catalytic oxidation of ammonia (NH3-SCO) to N-2 and H2O was examined as one of the most efficient solutions for NH3 pollution because NH3 has potentially harmful effects on human health and the environment. The acidic metal oxide Nb2O5 that possesses both Bronsted and Lewis acid sites was chosen as the support of Pt and Pd catalysts for SCO of 50 ppm NH3. Both Pt/Nb2O5 and Pd/Nb2O5 showed extremely high levels of N-2 selectivity (98% and 100%, respectively) at 100% NH3 conversion. The role of the acid sites of Pt/Nb2O5 and Pd/Nb2O5 in NH3-SCO was investigated by the NaOH treatment to neutralize the Bronsted acid sites. The selectivity to N-2 decreased by the NaOH treatment of Pt/Nb2O5 and Pd/Nb2O5. These results suggested that the Bronsted acid sites were essentially important for improving N-2 selectivity. This study provides a new concept for the design of a catalyst by using the acid sites of acidic metal oxide to improve the N-2 selectivity of NH3-SCO. (C) 2020 Elsevier Inc. All rights reserved.

Ligand effect of gold colloid in the preparation of Au/Nb2O5 for CO oxidation
Mingyue Lin, Chihiro Mochizuki, Baoxiang An, Tetsuo Honma, Masatake Haruta, Tamao Ishida, Toru Murayama
JOURNAL OF CATALYSIS, 389, 9, 18, ACADEMIC PRESS INC ELSEVIER SCIENCE, 2020年09月, ［査読有り］
英語, 研究論文（学術雑誌）, Sol immobilization method by using a ligand protected gold colloid precursor, Au-n(SC12H25)(m), was applied for the deposition of gold on Nb2O5 which is a typical solid acid. The effects of the thiolate ligand on the preparation of Au/Nb2O5 and on the catalytic activity for CO oxidation were investigated. Although most of the thiolate ligands were removed during the calcination at 300 degrees C, a small amount of sulfur species still remained on the catalyst, which played an important role for preventing the aggregation of the gold nanoparticles to give ca. 2.8 nm in a mean diameter with the gold loading amounts in the range from 0.9 wt% to 4.2 wt%. Calcination at a lower temperature (250 degrees C) gave a larger amount of the sulfur species than did the calcination at 300 degrees C, lowering catalytic activity for CO oxidation. The temperature for 50% CO conversion (T-50%) was 3 degrees C for 0.9 wt% Au/Nb2O5 under 20,000 mL h(-1) g(cat)(-1), using 1 vol% CO in air. With an increase in the loading amount of gold, the catalytic activity became higher. The T-50% of 4.2 wt% Au/Nb2O5 was -41 degrees C and turnover frequency (TOF) based on a number of the perimeter gold atom was calculated to be 8.7 s(-1) at 20 degrees C. The TOF value obtained by Au/Nb2O5 prepared by deposition-reduction without thiolate ligands was 5.0 s(-1). This result suggests that the sulfur remained on the catalyst did not inhibit CO oxidation. (C) 2020 Elsevier Inc. All rights reserved.

Elucidation of Active Sites of Gold Nanoparticles on Acidic Ta2O5 Supports for CO Oxidation
Mingyue Lin, Chihiro Mochizuki, Baoxiang An, Yusuke Inomata, Tamao Ishida, Masatake Haruta, Toru Murayama
ACS CATALYSIS, 10, 16, 9328, 9335, AMER CHEMICAL SOC, 2020年08月
英語, 研究論文（学術雑誌）, Gold nanoparticles of small sizes with a highly uniform dispersion were successfully deposited on several crystalline forms of Ta2O5 (pseudohex-agonal, orthorhombic, and pyrochlore) by the sol immobilization method. The pseudohexagonal Ta2O5 (TT-Ta2O5) synthesized by a hydrothermal method showed the highest catalytic activity for CO oxidation as a support for gold catalysts. The temperature at 50% CO conversion was -11 degrees C for 1 wt % Au/TT-Ta2O5, and the temperature was 23 degrees C at 100% CO conversion (space velocity of 20000 mL h(-1 )g(cat)(-1)). To investigate the reaction mechanism, in situ performed, and the sequential delivery of adsorbed CO on Ta2O5 sites and Au sites to the active sites was observed at -120 degrees C. The results of temperature-programmed CO reduction suggested that the oxygen adsorbed at -100 degrees C contributed mainly to the high catalytic activity of CO oxidation, while the lattice oxygen played a minor role for CO oxidation from -60 to 100 degrees C, which was the same temperature range with the actual reaction condition.

Gold Nanoparticles Supported on Nb2O5 for Low-Temperature CO Oxidation and as Cathode Materials for Li-ion Batteries
Luong Xuan Dien, Quang Duc Truong, Toru Murayama, Huynh Dang Chinh, Ayako Taketoshi, Itaru Honma, Masatake Haruta, Tamao Ishida
APPLIED CATALYSIS A-GENERAL, 603, 117747, 117747, ELSEVIER, 2020年08月
英語, 研究論文（学術雑誌）, We prepared a series of Nb2O5 polymorphs by the sol-gel method and the sol-gel hydrothermal method. Gold nanoparticles supported on Nb2O5 were prepared by solid grinding method. Au on pseudohexagonal (TT-phase) Nb2O5 containing an amorphous phase exhibited higher catalytic activity for CO oxidation than did other Au/Nb2O5 polymorphs. For the electrochemical properties for cathode materials of Li-ion batteries, Nb2O5 (TT) exhibited high capacity of 208 mA h g(-1), and the deposition of Au onto Nb2O5 (TT) improved the capacity to 232 mA h g(-1). Capacity and CO oxidation activity were related; the higher the catalytic activity Au/Nb2O5 shows, the higher is the discharging capacity. From the characterization results, Nb2O5 (TT) contains oxygen vacancies (Nb4+ sites), and the oxygen vacancies of Nb2O5 (TT) would play an important role for CO oxidation and the performance for Li-ion batteries.

Low-Temperature Propylene Epoxidation Activity of CuO-CeO2 Catalyst with CO + O-2: Role of Metal-Support Interaction on the Reducibility and Catalytic Property of CuOx Species
Tinku Baidya, Tanmoy Mazumder, Konstantin Yu Koltunov, Pravin R. Likhar, Adam H. Clark, Khushubo Tiwari, Vladimir Sobolev, Soumitra Payra, Toru Murayama, Mingyue Lin, Parthasarathi Bera, Sounak Roy, Krishanu Biswas, Olga Safonova, Bolla Srinivasa Rao, Masatake Haruta
JOURNAL OF PHYSICAL CHEMISTRY C, 124, 26, 14131, 14146, AMER CHEMICAL SOC, 2020年07月
英語, 研究論文（学術雑誌）, Epoxidation of propylene into propylene oxide (PO) in the gas phase is a highly challenging reaction. Cu-based catalysts have been active for this reaction, but the state of Cu as an active species is still debatable. In this paper, we report the propylene epoxidation activity of solution combustion synthesized Cu/CeO2 catalysts with the CO + O-2 mixture at low temperatures (50-100 degrees C) peaking at similar to 80 degrees C. The highest PO yield was obtained with 20-25% Cu loading in CeO2. In contrast, the reaction over the catalyst containing nonreducible support such as Cu/SiO2 occurred above 170 degrees C. Detailed structural characterization indicated two types of Cu species such as Cu(2+ )partly (similar to 3%) dissolved in CeO2 forming a CuxCe1-xO2-delta phase and the remaining amount formed highly dispersed CuO as a separate phase. Thus, the highest activity relates to the optimum presence of CuO along with Ce1-xCuxO2-delta. The reducibility of the Cu species in two phases was significantly shifted toward lower temperatures, indicating strong electronic interaction between the two phases. The substituted Cu2+ was reduced first, and then, the bulk CuO reduction was initiated. In situ spectroscopic studies showed Cu+ formation from Cu2+ over Cu/CeO2 catalysts even at room temperature unlike in CeO2 or CuO + CeO2 physical mixtures, indicating strong electronic interaction between Ce1-xCuxO2-delta and CuO phases on CO adsorption in the Cu/CeO2 catalyst. It is proposed that substituted Cu2+ along with Ce4+ is reduced easily, and then, Ce3+ promotes the reduction of the interfacial CuO phase that might donate active oxygen species for epoxidation reaction.

CO2 Reduction to Methanol on Au/CeO2 Catalysts: Mechanistic Insights from Activation/Deactivation and SSITKA Measurements
Azita Rezvani, Ali M. Abdel-Mageed, Tamao Ishida, Toru Murayama, Magdalena Parlinska-Wojtan, R. Juergen Behm
ACS CATALYSIS, 10, 6, 3580, 3594, AMER CHEMICAL SOC, 2020年03月
英語, 研究論文（学術雑誌）, Aiming at a mechanistic understanding of the methanol (MeOH) synthesis from CO2/H-2 over Au/CeO2 catalysts and the activation/deactivation of these catalysts, we have investigated these processes by a combination of kinetic measurements, time-resolved in situ diffuse reflectance Fourier transform infrared (FTIR) spectroscopy (DRIFTS) measurements, and structural characterization by X-ray diffraction (XRD) and scanning transmission electron microscopy (STEM). Kinetic measurements indicated a rapid activation phase, followed by a continuous slow deactivation. A faster deactivation of CO formation (reverse water-gas shift reaction) compared to that of methanol formation results in an increasing selectivity toward MeOH formation with time on stream. The activation of the catalyst is attributed to a rapid initial reduction of the support (formation of O vacancies). Since based on STEM imaging and XRD measurements sintering of Au nanoparticles is negligible, the subsequent deactivation is attributed to the slow buildup of site-blocking adsorbates, specifically surface carbonates, and/or over-reduction of the catalyst. This is supported also by the reversible nature of the deactivation upon recalcination in O-2/N-2. Steady-state isotopic transient kinetic analysis (SSITKA) measurements, following the buildup/decay of adsorbed formate and methoxy species by DRIFTS upon changing from a CO2/H-2 to a CO2/D-2 mixture and back under steady-state conditions, indicate that surface formate species are reaction intermediates in the dominant reaction pathway for CO2 hydrogenation to methanol, with the calculated rates of formation/decay comparable to the rate of methanol formation. The consequences of these results for the mechanistic understanding of this reaction are discussed.

Importance of Size and Contact Structure of Gold Nanoparticles for the Genesis of Unique Catalytic Processes
Tamao Ishida, Toru Murayama, Ayako Taketoshi, Masatake Haruta
CHEMICAL REVIEWS, 120, 2, 464, 525, AMER CHEMICAL SOC, 2020年01月, ［国際誌］
英語, 研究論文（学術雑誌）, Since the discovery of catalysis by Au nanoparticles (NPs), unique catalytic features of Au have appeared that are greatly different from those of Pd and Pt. In this Review, we aimed to disclose how the unique catalytic abilities of Au are generated with respect to (a) the contact structures between Au and its supports and (b) the size of the Au particles. For CO oxidation, the catalytic activity of Au on reducible metal oxides (MOx) is strongly correlated with the amount of oxygen vacancies of the MOx surface, which play a key role in O-2 activation. Single atoms, bilayers of Au, sub-nm clusters, clusters (1-2 nm), and NPs (2-5 nm) have been proposed as the active sizes of the Au species, which may depend on the type of support. For propylene epoxidation, the presence of isolated TiO4 units in SiO2 supports is important for the production of propylene oxide (PO). Au NPs facilitate the formation of Ti-OOH species, which leads to PO in the presence of H-2 and O-2, whereas Au clusters facilitate propylene hydrogenation. However, Au clusters can produce PO by using only O-2 and water, whereas Au NPs cannot. For alcohol oxidation, the reducibility of the MOx supports greatly influences the catalytic activity of Au, and single Au atoms more effectively activate the lattice oxygen of CeO2. The basic and acidic sites of the MOx surface also play an important role in the deprotonation of alcohols and the activation of aldehydes, respectively. For selective hydrogenation, heterolytic dissociation of H-2 takes place at the interface between Au and MOx, and the basic sites of MOx contribute to H-2 activation. Recent research into the reaction mechanisms and the development of well-designed Au catalysts has provided new insights into the preparation of high-performance Au catalysts.

Multi-dimensional Crystal Structuring of Complex Metal Oxide Catalysts of Group V and VI Elements by Unit-Assembling
Satoshi Ishikawa, Zhenxin Zhang, Toru Murayama, Norihito Hiyoshi, Masahiro Sadakane, Wataru Ueda
TOPICS IN CATALYSIS, 62, 17-20, 1157, 1168, SPRINGER/PLENUM PUBLISHERS, 2019年11月, ［査読有り］
英語, 研究論文（学術雑誌）, Four new porous crystalline complex metal oxide families based on group V and VI elements, all of which are synthesized through unit-assembling, are introduced along with crystal structure formation mechanism. Polyoxometalates (POMs) are utilized as building units and assembled for constructing microporous complex metal oxides. Assembling of MoVO-POMs having pentagonal units of [Mo6O21] with {VO} linkers under hydrothermal conditions forms microporous orthorhombic (NH4)(4)[Mo30V4O106] {VO}(6) oxide and trigonal (NH4)(3)[Mo19.5V1.5O69] {VO}(6) oxide. Assembling of epsilon-Keggin Mo-POMs with bismuth ions as a linker under a hydrothermal condition produces a cubic (NH4)(4)[Mo9.4V3.6O40] {Bi}(2) crystal with cages and channels with the diameter sizes of 0.77 and 0.34 nm, respectively. One dimensional anionic tungstosellenate molecular wire building block, [SeW6O21](2-)(n), is first formed by linear connection of hexagonal tungstosellenate POM units [SeW6O27] and then linked with the Co-II ion to form a crystalline microporous materials, (NH4)(0.4) [SeW6O21] {Co(OH)}(1.3). [W4O16] building blocks are orderly connected with {VO} linkers to form a microporous framework (K-1.5(NH4)(0.2)H-0.3[W4O16]{VO}(3)) with a pore diameter of 0.43 nm which is fully opened and is accessible to small molecules. These new porous crystalline complex metal oxides showed high catalytic performance for alkane oxidation, aldehyde oxidation, alcohol oxidation, H2O2 oxidation, NH3-SCR, and so on.

Bulk Vanadium Oxide versus Conventional V2O5/TiO2: NH3-SCR Catalysts Working at a Low Temperature Below 150 degrees C
Yusuke Inomata, Shinichi Hata, Makoto Mino, Eiji Kiyonaga, Keiichiro Morita, Kenji Hikino, Kazuhiro Yoshida, Hiroe Kubota, Takashi Toyao, Ken-ichi Shimizu, Masatake Haruta, Toru Murayama
ACS CATALYSIS, 9, 10, 9327, 9331, AMER CHEMICAL SOC, 2019年10月, ［査読有り］
英語, 研究論文（学術雑誌）, Practical catalysts that work at a low temperature for selective catalytic reduction of NOx using NH3 (NH3-SCR) have been required to treat NOx at the outlet temperature in boiler systems (100-150 degrees C). In this paper, we report bulk vanadium oxide catalysts that show NH3-SCR activity at a low temperature below 150 degrees C. Defective bulk vanadium oxide (V(V)+V(IV)) catalysts were synthesized by the calcination of vanadium(IV)-oxalate at 270 degrees C (1-4 h). The reaction rate per mol of surface vanadium atom of the catalyst calcined at 270 degrees C for 2 h (V 270-2, 6.4 x 10(-2) mol(NO) molV(-1) s(-1)) was 10-14 times faster than those of conventional 1-9 wt % V2O5/TiO2 (4.5 x 10(-3)-6.1 x 10-3 mol(NO) mol(V)(-1) s(-1)), indicating that bulk vanadium oxide is more favorable for NH3-SCR and V(IV) species enhance the activity. The NH3-SCR of V 270-2 is driven by the Lewis acid mechanism, which proceeds faster than the Bronsted acid mechanism.

Oxidative esterification of aliphatic aldehydes and alcohols with ethanol over gold nanoparticle catalysts in batch and continuous flow reactors
Ayako Taketoshi, Tamao Ishida, Toru Murayama, Tetsuo Honma, Masatake Haruta
Applied Catalysis A: General, 585, 117169, 117169, Elsevier BV, 2019年09月
研究論文（学術雑誌）

CO Oxidation over Au/ZnO: Unprecedented Change of the Reaction Mechanism at Low Temperature Caused by a Different O-2 Activation Process
Takashi Fujita, Tamao Ishida, Kohei Shibamoto, Tetsuo Honma, Hironori Ohashi, Toru Murayama, Masatake Haruta
ACS CATALYSIS, 9, 9, 8364, 8372, AMER CHEMICAL SOC, 2019年09月
英語, 研究論文（学術雑誌）, Au/ZnO prepared by coprecipitation exhibited extremely high catalytic activity for low-temperature CO oxidation below room temperature. The catalytic activity was influenced by the reduction atmosphere in the preparation and the heat treatment in air before the reaction. Reduction of Au(III )by H-2 not only gave smaller Au particles (Au/ZnO (H-2-xK), H-2 treatment at x = 373-673 K) but also a larger amount of Au-0 species than did calcination in air (Au/ZnO (O-2 -xK)), resulting in better activity. In addition, the catalytic activity of Au/ZnO (H-2-xK) was markedly enhanced by heat treatment in air prior to the CO oxidation. Kinetic measurements revealed that the activation energy (E-a) of Au/ZnO (H-2-xK) suddenly changed from 26 to 1.6 kJ mol(-1 )at a temperature below 253 K while the E a of Au/ZnO (O-2-xK) was constant, suggesting that the reaction mechanism for Au/ZnO (H-2-xK) changed at 253 K. UV-vis spectroscopy suggested a larger amount of defects of ZnO. Electron paramagnetic resonance results indicated that the amount of oxygen vacancies of ZnO or O-2- radicals formed on the oxygen vacancies was increased by H-2 reduction and heat treatment in air. In temperature-programmed O-2 desorption, a desorption peak was observed at a lower temperature for Au/ZnO (H-2-xK) after heat treatment than that for Au/ZnO (H-2-xK) before heat treatment and Au/ZnO (O-2-xK). These results suggested that the heat treatment of Au/ZnO (H-2-xK) created oxygen vacancies of which O-2 is activated around the perimeter interface and the activated oxygen is easily desorbed. These oxygen vacancies may become more efficient at a low temperature, resulting in the change of the reaction mechanism at 253 K. This study showed that the effect of the perimeter interface on activation of O-2 changes depending on the temperature and can be controlled by catalyst preparation and heat treatment.

Influence of the structure of trigonal Mo-V-M3rd oxides (M3rd=-, Fe, Cu, W) on catalytic performances in selective oxidations of ethane, acrolein, and allyl alcohol
Satoshi Ishikawa, Toru Murayama, Benjamin Katryniok, Franck Dumeignil, Marcia Araque, Svetlana Heyte, Sebastien Paul, Yudai Yamada, Mizuki Iwazaki, Nagisa Noda, Wataru Ueda
APPLIED CATALYSIS A-GENERAL, 584, ELSEVIER, 2019年08月
英語, 研究論文（学術雑誌）, Crystalline "MoVO", "MoVCuO", "MoVFeO" and "MoVWO" catalysts with a trigonal symmetry were successfully synthesized and characterized. The influence of the as-obtained structures on catalytic performances in selective oxidation reactions was investigated. MoVFeO and MoVCuO accomodated Fe and Cu species inside heptagonal channels, while W in MoVWO was incorporated in pentagonal {Mo6O21}(6-) units. Whereas MoVO and MoVWO showed catalytic activity in the selective oxidation of ethane and acrolein, MoVFeO and MoVCuO performed very poorly in the same reaction, suggesting that the presence of empty heptagonal channels is related to ethane and acrolein activations. In the selective oxidation of allyl alcohol, substantial amounts of acrolein (formed by oxidative dehydrogenation) and propanal (formed by isomerization) were formed as primary products over MoVO and MoVWO, whereas MoVFeO and MoVCuO preferentially promoted the formation of acrolein. It was found that the local crystal structure around the heptagonal channel was related with a modification of the reaction pathway for the selective oxidation of allyl alcohol. Due to the prevention of isomerization over MoVFeO, a high acrylic acid yield of 83.1% from allyl alcohol was achieved at 350 degrees C over this sample.

Ultra-Low-Temperature CO Oxidation Activity of Octahedral Site Cobalt Species in Co3O4 Based Catalysts: Unravelling the Origin of the Unique Catalytic Property
Tinku Baidya, Toru Murayama, Subramanian Nellaiappan, Nirmal Kumar Katiyar, Parthasarathi Bera, Olga Safonova, Mingyue Lin, Kaustubh R. Priolkar, Samapti Kundu, Bolla Srinivasa Rao, Patrick Steiger, Sudhanshu Sharma, Krishanu Biswas, Swapan Kumar Pradhan, Nakka Lingaiah, Kirtiman Deo Malviya, Masatake Haruta
JOURNAL OF PHYSICAL CHEMISTRY C, 123, 32, 19557, 19571, AMER CHEMICAL SOC, 2019年08月
英語, 研究論文（学術雑誌）, Co3O4 with spinel structure shows CO oxidation activity at very low temperature under dry conditions. This study aims at finding the origin of the unique catalytic activity of Co species in Co3O4 based oxides. Although, octahedral site Co3+ species have been reported to be active in Co3O4 based catalysts, there is no solid explanation as to why Co is so special as compared with other metals like Fe having similar redox states. In this study, mainly, three model spinel catalysts including MnCo2O4, MnFe2O4, and CoCr2O4 have been chosen. A detailed analysis of bulk and crystal surface structure, surface properties of the catalysts, and redox properties of the active metals has been performed to understand the unusual catalytic activity. Low-temperature CO oxidation activity decreases in the following order: MnCo2O4 >> MnFe2O4 > CoCr2O4. It indicates that the Co2+ species in a tetrahedral site (in CoCr2O4) remains inactive for low-temperature catalytic activity, while Co3+ in an octahedral site (in MnCo2O4) is active in Co3O4 based catalysts. This result is corroborated with CoFe2O4 which shows a higher activity than CoCr2O4, as it has partial occupation of the octahedral site. Fe, being a weak redox metal, does not show low-temperature activity, although crystallite facets of MnCo2O4 and MnFe2O4 catalysts are predominantly exposed in the (100) and (110) lattice planes, which contain quite similar concentrations of Co3+ and Fe3+ species in both. The intensity of the redox peak for CO oxidation involving a Co3+/Co2+ couple in MnCo2O4 indicates a highly favorable reaction, while a nonresponsive behavior of Co species is observed in CoCr2O4. As expected, MnFe2O4 is proven to be weak, giving a much lower intensity of electrochemical CO oxidation. Both CO- and H-2-TPR indicate a much higher reducibility of Co species in MnCo2O4 as compared with Co species in CoCr2O4 or Fe in MnFe2O4.

Redox-Active Zeolitic Transition Metal Oxides Based on epsilon-Keggin Units for Selective Oxidation
Zhenxin Zhang, Satoshi Ishikawa, Qianqian Zhu, Toru Murayama, Masahiro Sadakane, Michikazu Hara, Wataru Ueda
INORGANIC CHEMISTRY, 58, 9, 6283, 6293, AMER CHEMICAL SOC, 2019年05月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, The design and development of zeolitic transition metal oxides for selective oxidation are interesting due to the combination of the redox properties and microporosities. Redoxactive zeolitic transition metal oxides based on e-Keggin iron molybdates were synthesized. O-2 can be activated by the materials via an electron-transfer-based process, and the materials can be oxidized even at room temperature. The materials are oxidized and reduced reversibly while the crystal structures are maintained. V is uniformly incorporated in the materials without changing the basic structures, and the redox properties of the materials are tuned by V. The materials are used as robust catalysts for ethyl lactate oxidation to form ethyl pyruvate using O-2 as an oxidant.

New crystalline complex metal oxide catalysts with porous, acidic, and redox properties　　　　　　　　　　　　　　　
Satoshi Ishikawa, Zhenxin Zhang, Toru Murayama, Masahiro Sadakane, Wataru Ueda
Complex Oxides: An Introduction, 199, 222, World Scientific Publishing Co. Pte. Ltd., 2019年03月20日
英語, 論文集(書籍)内論文

Role of the Acid Site for Selective Catalytic Oxidation of NH 3 over Au/Nb 2 O 5
Mingyue Lin, Baoxiang An, Nao Niimi, Yohei Jikihara, Tsuruo Nakayama, Tetsuo Honma, Takashi Takei, Tetsuya Shishido, Tamao Ishida, Masatake Haruta, Toru Murayama
ACS Catalysis, 9, 3, 1753, 1756, 2019年03月01日
研究論文（学術雑誌）, © 2019 American Chemical Society. Selective catalytic oxidation (SCO) of NH 3 to harmless N 2 and H 2 O is an ideal technology for its removal. To develop air purification systems for a living environment, catalysts that can work at room temperature with high selectivities to N 2 are required. However, it has been a technical challenge because the reported catalysts either needed high operating temperatures or showed low selectivities to N 2 . In this study, we first demonstrated that acidic metal-oxide-supported gold catalysts showed good N 2 selectivities compared with that of other metal-oxide-supported gold catalysts. A gold catalyst with niobium oxide synthesized by the hydrothermal method as a support showed high catalytic activity and high selectivity to N 2 at low temperatures (18% NH 3 conversion with 100% N 2 selectivity at 25 °C) and at high temperatures (100% NH 3 conversion with 95% N 2 selectivity at 245 °C). Important roles of Brønsted acid sites and formation of active oxygen sites in improving N 2 selectivity were revealed in this study. To the best of our knowledge, this is the first report of efficient catalysts that presented high NH 3 conversion with high N 2 selectivity at 25 °C which will offer great scopes for commercial applications related to control of odors. In addition, this breakthrough finding that acid sites would greatly affect N 2 selectivity and catalytic activity will provide a new trend in designing efficient catalysts not only for SCO of NH 3 but also for the other selective catalytic oxidation.

Dehydrative Allylation of Amine with Allyl Alcohol by Titanium Oxide Supported Molybdenum Oxide Catalyst
Yoshihiro Kon, Takuya Nakashima, Tadahiro Fujitani, Toru Murayama, Wataru Ueda
SYNLETT, 30, 3, 287, 292, GEORG THIEME VERLAG KG, 2019年02月, ［査読有り］
英語, 研究論文（学術雑誌）, The dehydrative allylation from allyl alcohol with amines to generate various allyl amines by MoO3/TiO2 solid catalyst is described. The catalyst can be reused at least three times without a decrease of activity.

W₄V₃O₁₉複合酸化物のイオン交換によるミクロ細孔性質制御およびそのNH₃-SCR触媒活性
神山 曜帆, Zhang Zhenxing, 石川 理史, 猪股 雄介, 村山 徹, 上田 渉
石油学会 年会・秋季大会講演要旨集, 2019, 0, 174, 174, 公益社団法人 石油学会, 2019年, ［査読有り］
日本語,

ミクロ細孔性W₄V₃O₁₉複合酸化物（WVO）は、アンモニアを用いたSCRに対し高い触媒活性を示す。本研究では、WVOにTiやCuでイオン交換することでミクロ細孔容積が顕著に増大することを見出した。イオン交換後の試料は本反応に対し高い触媒活性、安定性を示した。発表ではイオン交換後試料の物性解析と触媒反応について、その詳細を述べる。

4価バナジウムを含んだバルク酸化バナジウム触媒の低温(150^oC以下)におけるNH₃-SCR活性
猪股 雄介, 清永 英嗣, 盛田 啓一郎, 吉田 和広, 窪田 博愛, 鳥屋尾 隆, 清水 研一, 春田 正毅, 村山 徹
石油学会 年会・秋季大会講演要旨集, 2019, 0, 175, 175, 公益社団法人 石油学会, 2019年, ［査読有り］
日本語,

150^oC以下での低温脱硝を目指し、バルク酸化バナジウムをベースとしたNH₃-SCR触媒を検討した。前駆体にバナジウムシュウ酸錯体を用い、焼成温度を270^oC、焼成時間を1-4hとすることで4価および5価バナジウム成分が共存した酸化バナジウム触媒を合成した。この触媒のNH₃-SCR活性を測定したところ、酸化チタン担持酸化バナジウム触媒および5価バナジウムのみからなるV₂O₅触媒と比較し、NO転化率および反応速度の増大が確認された。4価バナジウム成分が存在することによる活性化エネルギーの低下に起因することが示唆された。

Low-temperature NH3-SCR Activity of Nanoparticulate Gold Supported on a Metal Oxide
Yusuke Inomata, Makoto Mino, Shinichi Hata, Eiji Kiyonaga, Keiichiro Morita, Kenji Hikino, Kazuhiro Yoshida, Masatake Haruta, Toru Murayama
Journal of the Japan Petroleum Institute, 62, 5, 234, 243, 2019年, ［査読有り］
研究論文（学術雑誌）, The development of catalysts that can work to reduce NOx, the main pollutant produced from power plants and boiler, under ambient conditions at a low reaction temperature has been required. The NH3-SCR activity of metal oxide-supported gold catalysts was assessed to develop NH3-SCR catalysts working at low temperatures. Au/CuO showed NH3-SCR activity at 100°C (NO conversion = 20%, N2 selectivity = ca. 100%), though the production of N2O as a by-product caused by NH3 oxidation was observed at a higher reaction temperature. The deposition of 0.1 wt.% of gold on CuO was enough for NH3-SCR to proceed and that NH3 oxidation proceeded with increase in the loading amount of gold (< 0.5 %) at a high reaction temperature. Although the NH3-SCR activities of Pt/CuO and Pd/CuO were measured, Au/CuO showed better activity than those of other precious metal catalysts. Tested binary metal oxide-supported gold catalysts showed that 1 wt.%Au/10 wt.%CuO/Al2O3 showed the largest N3 yield (45%) due to the introduction of other metal oxide species to CuO.

金属酸化物担持金ナノ粒子が示す低温NH₃-SCR活性
猪股 雄介, 美濃 真, 秦 慎一, 清永 英嗣, 盛田 啓一郎, 引野 健治, 吉田 和広, 春田 正毅, 村山 徹
Ｊｏｕｒｎａｌ ｏｆ ｔｈｅ Ｊａｐａｎ Ｐｅｔｒｏｌｅｕｍ Ｉｎｓｔｉｔｕｔｅ, 62, 5, 234, 243, 公益社団法人 石油学会, 2019年, ［査読有り］
英語, 研究論文（学術雑誌）,

石炭火力発電所あるいは工業用ボイラーでの燃焼活動によって生成する窒素酸化物（NO_x）の効率的な除去が望まれている。その方策としてアンモニアを還元剤として用いたNH₃-SCR（Selective Catalytic Reduction）が挙げられるが，低温で活性を示す実用触媒の開発が急務の課題となっている。本研究では，金属酸化物担持金ナノ粒子の低温脱硝触媒としての可能性を検討した。様々な金属酸化物に担持した金ナノ粒子のNH₃-SCRを検討したところ，1 wt%Au/CuOが100 ℃でNO転化率20 %，N₂選択率約100 %を示すことが明らかとなった。一方，200 ℃では金を担持することで起こるアンモニア酸化反応に起因し，副生成物としてN₂Oが生成することが明らかとなった。他の貴金属担持触媒（Pt/CuO，Pd/CuO）についても同様に活性検討を行ったが，低温（100～120 ℃）ではAu/CuOが最も高い活性を示した。さらに，2元金属酸化物担持金ナノ粒子触媒のNH₃-SCRを検討し，1 wt%Au/10 wt%CuO/Al₂O₃が最も高いN₂収率（45 %）を示すことが明らかとなった。

Control of catalytic nanoparticle synthesis: general discussion.
Adishev A, Arrigo R, Baletto F, Bordet A, Bukhtiyarov V, Carosso M, Catlow R, Conway M, Davies J, Davies P, De Masi D, Demirci C, Edwards JK, Friend C, Gallarati S, Hargreaves J, Huang H, Hutchings G, Lai S, Lamberti C, Macino M, Marchant D, Murayama T, Odarchenko Y, Peron J, Prati L, Quinson J, Richards N, Rogers S, Russell A, Selvam P, Shah P, Shozi M, Skylaris CK, Soulantica K, Spolaore F, Tooze B, Torrente-Murciano L, Trunschke A, Venezia B, Walker J, Whiston K
Faraday discussions, 208, 471, 495, 2018年09月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）

The challenges of characterising nanoparticulate catalysts: general discussion.
Arrigo R, Badmus K, Baletto F, Boeije M, Bowker M, Brinkert K, Bugaev A, Bukhtiyarov V, Carosso M, Catlow R, Chanerika R, Davies PR, Dononelli W, Freund HJ, Friend C, Gallarati S, Gates B, Genest A, Gibson EK, Hargreaves J, Helveg S, Huang H, Hutchings G, Irvine N, Johnston R, Lai S, Lamberti C, Macginley J, Marchant D, Murayama T, Nome R, Odarchenko Y, Quinson J, Rogers S, Russell A, Said S, Sermon P, Shah P, Simoncelli S, Soulantica K, Spolaore F, Tooze B, Torrente-Murciano L, Trunschke A, Willock D, Zhang J
Faraday discussions, 208, 339, 394, 2018年09月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）

A zeolitic vanadotungstate family with structural diversity and ultrahigh porosity for catalysis
Zhenxin Zhang, Qianqian Zhu, Masahiro Sadakane, Toru Murayama, Norihito Hiyoshi, Akira Yamamoto, Shinichi Hata, Hisao Yoshida, Satoshi Ishikawa, Michikazu Hara, Wataru Ueda
NATURE COMMUNICATIONS, 9, 1, 3789, 3789, NATURE PUBLISHING GROUP, 2018年09月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, Design of the structure and composition of crystalline microporous inorganic oxides is of great importance in catalysis. Developing new zeolites is one approach towards this design because of the tunable pore system and high thermal stability. Zeolites are limited to main group elements, which limits their applications in redox catalysis. Another promising choice is zeolitic transition metal oxides providing both porosity and redox activity, thereby further expanding the diversity of porous materials. However, the examples of zeolitic transition metal oxides are rare. Here, we report a new class of zeolitic vanadotungstates with tunable frameworks exhibiting a large porosity and redox activity. The assembly of [W4O16](8-) units with VO2+ forms two isomeric porous frameworks. Owing to the complex redox properties and open porosity, the vanadotungstates efficiently catalyse the selective reduction of NO by NH3. This finding provides an opportunity for design and synthesis of inorganic multifunctional materials for future catalytic applications.

Control of catalytic nanoparticle synthesis: general discussion
Aldiar Adishev, Rosa Arrigo, Francesca Baletto, Alexis Bordet, Valerii Bukhtiyarov, Michele Carosso, Richard Catlow, Matthew Conway, Josh Davies, Philip Davies, Deborah De Masi, Cansunur Demirci, Jennifer K. Edwards, Cynthia Friend, Simone Gallarati, Justin Hargreaves, Haoliang Huang, Graham Hutchings, Stanley Lai, Carlo Lamberti, Margherita Macino, David Marchant, Toru Murayama, Yaroslav Odarchenko, Jennifer Peron, Laura Prati, Jonathan Quinson, Nia Richards, Scott Rogers, Andrea Russell, Parasuraman Selvam, Parag Shah, Mzamo Shozi, Chris-Kriton Skylaris, Katerina Soulantica, Federico Spolaore, Bob Tooze, Laura Torrente-Murciano, Annette Trunschke, Baldassarre Venezia, James Walker, Keith Whiston
FARADAY DISCUSSIONS, 208, 471, 495, ROYAL SOC CHEMISTRY, 2018年08月, ［査読有り］
英語

The challenges of characterising nanoparticulate catalysts: general discussion
Rosa Arrigo, Kassim Badmus, Francesca Baletto, Maurits Boeije, Michael Bowker, Katharina Brinkert, Aram Bugaev, Valerii Bukhtiyarov, Michele Carosso, Richard Catlow, Revana Chanerika, Philip R. Davies, Wilke Dononelli, Hans-Joachim Freund, Cynthia Friend, Simone Gallarati, Bruce Gates, Alexander Genest, Emma K. Gibson, Justin Hargreaves, Stig Helveg, Haoliang Huang, Graham Hutchings, Nicola Irvine, Roy Johnston, Stanley Lai, Carlo Lamberti, Joseph Macginley, David Marchant, Toru Murayama, Rene Nome, Yaroslav Odarchenko, Jonathan Quinson, Scott Rogers, Andrea Russell, Said Said, Paul Sermon, Parag Shah, Sabrina Simoncelli, Katerina Soulantica, Federico Spolaore, Bob Tooze, Laura Torrente-Murciano, Annette Trunschke, David Willock, Jiaguang Zhang
FARADAY DISCUSSIONS, 208, 339, 394, ROYAL SOC CHEMISTRY, 2018年08月, ［査読有り］
英語

W-Ti-O Mixed Metal Oxide Catalyzed Dehydrative Cross-etherification of Alcohols
Akira Yada, Toru Murayama, Jun Hirata, Takuya Nakashima, Masanori Tamura, Yoshihiro Kon, Wataru Ueda
CHEMISTRY LETTERS, 47, 4, 447, 449, CHEMICAL SOC JAPAN, 2018年04月, ［査読有り］
英語, 研究論文（学術雑誌）, A dehydrative cross-etherification reaction of two different alcohols is achieved in the presence of hydrothermally synthesized tungsten-titanium mixed metal oxide (W-Ti-O) catalyst. The reaction is environmentally benign: organic solvent is not necessary and the catalyst is readily recovered and reusable.

Carbon Monoxide Oxidation by Polyoxometalate-Supported Gold Nanoparticulate Catalysts: Activity, Stability, and Temperature- Dependent Activation Properties
Takuya Yoshida, Toru Murayama, Norihito Sakaguchi, Mitsutaka Okumura, Tamao Ishida, Masatake Haruta
Angewandte Chemie, 57, 6, 1523, 1527, Wiley-Blackwell, 2018年02月05日, ［査読有り］
英語, 研究論文（学術雑誌）, Nanoparticulate gold supported on a Keggin-type polyoxometalate (POM), Cs4[α-SiW12O40]⋅n H2O, was prepared by the sol immobilization method. The size of the gold nanoparticles (NPs) was approximately 2 nm, which was almost the same as the size of the gold colloid precursor. Deposition of gold NPs smaller than 2 nm onto POM (Au/POM) was essential for a high catalytic activity for CO oxidation. The temperature for 50 % CO conversion was −67 °C. The catalyst showed extremely high stability for at least one month at 0 °C with full conversion. The catalytic activity and the reaction mechanism drastically changed at temperatures higher than 40 °C, showing a unique behavior called a U-shaped curve. It was revealed by IR measurement that Auδ+ was a CO adsorption site and that adsorbed water promoted CO oxidation for the Au/POM catalyst. This is the first report on CO oxidation utilizing Au/POMs catalysts, and there is a potential for expansion to various gas-phase reactions.

Carbon Monoxide Oxidation by Polyoxometalate-Supported Gold Nanoparticulate Catalysts: Activity, Stability, and Temperature-Dependent Activation Properties
Takuya Yoshida, Toru Murayama, Norihito Sakaguchi, Mitsutaka Okumura, Tamao Ishida, Masatake Haruta
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 57, 6, 1523, 1527, WILEY-V C H VERLAG GMBH, 2018年02月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, Nanoparticulate gold supported on a Keggin-type polyoxometalate (POM), Cs-4[-SiW12O40]nH(2)O, was prepared by the sol immobilization method. The size of the gold nanoparticles (NPs) was approximately 2nm, which was almost the same as the size of the gold colloid precursor. Deposition of gold NPs smaller than 2nm onto POM (Au/POM) was essential for a high catalytic activity for CO oxidation. The temperature for 50% CO conversion was -67 degrees C. The catalyst showed extremely high stability for at least one month at 0 degrees C with full conversion. The catalytic activity and the reaction mechanism drastically changed at temperatures higher than 40 degrees C, showing a unique behavior called a U-shaped curve. It was revealed by IR measurement that Au+ was a CO adsorption site and that adsorbed water promoted CO oxidation for the Au/POM catalyst. This is the first report on CO oxidation utilizing Au/POMs catalysts, and there is a potential for expansion to various gas-phase reactions.

低温(200℃以下)での脱硝を目的としたV₂O₅触媒の開発
猪股 雄介, 秦 慎一, 清永 英嗣, 盛田 啓一郎, 吉田 和広, 春田 正毅, 村山 徹
石油学会 年会・秋季大会講演要旨集, 2018, 0, 184, 184, 公益社団法人 石油学会, 2018年, ［査読有り］
日本語, NH₃を還元剤とする選択的触媒還元法（NH₃-SCR）は、NO_xを無害化する方法として知られている。現在使用されている触媒の動作温度は高く、低温でも作用する脱硝プロセスの設計が望まれている。本研究では、酸化バナジウム触媒を調製し、低温条件下における触媒活性を調べた。その結果、150℃で90%以上の高いNO転化率を示した。

Identification of the catalytically active component of Cu-Zr-O catalyst for the hydrogenation of levulinic acid to gamma-valerolactone
Satoshi Ishikawa, Daniel R. Jones, Sarwat Iqbal, Christian Reece, David J. Morgan, David J. Willock, Peter J. Miedziak, Jonathan K. Bartley, Jennifer K. Edwards, Toru Murayama, Wataru Ueda, Graham J. Hutchings
GREEN CHEMISTRY, 19, 1, 225, 236, ROYAL SOC CHEMISTRY, 2017年01月, ［査読有り］
英語, 研究論文（学術雑誌）, Cu-ZrO2 catalysts were synthesized by the methanothermal (Me) and oxalate gel precipitation (Og) methods. Detailed characterization of the catalysts synthesized by the Me method shows that these contain only Cu substituted into the tetragonal ZrO2 lattice. For catalysts prepared using the Og method Cu is found not only in the tetragonal ZrO2 lattice but also in the form of CuO particles on the zirconia surface. When these materials were tested for the hydrogenation of levulinic acid (LA) to.-valerolactone (GVL) it was found that Me materials show no catalytic activity, whereas GVL was formed using Og catalysts. A reduction treatment of the Og catalysts prior to use resulted in a marked increase in the catalytic activity, however, no activity increase was observed when the Me material was exposed to a similar treatment before testing. Based on these results and characterization data, we conclude that the catalytically active component of Cu-ZrO2 catalysts for the hydrogenation of LA is reduced Cu particles dispersed on the catalyst surface with strong interaction with the Cu incorporated zirconia support, while the role of Cu in the zirconia lattice is to improve the adhesion of these particles and maintain their dispersion.

Hydrothermal synthesis of a layered-type W-Ti-O mixed metal oxide and its solid acid activity
Toru Murayama, Kiyotaka Nakajima, Jun Hirata, Kaori Omata, Emiel J. M. Hensen, Wataru Ueda
CATALYSIS SCIENCE & TECHNOLOGY, 7, 1, 243, 250, ROYAL SOC CHEMISTRY, 2017年01月, ［査読有り］
英語, 研究論文（学術雑誌）, A layered-type W-Ti-O mixed oxide was synthesized by hydrothermal synthesis from an aqueous solution of ammonium metatungstate and titanium sulfate. To avoid the formation of titania, oxalic acid was used as a reductant. Optimized synthesis led to rod-like particles comprised of MO6 (M = W, Ti) octahedra connected in a corner-sharing fashion in the c-direction and in the form of micropore-containing {W6O21} units in the a-b plane. The surface area, acidity and acid catalytic activity (alkylation) increased with the amount of the layered-type W-Ti-O phase. Strong Bronsted acid sites formed due to the thermal release of ammonia from the uncalcined precursor. Calcination at 400 degrees C led to the highest acidity and alkylation activity. Alkylation of benzyl alcohol and toluene led to heavy product formation due to over-alkylation of the product. The selectivity to the mono-alkylated product was improved by the addition of water, which competes with the selectively formed products for adsorption on the acid sites. FT-IR measurements showed that the layered-type W-Ti-O possesses Bronsted acid sites and at least two different Lewis acid sites. The stronger Lewis acid sites can be converted into Bronsted acid sites in the presence of water, and the weaker Lewis acid sites functioned in the presence of water. This water tolerance of Lewis acid sites is an important characteristic of layered-type W-Ti-O, as it allows the bifunctional catalyst to convert 1,3-DHA into lactic acid in water.

NH3-efficient ammoxidation of toluene by hydrothermally synthesized layered tungsten-vanadium complex metal oxides
Yoshinori Goto, Ken-ichi Shimizu, Kenichi Kon, Takashi Toyao, Toru Murayama, Wataru Ueda
JOURNAL OF CATALYSIS, 344, 346, 353, ACADEMIC PRESS INC ELSEVIER SCIENCE, 2016年12月, ［査読有り］
英語, 研究論文（学術雑誌）, Hydrothermally synthesized W-V-O layered metal oxides (W-V-O) are studied for the vapor phase ammoxidation of toluene to benzonitrile (PhCN). Under similar conversion levels at 400 degrees C, W-V-O shows higher selectivity (based on toluene) to PhCN and lower selectivity to COx than conventional V-based catalysts (V2O5 and VOx/TiO2). Under the conditions of high contact time, W-V-O shows 99.7% conversion of toluene and 93.5% selectivity to PhCN. Another important feature of W-V-O is high NH3-utilization efficiency in ammoxidation, which originates from the lower activity of W-V-O for NH3 oxidation than that of V2O5. In situ infrared (IR) study shows that toluene is oxidized by the surface oxygen species of W83V17 to yield benzaldehyde which undergoes the reaction with adsorbed NH3 to give benzonitrile. Model reaction studies with W-V-O suggest that the rate of NH3 conversion to PhCN in the benzaldehyde + NH3 + O-2 reaction is 3 times higher than the rate of NH3 oxidation to N-2 in the NH3 + 02 reaction. It is shown that the high NH3-efficiency of W-V-O is caused by the preferential reaction of NH3 in PhCHO + NH3 + O-2 over NH3+O-2 reaction. (C) 2016 Elsevier Inc. All rights reserved.

Correlation between catalytic activity of supported gold catalysts for carbon monoxide oxidation and metal–oxygen binding energy of the support metal oxides
Takashi Fujita, Masanori Horikawa, Takashi Takei, Toru Murayama, Masatake Haruta
Chinese Journal of Catalysis, 37, 10, 1651, 1655, Elsevier {BV}, 2016年10月, ［査読有り］
英語, 研究論文（学術雑誌）, The effect of a wide variety of metal oxide (MOx) supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co-precipitation and deposition-precipitation methods and under identical calcination conditions, supported gold catalysts were prepared on a wide variety of MOx supports, and the temperature for 50% conversion was measured to qualitatively evaluate the catalytic activities of these simple MOx and supported Au catalysts. Furthermore, the difference in these temperatures for the simple MOx compared to the supported Au catalysts is plotted against the metal-oxygen binding energies of the support MOx. A clear volcano-like correlation between the temperature difference and the metal-oxygen binding energies is observed. This correlation suggests that the use of MOx with appropriate metal-oxygen binding energies (300-500 kJ/atom O) greatly improves the catalytic activity of MOx by the deposition of Au NPs. (C) 2016, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

Preparation of gold nanoparticles supported on Nb2O5 by deposition precipitation and deposition reduction methods and their catalytic activity for CO oxidation
Toru Murayama, Masatake Haruta
CHINESE JOURNAL OF CATALYSIS, 37, 10, 1694, 1701, SCIENCE PRESS, 2016年10月, ［査読有り］
英語, 研究論文（学術雑誌）, Nanoparticulate gold catalysts supported on niobium oxides (Nb2O5) were prepared by different deposition methods. The deposition precipitation (DP) method, DP method with urea, deposition reduction (DR) method and one-pot method were used to prepare a 1 wt% Au/Nb2O5 catalyst. Layered-type Nb2O5 synthesized by a hydrothermal method (Nb2O5(HT)) was the most suitable as a support among various types of Nb2O5 including commercially available Nb2O5 samples. It appeared that the large BET surface area of Nb2O5(HT) enabled the dispersion of gold as nanoparticles (NPs). Gold NPs with a mean diameter of about 5 nm were deposited by both the DP method and DR method on Nb2O5(HT) under an optimized condition. The temperature for 50% CO conversion for Au/Nb2O5(HT) prepared by the DR method was 73 degrees C. Without deposition of gold, Nb2O5(HT) showed no catalytic activity for CO oxidation even at 250 degrees C. Therefore, the enhancement of the activity by deposition of gold was remarkable. This simple Au/Nb2O5 catalyst will expand the types of gold catalysts to acidic supports, giving rise to new applications. (C) 2016, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

Correlation between catalytic activity of supported gold catalysts for carbon monoxide oxidation and metal-oxygen binding energy of the support metal oxides
Takashi Fujita, Masanori Horikawa, Takashi Takei, Toru Murayama, Masatake Haruta
CHINESE JOURNAL OF CATALYSIS, 37, 10, 1651, 1655, SCIENCE PRESS, 2016年10月, ［査読有り］
英語, 研究論文（学術雑誌）, The effect of a wide variety of metal oxide (MOx) supports has been discussed for CO oxidation on nanoparticulate gold catalysts. By using typical co-precipitation and deposition-precipitation methods and under identical calcination conditions, supported gold catalysts were prepared on a wide variety of MOx supports, and the temperature for 50% conversion was measured to qualitatively evaluate the catalytic activities of these simple MOx and supported Au catalysts. Furthermore, the difference in these temperatures for the simple MOx compared to the supported Au catalysts is plotted against the metal-oxygen binding energies of the support MOx. A clear volcano-like correlation between the temperature difference and the metal-oxygen binding energies is observed. This correlation suggests that the use of MOx with appropriate metal-oxygen binding energies (300-500 kJ/atom O) greatly improves the catalytic activity of MOx by the deposition of Au NPs. (C) 2016, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

Synthesis of Trigonal Mo–V–M3rd–O (M3rd = Fe, W) Catalysts by Using Structure-Directing Agent and Catalytic Performances for Selective Oxidation of Ethane
Satoshi Ishikawa, Toru Murayama, Masahiro Kumaki, Masaya Tashiro, Zhenxin Zhang, Akihiro Yoshida, Wataru Ueda
Topics in Catalysis, 59, 17-18, 1477, 1488, Springer Nature, 2016年10月, ［査読有り］
英語, 研究論文（学術雑誌）, Crystalline Mo-V-M(3)rd-O (M(3)rd = Fe, W) catalysts (MoVFeO and MoVWO) with trigonal symmetry were successfully obtained by a hydrothermal method in the presence of structure-directing agents (ammonium cation and ethylammonium cation) and their catalytic performances for selective oxidation of ethane were compared with trigonal Mo3VOx catalyst (MoVO). Fe and W were uniformly distributed throughout the rod-shaped crystals. XRD, Raman, XRD simulation, and Rietveld analysis revealed that MoVFeO contained Fe in a heptagonal channel and W in MoVWO substituted Mo in {Mo6O21}(6-) pentagonal unit in the structure. MoVWO catalyst showed comparable catalytic activity with MoVO for the selective oxidation of ethane. On the other hand, catalytic performance of MoVFeO was far less compared with those of MoVO and MoVWO. The picture that the catalytic reaction occurs at the specific part in the structure could be visualized.

Preparation of gold nanoparticles supported on Nb2O5 by deposition precipitation and deposition reduction methods and their catalytic activity for CO oxidation
Toru Murayama, Masatake Haruta
CHINESE JOURNAL OF CATALYSIS, 37, 10, 1694, 1701, SCIENCE PRESS, 2016年10月, ［査読有り］
英語, 研究論文（学術雑誌）, Nanoparticulate gold catalysts supported on niobium oxides (Nb2O5) were prepared by different deposition methods. The deposition precipitation (DP) method, DP method with urea, deposition reduction (DR) method and one-pot method were used to prepare a 1 wt% Au/Nb2O5 catalyst. Layered-type Nb2O5 synthesized by a hydrothermal method (Nb2O5(HT)) was the most suitable as a support among various types of Nb2O5 including commercially available Nb2O5 samples. It appeared that the large BET surface area of Nb2O5(HT) enabled the dispersion of gold as nanoparticles (NPs). Gold NPs with a mean diameter of about 5 nm were deposited by both the DP method and DR method on Nb2O5(HT) under an optimized condition. The temperature for 50% CO conversion for Au/Nb2O5(HT) prepared by the DR method was 73 degrees C. Without deposition of gold, Nb2O5(HT) showed no catalytic activity for CO oxidation even at 250 degrees C. Therefore, the enhancement of the activity by deposition of gold was remarkable. This simple Au/Nb2O5 catalyst will expand the types of gold catalysts to acidic supports, giving rise to new applications. (C) 2016, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

Deposition of Gold Nanoparticles on Niobium Pentoxide with Different Crystal Structures for Room-Temperature Carbon Monoxide Oxidation
Toru Murayama, Wataru Ueda, Masatake Haruta
CHEMCATCHEM, 8, 16, 2620, 2624, WILEY-V C H VERLAG GMBH, 2016年08月, ［査読有り］
英語, 研究論文（学術雑誌）, Nanoparticulate gold catalysts (NPGCs) supported on niobium oxides (Nb2O5) were prepared by different deposition methods. Au nanoparticles (NPs) with a mean diameter of approximately 5 nm were deposited by conventional deposition methods, which include the deposition-precipitation (DP) and deposition-reduction (DR) methods, on layered-type Nb2O5 that possesses a deformed orthorhombic structure. Moreover, Au NPs with a mean diameter of approximately 2.7 nm could be deposited by the sol immobilization method on several crystalline forms of Nb2O5 (deformed orthorhombic, pseudohexagonal, and orthorhombic). NPGCs deposited on deformed orthorhombic Nb2O5 had a higher catalytic activity for CO oxidation. The temperature for 50% CO conversion was 11 degrees C for 1 wt% Au/Nb2O5 (deformed orthorhombic) prepared by the sol immobilization method, and the CO conversion was 91% at 28 degrees C. As far as we know, this is the first report of highly active Au NPGCs (smaller than 3 nm in diameter) supported on Nb2O5. NPGCs supported on acidic metal oxides will expand the utilization of gold catalysts for new applications.

Role of Crystalline Structure in Allyl Alcohol Selective Oxidation over Mo3VOx Complex Metal Oxide Catalysts
Toru Murayama, Benjamin Katryniok, Svetlana Heyte, Marcia Araque, Satoshi Ishikawa, Franck Dumeignil, Sebastien Paul, Wataru Ueda
CHEMCATCHEM, 8, 14, 2415, 2420, WILEY-V C H VERLAG GMBH, 2016年07月, ［査読有り］
英語, 研究論文（学術雑誌）, The role of the crystalline phase of Mo3VOx in the catalytic oxidation of allyl alcohol over four kinds of crystalline (orthorhombic, trigonal, tetragonal, amorphous) Mo3VOx catalysts was investigated to determine the active sites for the reactions. Tetragonal Mo3VOx was found less active for the formation of acrylic acid from allyl alcohol, although acrolein was obtained selectively at higher temperature. For orthorhombic and trigonal Mo3VOx catalyst, allyl alcohol converted to acrolein and propanal competitively at the mouth of the heptagonal channel over the a-b plane of the rod-type crystalline particles, and these aldehydes were oxidized consecutively to acrylic acid. Acrylic acid was formed effectively at increased reaction temperature over orthorhombic, trigonal and amorphous Mo3VOx catalysts, and the maximum yields of acrylic acid were 73% for the orthorhombic Mo3VOx catalyst and 72% for the trigonal Mo3VOx catalyst at 350 degrees C.

Hydrothermal synthesis of W–Ta–O complex metal oxides by assembling MO6 (M=W or Ta) octahedra and creation of solid acid
Toru Murayama, Nozomi Kuramata, Wataru Ueda
Journal of Catalysis, 339, 143, 152, Elsevier {BV}, 2016年07月, ［査読有り］
英語, 研究論文（学術雑誌）, Layered-type tungsten and tantalum oxides (W-Ta-O) were synthesized by the hydrothermal method. The synthesized W-Ta-O showed characteristic peaks at 2 theta = 22.7 degrees and 46.2 in an X-ray diffraction pattern (Cu K alpha), indicating linear corner sharing of MO6 (M = W, Ta) octahedra in the c-direction. The same layered-type materials were obtained with a wide range of W and Ta composition ratios using soluble Lindqvist-type tantalum polyoxometalate (Na-8(Ta6O19)center dot 24.5H(2)O). Na+ cations of as-synthesized W-Ta-O were replaced with NH4+ and then calcined at 500 degrees C to form Bronsted acid sites. The catalytic activity of W-Ta-O increased with increasing W ratio, suggesting that strong acid sites were generated. From Raman and adsorption measurements of W-Ta-O with various crystalline structures, it was revealed that the crystalline motif of W-Ta-O in the a-b plane was an interconnection of MO6 (M = W, Ta) octahedra and (M6O21) pentagonal units and micropore channels, but without long-range order. (C) 2016 Elsevier Inc. All rights reserved.

ChemInform Abstract: Synthesis of Vanadium-Incorporated, Polyoxometalate-Based Open Frameworks and Their Applications for Cathode-Active Materials.
Zhenxin Zhang, Hirofumi Yoshikawa, Zhongyue Zhang, Toru Murayama, Masahiro Sadakane, Yasunori Inoue, Wataru Ueda, Kunio Awaga, Michikazu Hara
ChemInform, 47, 21, Wiley-Blackwell, 2016年05月, ［査読有り］
研究論文（学術雑誌）

Synthesis of Vanadium-Incorporated, Polyoxometalate-Based Open Frameworks and Their Applications for Cathode-Active Materials
Zhenxin Zhang, Hirofumi Yoshikawa, Zhongyue Zhang, Toru Murayama, Masahiro Sadakane, Yasunori Inoue, Wataru Ueda, Kunio Awaga, Michikazu Hara
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2016, 8, 1242, 1250, WILEY-V C H VERLAG GMBH, 2016年03月, ［査読有り］
英語, 研究論文（学術雑誌）, The tuning of the chemical composition of polyoxometalate (POM)-based open framework materials with the same structure, leading to a property change of the materials, is interesting. Here, we report the synthesis of a series of vanadium-incorporated, E-Keggin polyoxometalate-based open framework materials by using a hydrothermal method. The resulting materials were characterized by powder X-ray diffraction, FTIR spectroscopy, scanning electron microscopy, energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and elemental analysis. Our results indicate that V is successfully incorporated into the frameworks of the materials. The introduced amount of V can be adjusted by controlling the addition of the precursor V compounds. The performances of these materials as cathode materials for Li-ion batteries have been tested. Incorporation of V can improve the cycle performance. After the 20th cycle of the charge-discharge process, the materials were transformed to the Li2MoO4 phase.

Hydrothermal synthesis of microporous W–V–O as an efficient catalyst for ammoxidation of 3-picoline
Yoshinori Goto, Ken-ichi Shimizu, Toru Murayama, Wataru Ueda
Applied Catalysis A: General, 509, 118, 122, Elsevier {BV}, 2016年01月, ［査読有り］
英語, 研究論文（学術雑誌）, W-V complex metal oxide (W-V-O) was prepared by hydrothermal synthesis method. Characterization by XRD, XPS, ICP-AES, N-2 adsorption, and STEM showed that W-V-O had a layered structure with micropore. W-V-O was tested for the vapor phase ammoxidation of 3-picoline (PIC) to 3-cyanopyridine (CP) and compared with VOx/WO3 catalyst prepared by impregnation method and other V-based catalysts which were reported to be efficient for this reaction. W-added vanadium oxides, W-V-O and VOx/WO3, showed higher CP selectivity than conventional catalysts such as VOx/TiO2. The W-V-O catalyst showed the highest CP selectivity of 99.5% at full PIC conversion. Kinetic studies showed that CP was the primary product and small amount of pyridine and CO2 were produced from CP. The reaction by W-V-O in low NH3 concentration condition or without co-feeding of water was also studied to evaluate the catalytic performance of W-V-O in industrially relevant conditions. (C) 2015 Elsevier B.V. All rights reserved.

Direct oxidative transformation of glycerol to acrylic acid over Nb-based complex metal oxide catalysts
Kaori Omata, Keeko Matsumoto, Toru Murayama, Wataru Ueda
CATALYSIS TODAY, 259, 205, 212, ELSEVIER SCIENCE BV, 2016年01月, ［査読有り］
英語, 研究論文（学術雑誌）, W-V-Nb-0 complex metal oxides having a structure like that of orthorhombic Mo3VOx, were found to be an efficient catalyst for the gas-phase direct oxidative transformation of glycerol to acrylic acid. The catalysts with various compositions were facilely synthesized by hydrothermal method. The W-Nb-0 catalyst without V component, mainly promoted the glycerol dehydration, giving acrolein selectively. Since Nb-0 catalyst showed poor activity for the reaction, the introduction of W into the Nb-0 catalysts was found effective for improving the activity for the dehydration of glycerol to acrolein. This is mainly due to the increase of Bronsted acidity by the combination of W and Nb. When V was incorporated into the framework of W-Nb-0, the resulting catalyst was found to prominently promote the formation of acrylic acid in the glycerol transformation in the presence of O-2, while showed no effect on the dehydration of glycerol to acrolein. It was also found that V acts as an oxidation site only when glycerol is completely reacted. The optimum elemental composition for the reaction was W2.2V0.4Nb2.4O14 giving ca. 46% one path yield of acrylic acid and this catalytic performance was further improved by the surface modification with phosphoric acid, achieving ca. 60% one path yield of acrylic acid. (C)2015 Elsevier B.V. All rights reserved.

New crystalline complex metal oxides created by unit-synthesis and their catalysis based on porous and redox properties
Zhenxin Zhang, Satoshi Ishikawa, Yuta Tsuboi, Masahiro Sadakane, Toru Murayama, Wataru Ueda
FARADAY DISCUSSIONS, 188, 81, 98, ROYAL SOC CHEMISTRY, 2016年, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, The development of new complex metal oxides having structural complexity suitable for solid-state catalysis is of great importance in fundamental catalysis research and practical applications. However, examples of these materials are rare. Herein, we report two types of crystalline complex metal oxides with new structures and their catalytic properties. The first one is an all-inorganic 3-Keggin polyoxometalate-based material with intrinsic microporosity. The framework of the material is formed by the assembly of 3-Keggin polyoxomolybdate units with metal ion linkers in a diamondoid topology. The micropores of the material can be opened without change of the structures, and the material adsorbs small molecules. This material has both redox properties and acidity and can be applied to O-2 adsorption, selective oxidation of methacrolein, and hydrolysis of cellobiose. The other material is a crystalline metal oxide based on molecular nanowires. The hexagonal POM units stack along the c axis to form prismatic clusters as molecular wires. The molecular wires further assemble in a hexagonal fashion to form the crystals, and NH4+ and water are present in between the molecular wires. The material is active as an acid catalyst for cellobiose conversion.

Ultrathin inorganic molecular nanowire based on polyoxometalates
Zhenxin Zhang, Toru Murayama, Masahiro Sadakane, Hiroko Ariga, Nobuhiro Yasuda, Norihito Sakaguchi, Kiyotaka Asakura, Wataru Ueda
NATURE COMMUNICATIONS, 6, 7731, 7731, NATURE PUBLISHING GROUP, 2015年07月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, The development of metal oxide-based molecular wires is important for fundamental research and potential practical applications. However, examples of these materials are rare. Here we report an all-inorganic transition metal oxide molecular wire prepared by disassembly of larger crystals. The wires are comprised of molybdenum(VI) with either tellurium(IV) or selenium(IV): {(NH4)(2)[XMo6O21]}(n) (X = tellurium(IV) or selenium(IV)). The ultrathin molecular nanowires with widths of 1.2 nm grow to micrometre-scale crystals and are characterized by single-crystal X-ray analysis, Rietveld analysis, scanning electron microscopy, X-ray photoelectron spectroscopy, ultraviolet-visible spectroscopy, thermal analysis and elemental analysis. The crystals can be disassembled into individual molecular wires through cation exchange and subsequent ultrasound treatment, as visualized by atomic force microscopy and transmission electron microscopy. The ultrathin molecular wire-based material exhibits high activity as an acid catalyst, and the band gap of the molecular wire-based crystal is tunable by heat treatment.

Redox Treatment of Orthorhombic Mo29V11O112 and Relationships between Crystal Structure, Microporosity and Catalytic Performance for Selective Oxidation of Ethane
Satoshi Ishikawa, Daichi Kobayashi, Takeshi Konya, Shunpei Ohmura, Toru Murayama, Nobuhiro Yasuda, Masahiro Sadakane, Wataru Ueda
JOURNAL OF PHYSICAL CHEMISTRY C, 119, 13, 7195, 7206, AMER CHEMICAL SOC, 2015年04月, ［査読有り］
英語, 研究論文（学術雑誌）, Redox treatments of an orthorhombic Mo29V11O112 catalyst (MoVO) were conducted and its crystal structure, microporosity, and catalytic activity were investigated. TPR and TG revealed that MoVO evolved two kinds of lattice oxygen (alpha-oxygen and beta-oxygen) from the structure by reduction treatment. In the early stage of reduction, alpha-oxygen was evolved from the structure, causing expansion of the micropore channel. With further reduction, the atoms in the pentagonal [Mo6O21](6) unit moved toward the micropore channel, resulting in a decrease in micropore size. Expansion of the micropore drastically increased catalytic activity for selective oxidation of ethane, but the activity was decreased by a reduction in the micropore channel size. Strong relationships were found between crystal structure, microporosity, and catalytic activity for selective oxidation of ethane.

Synthesis of crystalline Mo–V–W–O complex oxides with orthorhombic and trigonal structures and their application as catalysts
Chuntian Qiu, Chen Chen, Satoshi Ishikawa, Zhenxin Zhang, Toru Murayama, Wataru Ueda
Catalysis, Structure {\&} Reactivity, 1, 2, 71, 77, Informa {UK} Limited, 2015年01月08日, ［査読有り］
研究論文（学術雑誌）

Synthesis of crystalline Mo-V-W-O complex oxides with orthorhombic and trigonal structures and their application as catalysts
Chuntian Qiu, Chen Chen, Satoshi Ishikawa, Zhenxin Zhang, Toru Murayama, Wataru Ueda
CATALYSIS STRUCTURE & REACTIVITY, 1, 2, 71, 77, TAYLOR & FRANCIS LTD, 2015年, ［査読有り］
英語, 研究論文（学術雑誌）, Crystalline Mo-V-W-O complex oxides with the orthorhombic or trigonal structure were synthesized by a hydrothermal method. Those Mo-V-W-O samples with various amounts of tungsten were characterized by inductively coupled plasma atomic emission spectroscopy, TEM, STEM-EDX, X-ray diffraction, Rietveld analysis and a N-2 adsorption method. It was found for the first case that an additional metal such as W can be successfully incorporated into the trigonal Mo-V-O structure by using (CH3CH2NH3)(2)Mo3O10. The alkylammonium cation acted as a structural stabilizer that was requisite for the formation of a trigonal structure when additional metal ions were present. For the orthorhombic Mo-V-W-O structure, introduction of W into the orthorhombic structure caused a rod segregation effect by which nanoscale crystals formed and the external surface area greatly increased. Additionally, these Mo-V-W-O materials were applied as catalysts for the gas phase selective oxidation of acrolein to acrylic acid. The best catalyst was assigned to the orthorhombic Mo-V-O-W7.5, which possessed an ordered arrangement of heptagonal and hexagonal channels and a large external surface area.

Selective carbon dioxide adsorption of ε-Keggin-type zincomolybdate-based purely inorganic 3D frameworks
Zhenxin Zhang, Masahiro Sadakane, Shin-ichiro Noro, Toru Murayama, Takashi Kamachi, Kazunari Yoshizawa, Wataru Ueda
J. Mater. Chem. A, 3, 2, 746, 755, Royal Society of Chemistry ({RSC}), 2015年, ［査読有り］
英語, 研究論文（学術雑誌）, Polyoxometalate-based 3D frameworks, Na1.5H11.4[ZnMo12O40{Zn-2}]center dot 5.5H(2)O and (NH4)(1.5)H-8.5-[ZnMo12O40{Zn-2}]center dot 6H(2)O, are synthesized in moderate yields. Rotation of the reactor under hydrothermal conditions is essential to improve the yield. The materials show zeolite-like selective molecule adsorption properties. Depending on the micropore aperture size of the materials, small molecules can be adsorbed in the materials, while large molecules cannot. The enthalpy of adsorption and DFT calculation indicate that the materials strongly interact with CO2, but weakly interact with CH4, due to electrostatic interactions between the materials and molecules. CO2/CH4 co-sorption experiments show that the materials can selectively adsorb CO2, and CO2 adsorption selectivity of the material with sodium cations is higher than that of the material with ammonium cations. The material with sodium ions can be utilized for gas chromatographic separation of CH4 and CO2.

Selective carbon dioxide adsorption of ε-Keggin-type zincomolybdate-based purely inorganic 3D frameworks
Zhenxin Zhang, Masahiro Sadakane, Shin-ichiro Noro, Toru Murayama, Takashi Kamachi, Kazunari Yoshizawa, Wataru Ueda
J. Mater. Chem. A, 3, 2, 746, 755, Royal Society of Chemistry ({RSC}), 2015年, ［査読有り］
英語, 研究論文（学術雑誌）, Polyoxometalate-based 3D frameworks, Na1.5H11.4[ZnMo12O40{Zn-2}]center dot 5.5H(2)O and (NH4)(1.5)H-8.5-[ZnMo12O40{Zn-2}]center dot 6H(2)O, are synthesized in moderate yields. Rotation of the reactor under hydrothermal conditions is essential to improve the yield. The materials show zeolite-like selective molecule adsorption properties. Depending on the micropore aperture size of the materials, small molecules can be adsorbed in the materials, while large molecules cannot. The enthalpy of adsorption and DFT calculation indicate that the materials strongly interact with CO2, but weakly interact with CH4, due to electrostatic interactions between the materials and molecules. CO2/CH4 co-sorption experiments show that the materials can selectively adsorb CO2, and CO2 adsorption selectivity of the material with sodium cations is higher than that of the material with ammonium cations. The material with sodium ions can be utilized for gas chromatographic separation of CH4 and CO2.

Catalysis field in orthorhombic Mo3VOx oxide catalyst for the selective oxidation of ethane, propane and acrolein
Satoshi Ishikawa, Xiaodong Yi, Toru Murayama, Wataru Ueda
CATALYSIS TODAY, 238, 35, 40, ELSEVIER SCIENCE BV, 2014年12月, ［査読有り］
英語, 研究論文（学術雑誌）, Orthorhombic Mo3VOx oxide catalysts in various crystal sizes with different external surface areas and the same micropore volumes were synthesized hydrothermally by adding sodium dodecyl sulphonate (SDS, C12H25SO3Na) to preparation solution and by changing synthesis temperature. The synthesized catalysts were then tested for the selective oxidations of ethane, propane, and acrolein, in order to clarity catalysis field for the reactions. It was found that ethane converted to ethene in the heptagonal channel in the structure of the catalyst and propane was also oxidized to COx in the heptagonal channel. Acrolein, on the other hand, was converted to acrylic acid at the mouth of the heptagonal channel. It is concluded that the heptagonal channel is all responsible for the catalysis for ethane, propane, and acrolein. However, the catalysis field is different in a reflection of the molecular size of the reactants. (C) 2014 Elsevier B.V. All rights reserved.

Hydrogen-transfer dehydration between alcohols over V2O3 and MoO2 catalysts for the formation of corresponding alkanes and aldehydes
Yoichi Nakamura, Toru Murayama, Wataru Ueda
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 394, 137, 144, ELSEVIER SCIENCE BV, 2014年11月, ［査読有り］
英語, 研究論文（学術雑誌）, Conversion of alcohols in a gas phase under N-2 flow at 573 K was carried out using V2O3 and MoO2 oxides with low valence oxidation states. It was found in the reaction of ethanol that equimolar amounts of ethane and acetaldehyde were catalytically formed as the main products over the oxides. Bi-products were small amounts of ethene and C4 compounds. Reactions of other alcohols (methanol, 1-propanol and 2-propanol) over the V2O3 and MoO2 catalysts also led to the equimolar formation of corresponding alkanes and aldehydes or ketone. It was confirmed by XRD and XPS that the low valence states of V2O3 and MoO2 were unchanged during the reactions and the oxides stably worked as the catalyst. Based on catalytic reaction results obtained under various reaction conditions (reaction temperature, contact time, introduction of H-2 and C2H4 into reaction stream) and on experiments of kinetic isotope effects on the ethanol reaction, a reaction scheme is proposed, in which hydrogen transfer reaction between two alcohol molecules adsorbed on metal-O2--metal sites on the surface of V2O3 and MoO2 catalysts takes place via 6-membered transition state, followed by dehydration. (C) 2014 Elsevier B.V. All rights reserved.

ChemInform Abstract: Preparation, Structural Characterization, and Ion-Exchange Properties of Two New Zeolite-like 3D Frameworks Constructed by ε-Keggin-Type Polyoxometalates with Binding Metal Ions, H11.4 [ZnMo12O40Zn2]1.5- and H7.5 [Mn0.2Mo12O40Mn2] 2.1
Zhenxin Zhang, Masahiro Sadakane, Toru Murayama, Norihito Sakaguchi, Wataru Ueda
ChemInform, 45, 39, no, no, Wiley-Blackwell, 2014年09月11日, ［査読有り］
英語, 研究論文（学術雑誌）, Two new ε-Keggin-type polyoxometalate-based 3D frameworks, Na 1.5H11.4[ε-ZnIIMoV 10.9MoVI1.1O40{ZnII} 2] and (NH4)2.1H7.5[ε-Mn II0.2MoV6MoVI 6O40{MnII}2], are prepared, and their structures are determined by powder X-ray diffraction, Fourier transform infrared, Raman spectroscopy, and elemental analysis. ε-Keggin-type polyoxomolybdate units, [ε-ZnMo12O40] and [ε-Mn0.2Mo12O40], are linked with Zn 2+ and Mn2+, respectively, in a tetrahedral fashion to form 3D frameworks. They show zeolite-like ion-exchange properties and redox properties. The ε-Keggin-based 3D framework shows high chemical composition diversity and can incorporate different elements in the framework. © 2014 American Chemical Society.

Investigation of the formation process of zeolite-like 3D frameworks constructed with ε-Keggin-type polyoxovanadomolybdates with binding bismuth ions and preparation of a nano-crystal.
Zhang Z, Sadakane M, Murayama T, Ueda W
Dalton transactions (Cambridge, England : 2003), 43, 36, 13584, 13590, Royal Society of Chemistry ({RSC}), 2014年09月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, Reaction conditions for the synthesis of an epsilon-Keggin-type polyoxometalate-based 3D framework, (NH4)(2.8)H-0.9[epsilon-VMo9.4V2.6O40Bi2]center dot 7.2H(2)O (denoted as Mo-V-Bi oxide), are studied. It is found that the reaction time, temperature, pH of the solution, and starting compounds affect the production of Mo-V-Bi oxide. The crystal size of Mo-V-Bi oxide is controllable by changing bismuth compounds. Nanometer-sized Mo-V-Bi oxide is produced using a water-soluble bismuth compound, Bi(NO3)(3)center dot 5H(2)O, whereas micrometer to submicrometer-sized Mo-V-Bi oxide is produced using Bi(OH)(3), which is less soluble in water. The particle size of the material affects the properties of the material, such as surface area and catalysis. The investigation of the formation process of the material is carried out with Raman spectroscopy, which indicates that mixing (NH4)(6)Mo7O24 center dot 4H(2)O, VOSO4 center dot 5H(2)O, and bismuth ions in water produces the epsilon-Keggin polyoxovanadomolybdate together with a ball-shaped polyoxovanadomolybdate, [Mo72V30O282(H2O)(56)(SO4)(12)](36-) (denoted as {Mo72V30}). By heating the reaction mixture, the epsilon-Keggin polyoxovanadomolybdate assembles with bismuth ions to form Mo-V-Bi oxide, whereas {Mo72V3O} assembles with other vanadium and molybdenum ions to form orthorhombic Mo-V oxide.

Crystalline Mo-V–W-mixed Oxide with Orthorhombic and Trigonal Structures as Highly Efficient Oxidation Catalysts of Acrolein to Acrylic Acid
Chuntian Qiu, Chen Chen, Satoshi Ishikawa, Toru Murayama, Wataru Ueda
Topics in Catalysis, 57, 14-16, 1163, 1170, Springer Science $\mathplus$ Business Media, 2014年09月, ［査読有り］
英語, 研究論文（学術雑誌）, We succeeded in introducing W in Mo3VOx with keeping the orthorhombic, trigonal, and amorphous structures. Synthesized crystalline Mo(W)(3)VOx with orthorhombic and trigonal structures, both of which possess heptagonal channels, showed catalytic activity for gas-phase selective acrolein oxidation to acrylic acid superior to amorphous Mo(W)(3)VOx and to tetragonal Mo3VOx. The results strongly suggest that the crystalline Mo(W)(3)VOx with orthorhombic and trigonal structures are real active phase of industrial acrolein oxidation catalysts based on Mo, W, and V oxides. Furthermore, we found that the resulting W-containing catalyst showed less-dependency of water partial pressure in the reactant feed on the acrolein conversion.

Seed-Assisted Synthesis of Crystalline Mo3VOx Oxides and Their Crystal Formation Mechanism
Satoshi Ishikawa, Masaya Tashiro, Toru Murayama, Wataru Ueda
CRYSTAL GROWTH & DESIGN, 14, 9, 4553, 4561, AMER CHEMICAL SOC, 2014年09月, ［査読有り］
英語, 研究論文（学術雑誌）, The effects of the addition of crystalline Mo3VOx oxides (MoVO) seeds on an assembly of pentagonal [Mo6O21](6-) building units with Mo and V octahedra for forming MoVO were investigated. In the absence of the seeds, the crystal phase of formed MoVO depended on the pH of the preparative solution, while the crystal phase of the formed MoVO was decided by the phase of the MoVO seeds used irrespective of the pH. Interestingly, MoVO were formed even in the pH condition where no crystals were formed in the absence of the seeds. It was shown by X-ray diffraction, scanning transmission electron microscopy energy-dispersive X-ray spectroscopy, and scanning electron microscopy that MoVO crystals were grown from the cross-section of the rod-shaped crystals of the MoVO seeds.

Preparation, structural characterization, and ion-exchange properties of two new zeolite-like 3D frameworks constructed by ε-Keggin-type polyoxometalates with binding metal ions, H11.4[ZnMo12O40Zn2]1.5- and H7.5[Mn0.2Mo12O40Mn2]2.1-.
Zhang Z, Sadakane M, Murayama T, Sakaguchi N, Ueda W
Inorganic chemistry, 53, 14, 7309, 7318, American Chemical Society ({ACS}), 2014年07月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, Two new epsilon-Keggin-type polyoxometalate-based 3D frameworks, Na1.5H11.4[epsilon-(ZnMo10.9Mo1.1O40)-Mo-II-Mo-V-O-VI{Zn-II}(2)] and (NH4)(2).H-1(7.5)[epsilon-(Mn0.2Mo6Mo6O40)-Mo-II-Mo-V-O-VI{Mn-II}(2)], are prepared, and their structures are determined by powder X-ray diffraction, Fourier transform infrared, Raman spectroscopy, and elemental analysis. epsilon-Keggin-type polyoxomolybdate units, [epsilon-ZnMo12O40] and [epsilon-Mn0.2Mo12O40], are linked with Zn2+ and Mn2+, respectively, in a tetrahedral fashion to form 3D frameworks. They show zeolite-like ion-exchange properties and redox properties. The epsilon-Keggin-based 3D framework shows high chemical composition diversity and can incorporate different elements in the framework.

Investigation of the formation process of zeolite-like 3D frameworks constructed with ε-Keggin-type polyoxovanadomolybdates with binding bismuth ions and preparation of a nano-crystal.
Zhang Z, Sadakane M, Murayama T, Ueda W
Dalton transactions (Cambridge, England : 2003), 43, 36, 13584, 13584, Royal Society of Chemistry ({RSC}), 2014年07月, ［査読有り］
英語, 研究論文（学術雑誌）, Reaction conditions for the synthesis of an epsilon-Keggin-type polyoxometalate-based 3D framework, (NH4)(2.8)H-0.9[epsilon-VMo9.4V2.6O40Bi2]center dot 7.2H(2)O (denoted as Mo-V-Bi oxide), are studied. It is found that the reaction time, temperature, pH of the solution, and starting compounds affect the production of Mo-V-Bi oxide. The crystal size of Mo-V-Bi oxide is controllable by changing bismuth compounds. Nanometer-sized Mo-V-Bi oxide is produced using a water-soluble bismuth compound, Bi(NO3)(3)center dot 5H(2)O, whereas micrometer to submicrometer-sized Mo-V-Bi oxide is produced using Bi(OH)(3), which is less soluble in water. The particle size of the material affects the properties of the material, such as surface area and catalysis. The investigation of the formation process of the material is carried out with Raman spectroscopy, which indicates that mixing (NH4)(6)Mo7O24 center dot 4H(2)O, VOSO4 center dot 5H(2)O, and bismuth ions in water produces the epsilon-Keggin polyoxovanadomolybdate together with a ball-shaped polyoxovanadomolybdate, [Mo72V30O282(H2O)(56)(SO4)(12)](36-) (denoted as {Mo72V30}). By heating the reaction mixture, the epsilon-Keggin polyoxovanadomolybdate assembles with bismuth ions to form Mo-V-Bi oxide, whereas {Mo72V3O} assembles with other vanadium and molybdenum ions to form orthorhombic Mo-V oxide.

Direct Oxidative Transformation of Glycerol into Acrylic Acid over Phosphoric Acid-added W–V–Nb Complex Metal Oxide Catalysts
Kaori Omata, Keeko Matsumoto, Toru Murayama, Wataru Ueda
Chem. Lett., 43, 4, 435, 437, The Chemical Society of Japan, 2014年04月, ［査読有り］
英語, 研究論文（学術雑誌）, The addition of phosphoric acid to W-Nb-O catalyst active for glycerol transformation to acrolein and to W-V-Nb-O catalyst active for direct transformation of glycerol to acrylic acid appreciably improved their catalytic performance. The phosphoric acid-added W-Nb-O catalyst gave acrolein yield of 81.8%, and the phosphoric acid-added W-V-Nb-O catalyst gave acrylic acid yield of 59.2% in the direct glycerol transformation. The improvement of the catalytic performance seems due to the increases of the acid amount and the Bronsted acidity.

Reduced Vanadium and Molybdenum Oxides Catalyze the Equivalent Formation of Ethane and Acetaldehyde from Ethanol
Yoichi Nakamura, Toru Murayama, Wataru Ueda
CHEMCATCHEM, 6, 3, 741, 744, WILEY-V C H VERLAG GMBH, 2014年03月, ［査読有り］
英語, 研究論文（学術雑誌）, Catalytic tests for ethanol conversion were performed on vanadium and molybdenum oxides with different oxidation states. We found for the first time that equivalent amounts of ethane and acetaldehyde were formed catalytically over V2O3 and MoO2. No influence of the reaction temperature was observed on the selectivity to ethane and acetaldehyde in the range of 533-653K over V2O3 and MoO2. The reactions of methanol, 1-propanol, and 2-propanol also produced the corresponding alkanes and aldehydes in a 1:1 ratio. A reaction scheme for the formation of ethane and acetaldehyde from ethanol is proposed in which a hydrogen transfer reaction occurs between two ethanol molecules adsorbed on the adjacent metal cation-oxygen anion pair sites to form ethane, acetaldehyde, and water in one step.

Heptagonal channel micropore of orthorhombic Mo3VOx as catalysis field for the selective oxidation of ethane
Satoshi Ishikawa, Xiaodong Yi, Toru Murayama, Wataru Ueda
APPLIED CATALYSIS A-GENERAL, 474, 10, 17, ELSEVIER, 2014年03月, ［査読有り］
英語, 研究論文（学術雑誌）, A number of orthorhombic Mo3VO chi oxide catalysts with different external surface areas measured by N-2 adsorption and with the same micropore volumes measured by ethane adsorption were synthesized hydrothermally by adding sodium dodecyl sulphonate (SDS, C12H25SO3Na) and by changing synthesis temperature. The synthesized catalysts were then tested for the selective oxidations of ethane accessible to the micropore and of 2-propanol inaccessible to the micropore in order to investigate the role of the micropore in the gas-phase oxidation of ethane. It was found that the conversion of ethane was almost similar for all the catalysts irrespective of their largely different external surface areas. On the other hand, the oxidation of 2-propanol to acetone clearly depended on the external surface area of the catalysts. Since other catalytically affective properties such as crystal structure, elemental compositions, and. oxidation states of Mo and V were comparable for all the catalysts, it was concluded that the heptagonal channel micropore of the orthorhombic Mo3VO chi oxide catalyst was responsible for the catalytic activity for the ethane selective oxidation and that the catalytic oxidation of ethane could take place inside the micropore. (C) 2013 Elsevier B.V. All rights reserved.

ChemInform Abstract: Tetrahedral Connection of ε-Keggin-Type Polyoxometalates to Form an All-Inorganic Octahedral Molecular Sieve with an Intrinsic 3D Pore System.
Zhenxin Zhang, Masahiro Sadakane, Toru Murayama, Shoko Izumi, Nobuhiro Yasuda, Norihito Sakaguchi, Wataru Ueda
ChemInform, 45, 13, no, no, Wiley-Blackwell, 2014年03月, ［査読有り］
研究論文（学術雑誌）

Tetrahedral connection of ε-Keggin-type polyoxometalates to form an all-inorganic octahedral molecular sieve with an intrinsic 3D pore system.
Zhang Z, Sadakane M, Murayama T, Izumi S, Yasuda N, Sakaguchi N, Ueda W
Inorganic chemistry, 53, 2, 903, 911, 2, 2014年01月, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, A new type of polyoxometalate-based porous material was successfully synthesized. The new material is the first fully inorganic Keggin-type polyoxometalate-based microporous material with intrinsically ordered open micropores and is the third member of the small family of octahedral molecular sieves (OMSs). Twelve MoO6 or VO6 octahedra surround a central VO4 tetrahedron to form epsilon-Keggin polyoxometalate building blocks (epsilon-VMo9.4V2.6O40) that are linked by Bi-III ions to form crystalline Mo-V-Bi oxide with a diamondoid topology. The presence of a tetrahedral shape of the epsilon-Keggin polyoxometalate building block results in arrangement of microporosity in a tetrahedral fashion which is new in OMSs. Owing to its microporosity, this Mo-V-Bi oxide shows zeolitic-like properties such as ion-exchange and molecule adsorption.

Hydrothermal synthesis of octahedra-based layered niobium oxide and its catalytic activity as a solid acid
Toru Murayama, Junli Chen, Jun Hirata, Keeko Matsumoto, Wataru Ueda
CATALYSIS SCIENCE & TECHNOLOGY, 4, 12, 4250, 4257, ROYAL SOC CHEMISTRY, 2014年, ［査読有り］
英語, 研究論文（学術雑誌）, Layered-structure-type niobium oxides were synthesized by the hydrothermal method by using ammonium niobium oxalate as a precursor. The X-ray diffraction pattern (Cu-K alpha) of the synthesized niobium oxide showed characteristic peaks at 2 theta = 22.7 degrees and 46.2 degrees indicating the linear corner-sharing of NbO6 octahedra in the c-direction. From Raman measurements, the layered-structure-type niobium oxide was composed of NbO6 octahedra and {Nb6O21} pentagonal units. The presence of micropores was confirmed by N-2 adsorption at low pressure (1.0 x 10(-6)), indicating that the arrangement of the a-b plane was an interconnection of the crystal structure motifs of {Nb6O21} units and micropore channels but without long-range order (deformed orthorhombic). Ammonium cations and water were desorbed from the deformed orthorhombic niobium oxide by calcination at 400 degrees C, and Bronsted acid sites were formed. The deformed orthorhombic niobium oxide showed high catalytic activity as a solid acid compared to the catalytic activities of other crystalline niobium oxides. The order of catalytic activity for the alkylation of benzyl alcohol and anisole was deformed orthorhombic Nb2O5 > TT-Nb2O5, amorphous Nb2O5 >> T-Nb2O5, pyrochlore Nb2O5.

Single-Crystalline-Phase Mo3VOx: An Efficient Catalyst for the Partial Oxidation of Acrolein to Acrylic Acid
Chen Chen, Nakatani Kosuke, Toru Murayama, Wataru Ueda
CHEMCATCHEM, 5, 10, 2869, 2873, WILEY-V C H VERLAG GMBH, 2013年10月, ［査読有り］
英語, 研究論文（学術雑誌）

Electrocatalysis of heat-treated cobalt-porphyrin/carbon for hydrogen peroxide formation
Ichiro Yamanaka, Ryo Ichihashi, Tatsuya Iwasaki, Naoya Nishimura, Toru Murayama, Wataru Ueda, Sakae Takenaka
ELECTROCHIMICA ACTA, 108, 321, 329, PERGAMON-ELSEVIER SCIENCE LTD, 2013年10月, ［査読有り］
英語, 研究論文（学術雑誌）, The electrocatalysis of heat-treated Co-TPP/carbon for O-2 reduction and H2O2 formation using a fuel cell reactor with an H2SO4 aqueous electrolyte was studied (TPP: 5,10,15,20-tetralds(pheny1)-21H,23H-porphyrin). Carbon supports, including vapor grown carbon fiber (VGCF), activated carbon (AC), carbon black XC-72 (XC72), and carbon black Black-Pearl-2000/3500 (BP2000/3500), strongly affected the electrocatalysis of the Co-TPP/carbon. The Co-TPP/VGCF heat-treated at 1023 K, abbreviated as CoTPP/VGCF(1073), showed a good electrocatalytic activity for H2O2 formation (1.0 mol dm(-3) with 40% current efficiency (CE)); however, other carbon supports were unfavorable. Electrocatalytic activities were Co-TPP/VGCF(1073) "Co-TPP/XC72(1073) > Co-TPP/AC(1073) > Co-TPP/BP2000(1073). Their electrocatalysis were studied by rotating ring-disk electrode voltammetry and kinetic studies of the decomposition of H(2)O(2)and the electroreduction of H2O2 to water. These studies indicated that the electrocatalytic activities for the successive reduction of H2O2 to water determined the final H2O2 concentrations and CEs. An active site of heat-treated Co-TPP/VGCF was characterized by X-ray photoelectron spectroscopy, and X-ray absorption near-edge fine structure spectroscopy. Partial pyrolysis of Co-TPP on the carbon surface was essential to generate the active site for the H2O2 formation. A model of the Co active site, CoN2-carbon, was proposed. Crown Copyright (C) 2013 Published by Elsevier Ltd. All rights reserved.

ChemInform Abstract: Synthesis of Novel Orthorhombic Mo and V Based Complex Oxides Coordinating Alkylammonium Cation in Its Heptagonal Channel and Their Application as a Catalyst.
Satoshi Ishikawa, Toru Murayama, Shunpei Ohmura, Masahiro Sadakane, Wataru Ueda
ChemInform, 44, 34, no, no, Wiley-Blackwell, 2013年08月01日, ［査読有り］
研究論文（学術雑誌）

Synthesis of Novel Orthorhombic Mo and V Based Complex Oxides Coordinating Alkylammonium Cation in Its Heptagonal Channel and Their Application as a Catalyst
Satoshi Ishikawa, Toru Murayama, Shunpei Ohmura, Masahiro Sadakane, Wataru Ueda
CHEMISTRY OF MATERIALS, 25, 11, 2211, 2219, AMER CHEMICAL SOC, 2013年06月, ［査読有り］
英語, 研究論文（学術雑誌）, The effects of several alkylammonium cations on the synthesis of orthorhombic Mo3VO11.2 complex oxides (MoVO) were investigated. First, we synthesized various alkylammonium isopolymolybdates as precursors for the synthesis of MoVO. Methylammonium heptamolybdate, dimethylammonium trimolybdate, ethylammonium trimolybdate, and ethylenediammonium trimolybdate were obtained as pure materials in new crystalline structures. Orthorhombic MoVO complex oxides were synthesized under hydrothermal conditions when (CH3NH3)(6)Mo7O24 and ((CH3)(2)NH2)(2)Mo3O10 center dot H2O were used. It was found for the first case that methylammonium cations and dimethylammonium cations were incorporated into the orthorhombic MoVO structure, forming compounds of Mo32.3V7.7O112(CH3NH3)(4.0)center dot 9.7/H2O and Mo30.2V9.8O112((CH3)(2)NH2)(25)center dot 8.5H(2)O, respectively. These alkylammonium cations play an important role as a stabilizer in the synthesis of MoVO and act as a structure directing agent for the orthorhombic phase.

Assembly of a Pentagonal Polyoxomolybdate Building Block, [Mo6O21](6-), into Crystalline MoV Oxides
Masahiro Sadakane, Keisuke Endo, Katsunori Kodato, Satoshi Ishikawa, Toru Murayama, Wataru Ueda
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2013, 10-11, 1731, 1736, WILEY-V C H VERLAG GMBH, 2013年04月, ［査読有り］
英語, 研究論文（学術雑誌）, The building-block assembly of polyoxometalates to form crystalline MoV-based metal oxides is presented. Mixing of (NH4)6Mo7O24 and VOSO4 in water with a pH value higher than 1.7 produced the ball-shaped polyoxometalate [Mo72V30O282(H2O)56(SO4)12]36 ({Mo72V30}) with 12 pentagonal [Mo6O21]6 polyoxomolybdate units connected to 30 [V=O]2+ units, which was detected by using UV/Vis, Raman, and IR spectroscopy. Hydrothermal reaction of the precursor containing {Mo72V30} produced crystalline orthorhombic or trigonal MoV oxides. These oxides contain the pentagonal Mo unit in the crystal structure. The results indicate that the pentagonal polyoxomolybdate unit produced in the reaction precursor assembles with other Mo and V ions to form crystalline orthorhombic and trigonal MoV oxides.

Hydrothermal synthesis of W-Nb complex metal oxides and their application to catalytic dehydration of glycerol to acrolein
Kaori Omata, Shoko Izumi, Toru Murayama, Wataru Ueda
CATALYSIS TODAY, 201, 7, 11, ELSEVIER SCIENCE BV, 2013年03月, ［査読有り］
英語, 研究論文（学術雑誌）, W-Nb complex metal oxides (W-Nb-O) having a layered structure (linear arrangement of corner-shared octahedra) in the c-direction and a disordered structure in the a-b plane were prepared by a hydrothermal synthesis method. Following calcination of W-Nb-O at a temperature below 973 K resulted in a high yield of acrolein of more than 70% in gas-phase glycerol dehydration in the presence of water and oxygen. The acrolein yield and the deactivation rate in the W-Nb-O was found to be higher and slower respectively than those of WO3/ZrO2 and H-ZSM-5 which are typical acid catalysts. Product selectivity over W-Nb complex metal oxides, which have the same layered structure in the c-axis direction were tested at comparable glycerol conversion rates. The tetragonal W-Nb-O catalyst (Nb8W9O47) and the acid-treated Cs-0.5[Nb2.5W2.5O14] having orthorhombic structure showed different selectivity for glycerol transformation. However, the hydrothermally synthesized W-Nb-O calcined at a lower temperature had comparable acrolein selectivity to acid-treated Cs0.5[Nb2.5W2.5O14]. The results suggest that the structure of a-b plane affects the product distribution. (C) 2012 Elsevier B. V. All rights reserved.

Quantitative Analysis of Coke Formation during Steam Reforming of Methane on a Nickel–Hydrotalcite Catalyst under Practical Operation Conditions
Tatsuya Takeguchi, Hiroshi Watanabe, Toru Murayama, Hiroki Takahashi, Wataru Ueda
Chem. Lett., 42, 2, 124, 126, The Chemical Society of Japan, 2013年02月, ［査読有り］
英語, 研究論文（学術雑誌）, Relation between redox properties of a nickel-hydrotalcite (Ni-HT) catalyst and a Ni/Al2O3 catalyst and rate of coke deposition during steam reforming of methane is examined. Ni-HT is oxidized by water-vapor treatment to form Ni-incorporated hydrotalcite. Rate of coke deposition on Ni-HT under thermodynamically coke-deposition-free condition is less than one third of that on Ni/Al2O3. No coke deposition is expected on Ni-HT at H2O/CH4 = 1.4 even at equilibrium CH4 conversion owing to redox between metallic Ni and Ni-incorporated hydrotalcite.

An orthorhombic Mo3VOx catalyst most active for oxidative dehydrogenation of ethane among related complex metal oxides
Takeshi Konya, Tomokazu Katou, Toru Murayama, Satoshi Ishikawa, Masahiro Sadakane, Douglas Buttrey, Wataru Ueda
CATALYSIS SCIENCE & TECHNOLOGY, 3, 2, 380, 387, ROYAL SOC CHEMISTRY, 2013年, ［査読有り］
英語, 研究論文（学術雑誌）, Four distinct structural types (orthorhombic, trigonal, tetragonal and amorphous) of Mo3VOx catalyst were each synthesized by a hydrothermal method as a single phase, characterized structurally and tested for oxidative dehydrogenation of ethane. A common structural feature of the catalysts is that the materials are a layer-type structure and constructed with pentagonal {Mo6O21} units. The arrangement of the pentagonal units can form heptagonal channels to create different structural features. The orthorhombic Mo3VOx catalyst has microporosity due to the open heptagonal channels adsorbing nitrogen molecules and showed the highest activity for the reaction among four distinct catalysts. Furthermore, this phase appeared to be most active, currently, compared to other complex metal oxide catalysts reported. An observed positive relation between the microporosity and the oxidation activity suggests that the catalytic oxidation takes place at the heptagonal channels.

Morphology-controlled preparation of iron-based oxides using a paper template
Masahiro Sadakane, Rika Kato, Toru Murayama, Wataru Ueda
MATERIALS LETTERS, 81, 80, 83, ELSEVIER SCIENCE BV, 2012年08月, ［査読有り］
英語, 研究論文（学術雑誌）, Morphology-controlled iron-based oxides, including Fe2O3, LaFeO3, NiFe2O4, ZnFe2O4, and CoFe2O4, were obtained using filter paper as a template. A thimble filter paper was soaked in ethylene glycol solution of metal nitrates, and the thimble filter paper-metal nitrate composite was calcined to form the desired iron-based oxides with morphology of thimble filter paper. Choice of ethylene glycol as a solvent and slow heating for removal of the paper template are crucial for maintaining the morphology of paper. (C) 2012 Elsevier B.V. All rights reserved.

Synthesis of porous and acidic complex metal oxide catalyst based on group 5 and 6 elements
Toru Murayama, Nozomi Kuramata, Shunsuke Takatama, Kosuke Nakatani, Shoko Izumi, Xiaodong Yi, Wataru Ueda
CATALYSIS TODAY, 185, 1, 224, 229, ELSEVIER SCIENCE BV, 2012年05月, ［査読有り］
英語, 研究論文（学術雑誌）, Complex metal oxides of transition metals using Mo, W, V, Nb and Ta were synthesized by hydrothermal method. The synthesized complex metal oxides were characterized and the solid acid catalytic activity was tested through the Friedel-Crafts alkylation of anisole and benzyl alcohol. X-ray diffraction patterns of the obtained samples showed two peaks at 2 theta = 22 degrees and 46 degrees indicating these materials have layer-type crystal structure, regardless of the combination of several metals. Moreover, Mo-V-O, Mo-Nb-O, W-Nb-O and W-Ta-O showed microporosity from N-2 adsorption isotherm. Among of these combinations, Mo-Nb-O, W-Nb-O and W-Ta-O showed a higher catalytic performance for alkylation reaction. (C) 2011 Published by Elsevier B. V.

Phosgene-Free Method for Diphenyl Carbonate Synthesis at the Pd 0 /Ketjenblack Anode
Toru Murayama, Tomohiko Hayashi, Ryoichi Kanega, Ichiro Yamanaka
J. Phys. Chem. C, 116, 19, 10607, 10616, American Chemical Society ({ACS}), 2012年05月, ［査読有り］
英語, 研究論文（学術雑誌）, Electrocarbonylation of phenol (PhOH) with CO to diphenyl carbonate (DPC) at a Pd-0-supported Ketjenblack electrocatalyst (Pd/KB) was studied at P(CO) = 1 atm and 25 degrees C. Electrocarbonylation was conducted by galvanostatic electrolysis at 1 mA in an electrolyte containing PhOH, sodium phenoxide (PhONa), LiCl, and CH3CN. The electrocatalytic activity of DPC formation was strongly affected by the reduction temperature of a PdCl2/KB electrocatalyst with H-2. The Pd/KB electrocatalyst reduced at 393 K showed the highest electrocatalytic activity, while that reduced at 673 K showed less activity. Pd/KB was characterized by X-ray diffraction, transmission electron microscopy-energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. Pd particle sizes are strongly related to the electrocatalytic activity of DPC formation. Pd-0 particles less than 2 nm were active, whereas those greater than 6 nm were inactive. To reveal the electrocarbonylation mechanism, electrocarbonylations using p-cresol, p-chlorophenol, and sodium phenoxides were studied. Cyclic voltammetry studies were conducted using a palladiumized palladium-wire electrode. These results strongly indicated that sodium phenoxides did not incorporate into diaromatic carbonates and also functioned as proton acceptors during electrocarbonylation.

Motion Planning of Networked Multi-Vehicle System with Hybrid Measurement Model
Toru Murayama, Akinori Nagano, Kenneth Ho, Zhi-Wei Luo
2012 8TH INTERNATIONAL CONFERENCE ON COMPUTING AND NETWORKING TECHNOLOGY (ICCNT, INC, ICCIS AND ICMIC), 207, 212, IEEE, 2012年
英語, 研究論文（国際会議プロシーディングス）, This paper presents a new motion planning method of a multi-vehicle system in which vehicles can mutually measure the location of other vehicles when distances between vehicles are close. The mutual measurement method reduces uncertainty of location estimation by providing additional information. We propose a motion planning method based on the existence of maximal distance of mutual measurement. We formulate a multi-vehicle system with some disturbance and a new hybrid measurement model. The new model is a hybrid of maximal distance of mutual measurement and Kalman filter. The receding horizon control method is shown to be applicable to the new hybrid measurement model. We demonstrate the validity of our new hybrid measurement model in computer simulation.

Preparation and formation mechanism of three-dimensionally ordered macroporous (3DOM) MgO, MgSO4, CaCO3, and SrCO3, and photonic stop band properties of 3DOM CaCO3
Masahiro Sadakane, Rika Kato, Toru Murayama, Wataru Ueda
JOURNAL OF SOLID STATE CHEMISTRY, 184, 8, 2299, 2305, ACADEMIC PRESS INC ELSEVIER SCIENCE, 2011年08月, ［査読有り］
英語, 研究論文（学術雑誌）, Three-dimensionally ordered macroporous (3DOM) magnesium (Mg) oxide (MgO), MgSO4, calcium (Ca) carbonate (CaCO3), and strontium (Sr) carbonate (SrCO3) were prepared using a colloidal crystal of polymer spheres as a template. Ethanol or ethanol-water solution of metal salts (acetate or nitrate) and citric acid was infiltrated into the void of the colloidal crystal template of a monodispersed poly(methyl methacrylate) (PMMA) sphere. Heating of this PMMA-metal salt-citric acid composite produced the desired well-ordered 3DOM materials with a high pore fraction, which was confirmed by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and ultraviolet-visible (UV-vis) diffuse reflectance spectra. The presence of citric acid is crucial for production of the 3DOM structures. Reaction of citric acid with metal salt produces metal citrate solid in the void of PMMA spheres, which is necessary to maintain the 3DOM structure during the calcination process. 3DOM CaCO3 shows opalescent colors because of it's photonic stop band properties. (C) 2011 Elsevier Inc. All rights reserved.

Catalytic neutral hydrogen peroxide synthesis from O-2 and H-2 by PEMFC fuel
Toru Murayama, Satoshi Tazawa, Sakae Takenaka, Ichiro Yamanaka
CATALYSIS TODAY, 164, 1, 163, 168, ELSEVIER, 2011年04月, ［査読有り］
英語, 研究論文（学術雑誌）, Catalytic and direct synthesis of a neutral hydrogen peroxide solution from O-2 and H-2 was studied using a new conceptual PEMFC reactor with a new active cathode. A particular electrocatalyst of Co-TPP/vapor-grown-carbon-fiber (VGCF) heat-treated in He at 1073 K was found for two electrons reduction of O-2. The most active and efficient cathode was 0.05 wt.% Co-TPP/VGCF (2 mg cm(-2)) coated on the VGCF base electrode. The maximum concentration of 13.5 wt.% was obtained with 42% CE at 278 K. (C) 2011 Elsevier B.V. All rights reserved.

Electrosynthesis of Neutral H2O2 Solution from O-2 and Water at a Mixed Carbon Cathode Using an Exposed Solid-Polymer-Electrolyte Electrolysis Cell
Toru Murayama, Ichiro Yamanaka
JOURNAL OF PHYSICAL CHEMISTRY C, 115, 13, 5792, 5799, AMER CHEMICAL SOC, 2011年04月, ［査読有り］
英語, 研究論文（学術雑誌）, An improved solid-polymer-electrolyte (SPE) electrolysis method was applied for direct electrosynthesis of neutral H2O2 solution from O-2 and water. The exposure of a cathode prepared from activated carbon (AC), vapor-grown carbon fiber (VGCF), and polytetrafluoroethylene (PTFE) in the O-2 stream was essential for the electrosynthesis of the neutral H2O2 solution (Exp-SPE method). The oxidation treatment of the AC surface and the modification of the cathode using a Nafion solution enhanced the electrochemical activity of the cathode for the neutral H2O2 formation. The active site of the reduction of O-2 was characterized using TPD-Mass and FT-IR techniques; then, the concentration of phenol groups on the AC surface corresponded to the H2O2 formation. The reaction mechanism was proposed that O-2 electrochemically reduced to H2O2. at the active site of the phenol groups on the AC and in which HO2 center dot immediately reduced to H2O2 or disproportioned to H2O2 on the VGCF surface.

Catalytic synthesis of neutral H2O2 solution by a fuel cell with a CoN2Cx/carbon cathode
Ichiro Yamanaka, Satoshi Tazawa, Toru Murayama
ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 241, AMER CHEMICAL SOC, 2011年03月, ［査読有り］
英語

Direct synthesis of diphenyl carbonate by mediated electrocarbonylation of phenol at Pd2+-supported activated carbon anode
Toru Murayama, Tomohiko Hayashi, Yuji Arai, Ichiro Yamanaka
ELECTROCHIMICA ACTA, 56, 7, 2926, 2933, PERGAMON-ELSEVIER SCIENCE LTD, 2011年02月, ［査読有り］
英語, 研究論文（学術雑誌）, Mediated electrocarbonylation of phenol to diphenyl carbonate (DPC) at a PdCl2-supported activated carbon anode in 1 atm CO at 298 K was studied. A dry CH2Cl2 or CH3CN solvent and a galvanostatic electrolysis of 1 mA were necessary for formation of DPC, while the addition of a base and a supporting electrolyte was also essential. A combination of triethylamine (Et3N) and tetrabutylammonium perchlorate (Bu4NClO4) was suitable in various combinations. The addition of 2 equiv. of Et3N to the electrolyte (C6H5OH/Bu4NClO4/CH2Cl2) at 1-h intervals was more efficient in the formation of DPC than a single initial addition of the same amount of Et3N. The yield of DPC was 130% based on Pd and its current efficiency (CE) was 42% for 6 h. The CE of the CO2 formation was only 3%. Sodium phenoxide (PhONa) showed dual functionality as a base and supporting electrolyte. When the mediated electrocarbonylation was conducted in a C6H5OH/PhONa/CH3CN electrolyte, DPC was produced in 172% yield and 40% CE for 6 h. The CE of the CO2 formation was 10%. DPC formed continuously after a single initial addition of 4 equiv. of PhONa. Li or K phenoxide also worked as promoters for the mediated electrocarbonylation of phenol to DPC. (C) 2011 Elsevier Ltd. All rights reserved.

A Fuel-Cell Reactor for the Direct Synthesis of Hydrogen Peroxide Alkaline Solutions from H-2 and O-2
Ichiro Yamanaka, Takeshi Onisawa, Toshikazu Hashimoto, Toru Murayama
CHEMSUSCHEM, 4, 4, 494, 501, WILEY-V C H VERLAG GMBH, 2011年, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, The effects of the type of fuel-cell reactors (undivided or divided by cation-and anion-exchange membranes), alkaline electrolytes (LiOH, NaOH, KOH), vapor-grown carbon fiber (VGCF) cathode components (additives: none, activated carbon, Valcan XC72, Black Pearls 2000, Seast-6, and Ketjen Black), and the flow rates of anolyte (0, 1.5, 12 mLh(-1)) and catholyte (0, 12 mLh(-1)) on the formation of hydrogen peroxide were studied. A divided fuel-cell system, O-2 (g) jVGCF-XC72 cathode vertical bar 2M NaOH catholyte vertical bar cation-exchange membrane (Nafion-117) vertical bar Pt/XC72-VGCF anode vertical bar 2M NaOH anolyte at 12 mLh(-1) flow vertical bar H-2 (g), was effective for the selective formation of hydrogen peroxide, with 130 mAcm(-2), a 2M aqueous solution of H2O2/NaOH, and a current efficiency of 95% at atmospheric pressure and 298 K. The current and formation rate gradually decreased over a long period of time. The cause of the slow decrease in electrocatalytic performance was revealed and the decrease was stopped by a flow of catholyte. Cyclic voltammetry studies at the VGCF-XC72 electrode indicated that fast diffusion of O-2 from the gas phase to the electrode, and quick desorption of hydrogen peroxide from the electrode to the electrolyte were essential for the efficient formation of solutions of H2O2/NaOH.

Redox tunable reversible molecular sieves: orthorhombic molybdenum vanadium oxide
Masahiro Sadakane, Shunpei Ohmura, Katsunori Kodato, Takumi Fujisawa, Kazuo Kato, Ken-ichi Shimidzu, Toru Murayama, Wataru Ueda
CHEMICAL COMMUNICATIONS, 47, 38, 10812, 10814, ROYAL SOC CHEMISTRY, 2011年, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）, We demonstrated that the sorption behavior of orthorhombic Mo-V oxide (Mo29V11O112-x) is continually and reversibly tunable by redox treatment.

Direct Synthesis of Diphenyl Carbonate by Electrocarbonylation at a Pd2+-supported Anode
Toru Murayama, Yuji Arai, Tomohiko Hayashi, Ichiro Yamanaka
CHEMISTRY LETTERS, 39, 4, 418, 419, CHEMICAL SOC JAPAN, 2010年04月, ［査読有り］
英語, 研究論文（学術雑誌）, The first electrochemical synthesis of diphenyl carbonate was accomplished using triethylamine/tetrabutylammonium perchlorate/phenol/dichloromethane or sodium phenoxide/phenol/acetonitrile electrolyte at a [PdCl2/activated carbon and vapor grown carbon fiber] anode, 1 atm CO and 25 degrees C. Sodium phenoxide functioned as a promoter, triethylamine, and a supporting electrolyte, tetrabutylammonium perchlorate, for the carbonylation.

Neutral H2O2 Synthesis by Electrolysis of O-2 and Water
T. Murayama, I. Yamanaka
SYNTHETIC AND MECHANISTIC ORGANIC ELECTRON TRANSFER REACTIONS, 25, 18, 19, 24, ELECTROCHEMICAL SOC INC, 2010年, ［査読有り］
英語, 研究論文（国際会議プロシーディングス）, On-site production method of neutral H2O2 solution by electrolysis of O-2 and water was investigated. Improved SPE (solid-polymer-electrolyte) electrolysis method was applied for the synthesis of neutral H2O2 solution. We found that exposure of a cathode of the SPE electrolysis in O-2 stream (1 atm) was efficient for the neutral H2O2 formation (Exp-SPE method). A cathode prepared from oxidized activated carbon, vapor-grown carbon fiber and PTFE, and coating with Nafion solution was the most active for neutral H2O2 formation. The neutral H2O2 solution of 8 wt% was continuously produced with 27% CE at -0.3 V (Ag/AgCl) by the Exp-SPE method.

Study of the Electrochemical Carbonylation of Ethanol and Ethylene at Pd/C Anode
A. Funakawa, T. Murayama, I. Yamanaka
SYNTHETIC AND MECHANISTIC ORGANIC ELECTRON TRANSFER REACTIONS, 25, 18, 35, 40, ELECTROCHEMICAL SOC INC, 2010年, ［査読有り］
英語, 研究論文（国際会議プロシーディングス）, Electrochemical carbonylations of ethanol, methanol and ethylene were studied at the Pd/ C anode with NaClO4 electrolyte. The carbonylation of ethanol to diethyl carbonate (DEC) efficiently proceeded with a current efficiency of 50% as well as the carbonylation of methanol to dimethyl carbonate (DMC). Cross-carbonylations of ethanol and methanol to ethyl methyl carbonate (EMC) and of ethylene and methanol to methyl 3-methoxypropionate and dimethyl succinate proceeded at the Pd/ C anode. These facts indicated the formation of an alkoxycarbonyl intermediate on the Pd/ C anode during the carbonylation.

Catalytic Synthesis of Neutral Hydrogen Peroxide at a CoN2Cx Cathode of a Polymer Electrolyte Membrane Fuel Cell (PEMFC)
Ichiro Yamanaka, Satoshi Tazawa, Toru Murayama, Tatsuya Iwasaki, Sakae Takenaka
CHEMSUSCHEM, 3, 1, 59, 62, WILEY-BLACKWELL, 2010年, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）

Neutral H2O2 Synthesis by Electrolysis of O-2 and Water
T. Murayama, I. Yamanaka
SYNTHETIC AND MECHANISTIC ORGANIC ELECTRON TRANSFER REACTIONS, 25, 18, 19, 24, ELECTROCHEMICAL SOC INC, 2010年, ［査読有り］
英語, 研究論文（国際会議プロシーディングス）, On-site production method of neutral H2O2 solution by electrolysis of O-2 and water was investigated. Improved SPE (solid-polymer-electrolyte) electrolysis method was applied for the synthesis of neutral H2O2 solution. We found that exposure of a cathode of the SPE electrolysis in O-2 stream (1 atm) was efficient for the neutral H2O2 formation (Exp-SPE method). A cathode prepared from oxidized activated carbon, vapor-grown carbon fiber and PTFE, and coating with Nafion solution was the most active for neutral H2O2 formation. The neutral H2O2 solution of 8 wt% was continuously produced with 27% CE at -0.3 V (Ag/AgCl) by the Exp-SPE method.

Neutral H2O2 synthesis by electrolysis of water and O-2
Ichiro Yamanaka, Toru Murayama
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 47, 10, 1900, 1902, WILEY-BLACKWELL, 2008年, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）

Catalytic Synthesis of Neutral H2O2 Solutions from O-2 and H-2 by a Fuel Cell Reaction
Ichiro Yamanaka, Satoshi Tazawa, Toru Murayama, Ryo Ichihashi, Noriko Hanaizumi
CHEMSUSCHEM, 1, 12, 988, 992, WILEY-V C H VERLAG GMBH, 2008年, ［査読有り］, ［国際誌］
英語, 研究論文（学術雑誌）

ポリオキソメタレート上に担持した金ナノ粒子触媒によるCO酸化に関する理論研究
米森朋久, 村山徹, 奥村光隆, 触媒討論会予稿集(CD-ROM), 131st, 2023年

多孔性ポリオキソメタレート担持金属触媒による活性酸素種の生成機構に関する理論研究
米森朋久, 村山徹, 川上貴資, 山中秀介, 奥村光隆, 分子科学討論会講演プログラム&要旨(Web), 17th, 2023年

Ni-Ti層状複水酸化物から変換した複合酸化物を用いた担持金クラスター触媒のCO酸化活性評価
高橋あゆ, 中山晶皓, 村山徹, 坂口紀人, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会予稿集(CD-ROM), 131st, 2023年

ナノ粒子状の層状複水酸化物(LDH)を利用した担持金クラスター触媒の開発
中山晶皓, 吉田彩乃, 青野智香, 本間徹生, 坂口紀史, 竹歳絢子, 藤田隆史, 村山徹, 村山徹, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会予稿集(CD-ROM), 131st, 2023年

スチレン類のマルコフニコフ選択的ヒドロホウ素化反応のための担持酸化ニッケル触媒の開発
竹歳絢子, 平野英司, 木村友星, 村山徹, 村山徹, 山口佳隆, 日本プロセス化学会サマーシンポジウム講演要旨集(Web), 2023, 2023年

層状複水酸化物を変換したNi-Ti複合金属酸化物担持金触媒を用いたCO-PROX反応
高橋あゆ, 中山晶皓, 村山徹, 坂口紀史, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会予稿集(CD-ROM), 132nd, 2023年

微小な層状複水酸化物(LDH)を利用した担持金クラスター触媒によるCO-PROX反応
中山晶皓, 吉田彩乃, 本間徹生, 坂口紀史, 村山徹, 村山徹, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会予稿集(CD-ROM), 132nd, 2023年

担持酸化ニッケル触媒を用いたスチレン類のマルコフニコフ選択的ヒドロホウ素化反応
竹歳絢子, 平野英司, 木村友星, 村山徹, 村山徹, 山口佳隆, 触媒討論会予稿集(CD-ROM), 132nd, 2023年

担持Au触媒を用いた5-ホルミル-2-フランカルボン酸メチルの酸化的エステル化
新井直, SHEET Nirupama, 大須賀遼太, 菅沼学史, 村山徹, 中島清隆, 触媒討論会予稿集(CD-ROM), 132nd, 2023年

Au/ZrO₂触媒によるフタル酸ジメチルの酸化的C-Hカップリング反応
荒田晃生, 中山晶皓, 村山徹, 村山徹, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会予稿集(CD-ROM), 132nd, 2023年

固体酸担持金ナノ粒子触媒を用いた室温での空気浄化反応
村山徹, 村山徹, LIN Mingyue, LIN Mingyue, LIN Mingyue, Journal of the Japan Petroleum Institute (Web), 65, 2, 2022年

金属-有機構造体で被覆したAu/TiO₂触媒によるアルコール酸化
門脇伸太朗, 中山晶皓, 村山徹, 高木慎介, 嶋田哲也, 石田玉青, 触媒討論会講演予稿集(CD-ROM), 129th, 2022年

層状複水酸化物(LDH)を用いたAu/SiO₂表面への新たなCO酸化活性界面の形成
岡山夏帆, 中山晶皓, 村山徹, 坂口紀史, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会講演予稿集(CD-ROM), 129th, 2022年

ハイドロキシアパタイト担持貴金属触媒における強い金属-担体相互作用(SMSI)の効果
中山晶皓, 袖永竜生, GANGARAJULA Yuvaraj, 竹歳絢子, 村山徹, 村山徹, 本間徹生, 坂口紀史, 嶋田哲也, 高木慎介, 春田正毅, QIAO Botao, WANG Junhu, 石田玉青, 触媒討論会講演予稿集(CD-ROM), 129th, 2022年

層状複水酸化物(LDH)ナノ粒子を用いた酸化物担持金ナノ粒子複合触媒の開発
吉田彩乃, 岡山夏帆, 中山晶皓, 村山徹, 藤田隆史, 坂口紀史, 嶋田哲也, 高木慎介, 石田玉青, 日本化学会春季年会講演予稿集(Web), 102nd, 2022年

金属-有機構造体で被覆した金属酸化物担持金ナノ粒子触媒の調製とアルコール酸化触媒活性
門脇伸太朗, 中山晶皓, 坂口紀史, 村山徹, 高木慎介, 嶋田哲也, 石田玉青, 触媒討論会討論会A予稿集(CD-ROM), 130th, 2022年

層状複水酸化物(LDH)ナノ粒子を用いた担持金クラスター触媒の開発
中山晶皓, 吉田彩乃, 青野智香, 岡山夏帆, 本間徹生, 坂口紀史, 竹歳絢子, 藤田隆史, 村山徹, 村山徹, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会討論会A予稿集(CD-ROM), 130th, 2022年

層状複水酸化物ナノシートを用いた金属ナノ粒子触媒表面の修飾とその触媒活性
岡山夏帆, 中山晶皓, 村山徹, 坂口紀史, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会討論会A予稿集(CD-ROM), 130th, 2022年

Ag/Al₂O₃触媒を用いたアンモニアの選択酸化(NH₃-SCO)におけるAg粒子サイズが選択性に与える影響
WANG Haifeng, 村山徹, 村山徹, LIN Mingyue, 坂口紀史, 三浦大樹, 宍戸哲也, 触媒討論会討論会A予稿集(CD-ROM), 130th, 2022年

Ni-Ti層状複水酸化物から変換したNi-Ti複合酸化物担持Auクラスター触媒によるCO酸化反応
高橋あゆ, 中山晶皓, 村山徹, 坂口紀人, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会討論会A予稿集(CD-ROM), 130th, 2022年

バナジウムブロンズ化合物を用いた低温NH₃-SCR
猪股雄介, 窪田博愛, 本松吉典, 迫谷聡介, 吉田和広, 鳥屋尾隆, 清水研一, 村山徹, 村山徹, 触媒討論会討論会A予稿集(CD-ROM), 130th, 2022年

受賞講演 低温空気浄化のための酸化ニオブ担持金ナノ粒子触媒の開発 : 2020年度奨励賞—特集 2020年度受賞講演(2)
村山 徹, ペトロテック = Petrotech : 石油学会情報誌 / 石油学会 編, 44, 10, 672, 677, 2021年10月
東京 : 石油学会 ; 1978-, 日本語

金触媒の新展開 金触媒の新展開と商品化について
春田正毅, 春田正毅, 村山徹, 村山徹, 村山徹, 触媒, 63, 1, 2021年

アクロレイン選択酸化反応用工業触媒としての多元系Mo-V複合酸化物の触媒活性場の考察
石川理史, 山田雄大, 樫尾直樹, 下田光祐, 野田渚紗, 村山徹, 上田渉, 触媒討論会講演予稿集(CD-ROM), 127th, 2021年

低温空気浄化のための酸化ニオブ担持金ナノ粒子触媒の開発
村山徹, ペトロテック, 44, 10, 2021年

金担持触媒を利用した低温での気相酸化反応~金ナノ粒子から金シングルアトム~
村山徹, 村山徹, 触媒討論会討論会A予稿集(CD-ROM), 128th, 2021年

ハイドロキシアパタイト担持金触媒における強い金属-担体相互作用(SMSI)が触媒特性に与える影響
中山晶皓, 袖永竜生, GANGARAJURA Yuvaraj, 竹歳絢子, 村山徹, 本間徹生, 坂口紀史, 嶋田哲也, 高木慎介, 春田正毅, WANG Junhu, 石田玉青, 触媒討論会討論会A予稿集(CD-ROM), 128th, 2021年

Cuを蒸着した酸化バナジウム触媒による不飽和長鎖脂肪族エステルのエステル交換
SUDHAKARAN Swetha, 竹歳絢子, 村山徹, 野村琴広, 触媒討論会討論会A予稿集(CD-ROM), 128th, 2021年

層状複水酸化物(LDH)を用いたAu/SiO₂表面の修飾とCO酸化活性に及ぼす効果
岡山夏帆, 中山晶皓, 村山徹, 嶋田哲也, 高木慎介, 石田玉青, 触媒討論会討論会A予稿集(CD-ROM), 128th, 2021年

W置換V₂O₅触媒による低温・水蒸気雰囲気下でのNH₃-SCRと反応機構解析
猪股雄介, 清永英嗣, 盛田啓一郎, 吉田和広, 窪田博愛, 鳥屋尾隆, 清水研一, 春田正毅, 村山徹, 村山徹, 触媒討論会講演予稿集(CD-ROM), 127th, 2021年

金ナノ粒子触媒の最新動向
村山 徹, ペトロテック = Petrotech : 石油学会情報誌 / 石油学会 編, 43, 6, 1p,432, 436, 2020年06月
東京 : 石油学会 ; 1978-, 日本語

担持金ナノ粒子触媒を用いたフルフラール酸化反応における担体が与える影響と金粒子サイズの効果
望月ちひろ, LIN Mingyue, 竹歳絢子, 石田玉青, 宍戸哲也, 中島清隆, 春田正毅, 村山徹, 触媒討論会講演予稿集(CD-ROM), 125th, 2020年

強い金属-担体相互作用(SMSI)を利用した置換ハイドロキシアパタイト担持金ナノ粒子触媒による3,4-diacetoxybut-1-eneの異性化反応
中山晶皓, 袖永竜生, GANGARAJURA Yuvaraj, 竹歳絢子, 村山徹, 本間徹生, 坂口紀史, 嶋田哲也, 高木慎介, 春田正毅, WANG Junhu, 石田玉青, 触媒討論会講演予稿集(CD-ROM), 125th, 2020年

置換ハイドロキシアパタイト担持金触媒による3,4-diacetoxybut-1-eneの異性化反応-強い金属-担体相互作用(SMSI)の効果-
中山晶皓, 袖永竜生, GANGARAJURA Yuvaraj, 竹歳絢子, 村山徹, 本間徹生, 坂口紀史, 嶋田哲也, 高木慎介, 春田正毅, WANG Junhu, 石田玉青, 触媒討論会討論会A予稿集(CD-ROM), 126th, 2020年

水蒸気存在下での低温脱硝を目指したタングステン添加酸化バナジウム触媒
猪股雄介, 清永英嗣, 盛田啓一郎, 吉田和広, 窪田博愛, 鳥屋尾隆, 清水研一, 春田正毅, 村山徹, 村山徹, 石油・石油化学討論会講演要旨, 50th (Web), 2020年

ミクロ細孔を有するW₄V₃O₁₉複合酸化物へのTiの導入およびNH₃-SCR活性評価
神山曜帆, 石川理史, 猪股雄介, 村山徹, 上田渉, 触媒討論会討論会A予稿集(CD-ROM), 126th, 2020年

150°C以下でNH₃-SCR活性を示すバルク酸化バナジウム触媒
猪股雄介, 秦慎一, 清永英嗣, 盛田啓一郎, 吉田和広, 窪田博愛, 鳥屋尾隆, 清水研一, 春田正毅, 村山徹, 触媒討論会講演予稿集(CD-ROM), 125th, 2020年

水分共存下にて高い低温脱硝作用を示すW添加V₂O₅触媒
猪股雄介, 清永英嗣, 盛田啓一郎, 吉田和広, 窪田博愛, 鳥屋尾隆, 清水研一, 春田正毅, 村山徹, 村山徹, 触媒討論会討論会A予稿集(CD-ROM), 126th, 2020年

The Effects of Dopants on the Cu-ZrO2 Catalyzed Hydrogenation of Levulinic Acid
Jun Hirayama, Igor Orlowski, Sarwat Iqbal, Mark Douthwaite, Satoshi Ishikawa, Peter J. Miedziak, Jonathan K. Bartley, Jennifer Edwards, Qian He, Robert L. Jenkins, Toru Murayama, Christian Reece, Wataru Ueda, David J. Willock, Graham J. Hutchings, JOURNAL OF PHYSICAL CHEMISTRY C, 123, 13, 7879, 7888, 2019年04月
Catalytic hydrogenation of levulinic acid to form gamma-valerolactone was studied over Cu-ZrO2 catalysts doped with metal oxides from the first-row transition metals. The Cu-ZrO2 material was prepared by oxalate gel coprecipitation, and dopants were added by an incipient wetness approach. The addition of 1% Mn into Cu ZrO2 significantly increases the yield of y-valerolactone, and the catalytic activity of Mn/Cu-ZrO2 was found to be 1.6 times higher than that of the undoped Cu ZrO2 catalyst. Catalyst characterization suggests that the Mn dopant improves the dispersion of Cu on the surface of ZrO2. Kinetic studies show that the reaction order with respect to the substrate concentration is approximately zero. However, the order of reaction with respect to the partial pressure of H-2 is different for the Mn/Cu-ZrO2 and Cu-ZrO2 catalysts. Comparison of reaction products from reactions carried out in H2O and D2O solvents using H-1 NMR and C-13 NMR show that there is a pre equilibrium keto enol isomerization step under our reaction conditions. DFT calculations show that the enol isomers have a higher affinity for the Cu surface, which may improve the substrate in the hydrogenation step of the reaction., AMER CHEMICAL SOC, 英語

Supported gold cluster catalysts prepared by solid grinding using a non-volatile organogold complex for low-temperature CO oxidation and the effect of potassium on gold particle size
Luong Xuan Dien, Tamao Ishida, Ayako Taketoshi, Duc Q. Truong, Huynh Dang Chinh, Tetsuo Honma, Toru Murayama, Masatake Haruta, APPLIED CATALYSIS B-ENVIRONMENTAL, 241, 539, 547, 2019年02月
We have found that physical mixing (solid grinding, SG) of dimethylgold(III) acetylacetonate (Me 2 Au(acac)) adsorbed on SiO2 with potassium t-butoxide ((KOBu)-Bu-t) significantly improved the catalytic activity for CO oxidation at low temperature, and T-1/2 (the temperature at 50% CO conversion) became extremely low such as -43 degrees C. We have also developed an alternative Au complex for SG, and 2-(p-tolyl)pyridinebis(trifluoroacetate) gold(III) (AuTFA) could be adsorbed on metal oxide (MOx) supports by physical mixing of AuTFA with MOx in air at room temperature for 20 min, and small Au nanoparticles (NPs) were deposited after calcination. The sizes of Au NPs were almost the same as those prepared using Me2Au(acac) and smaller than those prepared by DP for Al2O3 and TiO2 supports. In addition, grinding AuTFA adsorbed on SiO2 with (KOBu)-Bu-t was also effective for reducing the size of Au particles and gave Au clusters with a mean diameter of 2.2 nm. Moreover, Au/Al2O3 and Au/K-SiO2 exhibited high catalytic activity for CO oxidation under simulated real exhaust gas conditions (low CO concentration and high humidity up to 100% relative humidity) at ambient temperature., ELSEVIER SCIENCE BV, 英語

フルフラール選択的酸化反応における担持金ナノ粒子触媒の担体・サイズ効果
望月ちひろ, 竹歳絢子, 石田玉青, 春田正毅, 村山徹, 石油学会年会講演要旨, 62nd, 2019年

酸化亜鉛に担持した金ナノ粒子触媒によるCO酸化-低温における酸素の活性化過程の変化-
藤田隆史, 石田玉青, 芝本幸平, 本間徹生, 大橋弘範, 村山徹, 春田正毅, 触媒討論会討論会A予稿集(CD-ROM), 124th, 2019年

Au/Nb₂O₅による5-ヒドロキシメチルフルフラールの選択的光酸化
望月ちひろ, 宍戸哲也, 石田玉青, 春田正毅, 村山徹, 触媒討論会討論会A予稿集(CD-ROM), 124th, 2019年

担持金ナノ粒子触媒における金ナノ粒子の電子状態がフルフラール酸化反応に与える影響
望月ちひろ, LIN Mingyue, 竹歳絢子, 石田玉青, 中島清隆, 春田正毅, 村山徹, 触媒討論会討論会A予稿集(CD-ROM), 124th, 2019年

強い金属-担体相互作用をもつハイドロキシアパタイト担持金ナノ粒子触媒によるビニル基交換反応
石田玉青, 袖永竜生, GANGARAJULA Yuvaraj, 中山晶晧, 竹歳絢子, 村山徹, WANG Junhu, 春田正毅, 触媒討論会討論会A予稿集(CD-ROM), 124th, 2019年

ハイドロキシアパタイト担持金ナノ粒子触媒による脂肪族アルデヒドの酸化的エステル化:カチオンおよびアニオン置換効果
竹歳絢子, GANGARAJULA Yuvaraj, 袖永竜生, 村山徹, WANG Junhu, 春田正毅, 石田玉青, 触媒討論会討論会A予稿集(CD-ROM), 124th, 2019年

酸化ニオブによる5-ヒドロキシメチルフルフラールの選択的光酸化における金ナノ粒子担持効果
望月ちひろ, 宍戸哲也, 石田玉青, 春田正毅, 村山徹, 石油・石油化学討論会講演要旨, 49th (Web), 2019年

150°C以下でNOのNH₃-SCRに活性を示す酸化バナジウム触媒
猪股雄介, 秦慎一, 清永英嗣, 盛田啓一郎, 吉田和広, 春田正毅, 村山徹, 触媒討論会講演予稿集(CD-ROM), 123rd, 2019年

金属酸化物担持金ナノ粒子が示す低温NH₃-SCR活性
猪股雄介, 美濃真, 秦慎一, 秦慎一, 清永英嗣, 盛田啓一郎, 引野健治, 吉田和広, 春田正毅, 村山徹, Journal of the Japan Petroleum Institute (Web), 62, 5, 2019年

150°C以下でNH₃-SCR活性を示すバルク酸化バナジウム触媒-4価バナジウムの効果-
猪股雄介, 秦慎一, 清永英嗣, 盛田啓一郎, 吉田和広, 春田正毅, 村山徹, 触媒討論会討論会A予稿集(CD-ROM), 124th, 2019年

Versatile etherification of alcohols with allyl alcohol by a titanium oxide- supported molybdenum oxide catalyst: gradual generation from titanium oxide and molybdenum oxide
Yoshihiro Kon, Tadahiro Fujitani, Takuya Nakashima, Toru Murayama, Wataru Ueda, CATALYSIS SCIENCE & TECHNOLOGY, 8, 18, 4618, 4625, 2018年10月
Etherification using allyl alcohol to produce allyl ether via dehydration is a fundamental technique for producing fine chemicals that can be applied to electronic devices. We demonstrate a sustainable method to synthesize allyl ethers from allyl alcohol with various alcohols up to a 91% yield, with water as the sole by-product. In this reaction, the active catalyst is gradually generated as the reaction proceeds through the simple mixing of TiO2 and MoO3. The dispersion of MoO3 on the spent catalyst has been observed by XRD, HAADF-STEM, and STEM-EDS mapping. This catalyst shows excellent catalytic activity by virtue of the highly dispersed nature of MoO3 supported on TiO2, which is reusable at least five times. According to a mechanistic study including the measurement of XPS of MoO3 on TiO2 and control experiments using SiO2 and Al2O3 supports, the suitable reducibility of MoO3 to coordinate the allyl moiety on TiO2 seems to be a key factor for high-yielding syntheses of various allyl ethers even under heterogeneous reaction conditions. The reaction mechanism is considered to be as follows: sigma-allyl species are formed from dehydration of the allyl alcohol, followed by a nucleophilic attack by another alcohol against the sigma-allyl carbon to give allyl ethers. The developed catalytic system should be suitable for easily handled syntheses of allyl ethers due to the employment of commercially available MoO3 and TiO2 with halide- and organic solvent-free reaction conditions., ROYAL SOC CHEMISTRY, 英語

ポリオキソメタレートに担持した金ナノ粒子触媒によるCO酸化反応
村山徹, 吉田拓也, 坂口紀史, 石田玉青, 春田正毅, 触媒討論会講演予稿集, 121st, 20‐22, 2018年03月09日
日本語

Facile Formation of Lactic Acid from a Triose Sugar in Water over Niobium Oxide with a Deformed Orthorhombic Phase
Nakajima, K., Hirata, J., Kim, M., Gupta, N.K., Murayama, T., Yoshida, A., Hiyoshi, N., Fukuoka, A., Ueda, W., ACS Catalysis, 8, 1, 283, 290, 2018年
© 2017 American Chemical Society. Hydrothermal treatment of NH4[NbO(C2O4)2(H2O)2]·nH2O in water at 448 K for 3 days produced crystalline Nb2O5with a deformed orthorhombic structure and a high surface area (208 m2g-1). Fourier-transform infrared spectroscopy measurements of pyridine adsorption revealed that the Nb2O5catalyst has both high densities of Brønsted and Lewis acid sites that can work in the presence of water. One feature of the Nb2O5catalyst is its high density of water-compatible Lewis acid sites (0.21 mmol g-1), which is much larger than that of Nb2O5·nH2O (0.03 mmol g-1). The Nb2O5catalyst was studied as a solid acid catalyst for the formation of lactic acid from 1,3-dihydroxyacetone and pyruvaldehyde in water at 373 K, and was determined to be a highly active and selective catalyst, compared with typical acid catalysts (H2SO4, Sc(OTf)3, and Nb2O5·nH2O). A high Lewis acid density with moderate acid strength is a crucial factor for the high catalytic performance exhibited for the former reaction. High densities of both Brønsted and Lewis acid sites in the catalyst promote the fast and selective production of lactic acid in the latter reaction. In addition, Such Lewis acidity of the Nb2O5is also effective over conventional acid catalysts in xylose dehydration to furfural in water, with respect to reaction rate and furfural selectivity. The combination of aqueous-phase dehydration of xylose over the Nb2O5and the continuous extraction of furfural with an immiscible organic solvent resulted in a high selectivity toward furfural of ∼78.5% with high xylose conversion (97%).

MoO₃担持チタニア触媒を鍵とする高選択的脱水型非対称アリルエーテル合成法の開発
今 喜裕, 矢田 陽, 中村 陽一, 藤谷 忠博, 中島 拓哉, 村山 徹, 上田 渉, 石油学会要旨集, 2018, 0, 2018年
従来の電子材料用途アリルエーテルの合成法では、塩化アリルを原料に用いるため、製品純度の低下、副生成物の処理、触媒コストが問題となる。我々は、アリルアルコールと1-オクタノールをTiO₂+MoO₃触媒存在下140 ℃で4時間反応させると、アリルオクチルエーテルが収率84%で得られることを発見し、塩素フリーな高選択的アリルエーテルの合成法を開発した。副生物は水のみで触媒は回収再使用できる。詳細な触媒解析と反応成績の考察から、反応機構の検討も行なった。, 公益社団法人 石油学会, 日本語

トルエンの安息香酸への選択酸化に高活性なW-V複合酸化物触媒の活性種構造
清水研一, 後藤文倫, 鳥屋尾隆, 村山徹, 日吉範人, 上田渉, 石油学会年会講演要旨, 61st, 0, 2018年
水熱合成によりW-V複合酸化物触媒を合成した。各種キャラクタリゼーションにより本触媒のバルク・表面構造を決定した。本触媒はトルエンの安息香酸への選択酸化に高い収率（７０％）を示した。対照触媒との比較から活性種の局所構造を提案する。, 公益社団法人 石油学会, 日本語

酸化物に担持した金ナノ粒子の抗炎症作用
藤田隆史, 石田玉青, 村山徹, 春田正毅, ラノーン ソフィー, ボクツコウスキ ジョージ, 日本生化学会大会(Web), 91st, 2018年

担持金ナノ粒子触媒による脂肪族アルデヒド,アルコールの酸化的エステル化
竹歳絢子, 石田玉青, 村山徹, 春田正毅, 触媒討論会討論会A予稿集, 122nd, 2018年

フルフラール酸化における金ナノ粒子触媒の担体・サイズ効果
望月ちひろ, 竹歳絢子, 石田玉青, 春田正毅, 村山徹, 酸化反応討論会講演要旨集, 51st, 2018年

酸化モリブデン担持触媒によるアミンのアリル化反応
今喜裕, 藤谷忠博, 中島拓哉, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 122nd, 2018年

低温(200°C以下)でのNOのNH₃-SCRにおけるV₂O₅の触媒作用
秦慎一, 猪股雄介, 美濃真, 清永英嗣, 盛田啓一郎, 吉田和広, 春田正毅, 村山徹, 触媒討論会討論会A予稿集, 122nd, 2018年

ポリオキソメタレートに担持した金クラスター触媒によるCO酸化反応-ポリオキソメタレート担体の効果-
猪股雄介, 吉田拓也, 春田正毅, 村山徹, 触媒討論会討論会A予稿集, 122nd, 2018年

酸化バナジウムを用いた低温(200°C以下)におけるNOのNH₃-SCR
秦慎一, 秦慎一, 猪股雄介, 美濃真, 清永英嗣, 盛田啓一郎, 吉田和広, 春田正毅, 村山徹, 分子科学討論会講演プログラム&要旨(Web), 12th, 2018年

Low-Temperature CO Oxidation over Combustion Made Fe- and Cr-Doped Co3O4 Catalysts: Role of Dopant's Nature toward Achieving Superior Catalytic Activity and Stability
Tinku Baidya, Tom Murayama, Parthasarathi Bera, Olga V. Safonova, Patrick Steiger, Nirmal Kumar Katiyar, Krishanu Biswas, Masatake Haruta, JOURNAL OF PHYSICAL CHEMISTRY C, 121, 28, 15256, 15265, 2017年07月
Co3O4 with a spinel structure shows unique activity for CO oxidation at low temperature under dry conditions; however the active surface is not very stable. In this study, two series of Fe- and Cr-doped Co3O4 catalysts were prepared by a single-step solution combustion technique. Fe was chosen because of its redox activity corresponding to the Fe2+/Fe3+ redox couple and compared to Cr, which is mainly stable in the Cr3+ state. The catalytic activity of new materials for low-temperature CO oxidation was correlated to the nature of the dopant. As a function of dopant concentration, the temperature corresponding to the 50% CO conversion (T-50) demonstrated significant differences. The maximal activity was achieved for 15% Fe-doped Co3O4 with T-50 of -85 degrees C and remained almost constant up to 25% Fe. In the case of Cr, the activity was observed to be maximum 100 for 7% of Cr with T50 of -42 degrees C and significantly decreased for higher Cr loadings. Similarly, there was a contrasting behavior in catalyst stability too. 100% CO conversion was achieved below -60 degrees C for 15% Fe/Co3O4 catalyst and remained unchanged even after calcination at 600 degrees C. In contrast, Co3O4 or 15% Cr/Co3O4 catalysts strongly deactivated after the same treatment. These differences were correlated to the oxidation states, coordination numbers, the nature of surface planes, and the redox properties. We observed that both Cr and Fe were typically present in the +3 oxidation state, occupying octahedral sites in the spinel structure. The catalysts were mainly exposed to (111) and (220) planes on the surface. H-2-TPR indicated clear differences in the redox activity of materials due to Fe and Cr substitutions. The reducibility of surface Co3+ species remained similar in all Fe-doped Co3O4 catalysts in contrast to nonreducible Cr-doped analogs, which shifted the reduction temperature to the higher values. As the Fe3+/Fe2+ redox couple partly substituted the Co3+/Co2+ redox couple in the spinel structure, similar bond strength of Fe-O keep redox activity of Co3+ species almost unchanged leading to higher activity and stability of Fe/Co3O4 catalysts for low-temperature CO oxidation. In contrast, nonreducible Cr3+ species characterized by strong Cr-O bond substituting active Co3+ sites can make the Cr/Co3O4 surface less active for CO oxidation., AMER CHEMICAL SOC, 英語

Synthesis of Crystalline Microporous Mo-V-Bi Oxide for Selective (Amm)Oxidation of Light Alkanes
Ishikawa, S., Goto, Y., Kawahara, Y., Inukai, S., Hiyoshi, N., Dummer, N.F., Murayama, T., Yoshida, A., Sadakane, M., Ueda, W., Chemistry of Materials, 29, 7, 2939, 2950, 2017年
© 2017 American Chemical Society. Bismuth (Bi) was successfully introduced into the crystalline orthorhombic Mo3VOx(MoVO) structure for the first time by using the ethylammonium cation (EtNH3+) as a structure-directing agent in hydrothermal synthesis, and the catalytic activities of MoVO-containing Bi (MoVBiO) for selective oxidation of ethane and ammoxidation of propane were compared with those of ternary MoVO. Bi and EtNH3+were located in hexagonal and heptagonal channels in the MoVO structure, respectively. EtNH3+could be removed without collapse of the crystal structure by appropriate heat treatment, leaving the heptagonal channels empty. The introduction of Bi had only a little effect on the catalytic activity for selective oxidation of ethane. On the other hand, the conversion of propane was significantly enhanced in propane ammoxidation. Acrylonitrile selectivity was also enhanced by the introduction of Bi, especially at high temperatures (>440 °C).

金ナノ粒子を担持した酸化ニオブ触媒によるフルフラールの酸化反応
村山 徹, 竹歳 絢子, 石田 玉青, 春田 正毅, 石油学会要旨集, 2017, 0, 2017年
金ナノ粒子を担持した酸化ニオブを用いてフルフラールの酸化反応を行った。実験は液相流通式反応装置を用いた。担体にアモルファス酸化ニオブ、単斜晶酸化ニオブ、斜方晶酸化ニオブ、層状酸化ニオブを用いて検討したところ、層状酸化ニオブに金を担持すると高活性であった。金担持層状酸化ニオブを用いたフルフラールの酸化反応は、反応温度が50℃から100℃において効率よく進行し、それ以上はフロ酸への選択率が低下した。, 公益社団法人 石油学会, 日本語

Au/Nb₂O₅触媒を用いた気相・液相酸化反応における担体の結晶相および酸性質の影響
村山徹, GUPTA Navneet Kumar, 中島清隆, 福岡淳, 春田正毅, 触媒討論会講演予稿集, 119th, 2017年

結晶性Mo-V-Bi複合酸化物の合成とそれを用いた低級アルカン(アンモ)酸化反応
石川理史, 後藤文倫, 河原義人, 犬飼将槙, 日吉範人, DUMMER Nicholas F., 村山徹, 吉田暁弘, 定金正洋, 上田渉, 触媒討論会討論会A予稿集, 120th, 2017年

金ナノ粒子担持触媒を用いたフルフラール酸化
村山徹, GUPTA Navneet Kumar, 中島清隆, 福岡淳, 春田正毅, 触媒討論会討論会A予稿集, 120th, 2017年

酸化バナジウムを用いた低温(200°C以下)におけるNOのNH₃-SCR
秦慎一, 村山徹, 美濃真, 清永英嗣, 盛田啓一郎, 引野健治, 春田正毅, 触媒討論会討論会A予稿集, 120th, 2017年

メソポーラスシリカ上に調製した酸化ニオブ薄膜を担体とした金ナノ粒子触媒の触媒活性評価
日吉優貴, 大須賀遼太, 横井俊之, 村山徹, 春田正毅, 野村淳子, 触媒討論会討論会A予稿集, 120th, 2017年

マグネシウムの水素吸蔵放出反応における種々のNb酸化物の触媒効果
宮岡裕樹, 新里恵多, 魏弘之, 定金正洋, 村山徹, 市川貴之, 日本金属学会講演概要(CD-ROM), 161st, 2017年

ポリオキソメタレートに担持した金クラスター触媒によるCO酸化反応
吉田拓也, 村山徹, 春田正毅, 触媒討論会講演予稿集, 119th, 2017年

W-Ti-O複合金属酸化物触媒によるアルコールの脱水交差エーテル化反応
矢田陽, 村山徹, 平田純, 中島拓哉, 今喜裕, 上田渉, 触媒討論会討論会A予稿集, 120th, 2017年

マイクロポーラスMo-V-O複合酸化物の調製と選択酸化反応への応用
石川 理史, 村山 徹, 上田 渉, ゼオライト, 33, 4, 110, 120, 2016年10月15日
ゼオライト学会, 日本語

酸化バナジウムを用いたNOの低温NH₃触媒的選択還元
美濃真, 村山徹, 春田正毅, 触媒討論会討論会A予稿集, 118th, 435, 2016年09月14日
日本語

酸性酸化物(Nb₂O₅)への金ナノ粒子担持
村山徹, 春田正毅, 触媒討論会討論会A予稿集, 118th, 254, 2016年09月14日
日本語

金ナノ粒子担持触媒の基礎および実用化研究~造粒と触媒活性~
村山徹, TIRIクロスミーティング要旨集, 2016, 114, 2016年06月08日
日本語

金ナノ粒子担持触媒の利用~バイオマス転換反応を例に~
村山徹, 触媒, 58, 2, 114, 2016年04月10日
日本語

固体酸性を示す酸化物担体への金ナノ粒子の担持:Au/NbOxの調製とその触媒活性
村山徹, 春田正毅, 触媒討論会講演予稿集, 117th, 196, 2016年03月10日
日本語

結晶性ニオブ酸によるトリオース水溶液からの乳酸合成
中島 清隆, 村山 徹, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2016, 0, 130, 130, 2016年
水溶性ニオブ錯体を水熱処理することによって結晶性のニオブ酸が合成できる。得られたニオブ酸はブレンステッド酸とルイス酸を有しており、それらの酸触媒サイトは吸着水存在下において塩基性プローブ分子と相互作用することができる。この触媒をトリオース水溶液に加えて加熱したところ、約80%の収率で乳酸が生成した。高い触媒活性は水中で機能するルイス酸およびブレンステッド酸の有効酸量が大きいためであると考えられる。, 公益社団法人 石油学会, 日本語

構造規定剤を用いて合成した三方晶Mo-V-M-O (M = Fe, W)のエタンおよびアクロレイン選択酸化活性
石川 理史, 村山 徹, 田代 雅也, ジェンシン ジャン, 吉田 曉弘, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2015, 0, 196, 196, 2015年11月05日
構造規定剤を用いることで、三方晶Mo-V-O, Mo-V-Fe-O, およびMo-V-W-Oを得た。これらは積層構造体であり、断面部にはMoから成る5員環ユニットとVによるネットワークにより、5、6、および7員環が形成している。Feは構造の7員環部位に位置しており、Wは5員環ユニット中のMoと置換していた。これらを用いて触媒反応を行ったところ、Mo-V-OとMo-V-W-Oはエタン、アクロレインの選択酸化反応にほぼ同様の活性を示した。一方、Mo-V-Fe-Oでは、触媒活性が激減した。触媒構造と触媒活性の明瞭な関係が見て取れた。, 公益社団法人 石油学会, 日本語

Cu-Zr-O触媒を用いたレブリン酸の水素化反応およびその触媒活性化部位
石川理史, 石川理史, JONES Daniel R., IQBAL Sarwat, MORGAN David J., WILLOCK David J., BARTLEY Jonathan K., EDWARDS Jennifer K., 村山徹, 清水研一, 上田渉, HUTCHINGS Graham J., 触媒討論会討論会A予稿集, 116th, 203, 2015年09月09日
日本語

担持金触媒によるアンモニアを用いた低温でのNO_x選択還元(NH₃‐SCR)
美濃真, 村山徹, 春田正毅, 触媒討論会討論会A予稿集, 116th, 391, 2015年09月09日
日本語

Ultrathin inorganic molecular nanowire based on polyoxometalates
Zhenxin Zhang, Toru Murayama, Masahiro Sadakane, Hiroko Ariga, Nobuhiro Yasuda, Norihito Sakaguchi, Kiyotaka Asakura, Wataru Ueda, NATURE COMMUNICATIONS, 6, 0, 2015年07月
The development of metal oxide-based molecular wires is important for fundamental research and potential practical applications. However, examples of these materials are rare. Here we report an all-inorganic transition metal oxide molecular wire prepared by disassembly of larger crystals. The wires are comprised of molybdenum(VI) with either tellurium(IV) or selenium(IV): {(NH4)(2)[XMo6O21]}(n) (X = tellurium(IV) or selenium(IV)). The ultrathin molecular nanowires with widths of 1.2 nm grow to micrometre-scale crystals and are characterized by single-crystal X-ray analysis, Rietveld analysis, scanning electron microscopy, X-ray photoelectron spectroscopy, ultraviolet-visible spectroscopy, thermal analysis and elemental analysis. The crystals can be disassembled into individual molecular wires through cation exchange and subsequent ultrasound treatment, as visualized by atomic force microscopy and transmission electron microscopy. The ultrathin molecular wire-based material exhibits high activity as an acid catalyst, and the band gap of the molecular wire-based crystal is tunable by heat treatment., NATURE PUBLISHING GROUP, 英語

V₂O₃およびMoO₂触媒を用いた分子内水素移行反応によるジオール類転換反応
中村 陽一, 村山 徹, 清水 研一, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2015, 0, 51, 51, 2015年05月26日
V₂O₃およびMoO₂触媒を用いたジオール転換反応について検討した。V₂O₃およびMoO₂触媒によるプロピレングリコールの転換反応では主生成物としてアセトンが観測され、副生成物としてプロピオンアルデヒドとプロピレンが同程度の選択率で生成した。V₂O₃およびMoO₂触媒によるプロピオンアルデヒドの生成は触媒表面に存在する酸サイトにて進行したと考えられる。本反応メカニズムの詳細を検討したところ、V₂O₃およびMoO₂触媒におけるアセトン生成は、水素移行脱水反応がプロピレングリコールの分子内にて進行すると提案した。, 公益社団法人 石油学会, 日本語

V₂O₃およびMoO₂触媒を用いた水素移行脱水反応によるアルコールからのアルカン,アルデヒドおよびケトン同時生成
中村陽一, 村山徹, 上田渉, 触媒討論会講演予稿集, 115th, 34, 36, 2015年03月10日
日本語

水熱合成により調製したW‐M‐O(M=Ti,Zr,Nb,Ta)触媒による加水分解および脱水反応
村山徹, 上田渉, 触媒討論会講演予稿集, 115th, 73, 2015年03月10日
日本語

Light alkane activation chemistry and technology using high dimensional crystalline complex metal oxide catalysts
Wataru Ueda, Satoshi Ishikawa, Toru Murayama, King Fahd University of Petroleum and Minerals, Research Institute - Annual Catalysts in Petroleum Refining and Petrochemicals Symposium Papers, 2015-January, 2, 12, 2015年01月01日
Research works on effective utilization of alkanes as sources of alkenes and their derivatives production are increasing because of the shale gas revolution and methane hydrate. Light alkanes are poorly reactive due to no lone pairs of electrons, no empty orbital, and little polarity of the C-H bonds, thus, the desired processes for the utilization are considered of catalytic technology, particularly catalytic oxidation. Complex metal oxides with high dimensional structures in nano-scale seem have high potentiality, particularly, crystalline Mo3VOx. Developments on complex metal oxide catalysts based on Mo3VOxmaterials for selective alkane oxidation are presented. Pure Mo3VOxare described in terms of crystal structure, structure formation, element incorporation, and alkane catalytic oxidation chemistry, particularly for ethane oxidation. This is an abstract of a paper presented at the 25th Annual Saudi-Japan Symposium on Catalysts in Petroleum Refining and Petrochemicals 2015 (Dhahran, Saudi Arabia 12/7-8/2015).

Light alkane activation chemistry and technology using high dimensional crystalline complex metal oxide catalysts
Wataru Ueda, Satoshi Ishikawa, Tom Murayama, International Air Safety Seminar Proceedings, 2015-January, 8, 18, 2015年01月01日
Effective utilization of alkanes as sources of alkenes and their derivatives production has long been targeted in chemistry and technological researches and the interest is even now expanding because of the shale gas revolution and methane hydrate. The targets are, however, still challenging. The main problem is that light alkanes are poorly reactive due to no lone pairs of electrons, no empty orbital, and little polarity of the C-H bonds, so that desired processes for the utilization are considered of catalytic technology, particularly catalytic oxidation. Complex metal oxides with high dimensional structures in nano-scale appear to have high potentiality, since the complex metal oxide materials can attain multi-functional catalytic properties. The most prominent examples is crystalline Mo3VOX, which is a new type of complex metal oxide catalysts and relating MoVTeNbO catalysts have been found highly active for alkane oxidation in gas-phase. The presentation will first focus on recent developments on complex metal oxide catalysts based on Mo3VOxmaterials for selective alkane oxidation and then more details on pure Mo3VOxmaterials will be described in terms of crystal structure, structure formation, element incorporation, and alkane catalytic oxidation chemistry, particularly for ethane oxidation.

結晶性Mo₃VO_xの7員環反応場を利用した低級アルカン,アルデヒド,アルコールの酸化反応
村山徹, 石川理史, QIU Chuntian, 後藤文倫, 上田渉, 酸化反応討論会講演要旨集, 47th, 62, 64, 2014年11月14日
日本語

W-Ti-O触媒によるスルフィドの高選択酸化反応の開発
今喜裕, 村山徹, 田中真司, 平田純, 中島拓哉, 佐藤一彦, 上田渉, 上田渉, 酸化反応討論会講演要旨集, 47th, 103, 105, 2014年11月14日
日本語

水熱合成法により調製したW‐Nb(‐V)‐O複合酸化物触媒による乳酸酸化反応
村山徹, 小俣香織, KATRYNIOK Benjamin, PAUL Sebastien, 上田渉, 石油・石油化学討論会講演要旨, 44th, 0, 139, 2014年10月16日
水熱合成法により調製したW-Nb-V-O複合酸化触媒を用いて乳酸の酸化反応を行った。合成した触媒は、共通して金属オクタヘドラル構造が点共有によりC軸方向に積層した層状の構造を有していた。Vの含有量を変化させて乳酸の酸化反応を行ったところ、V含有量が多くなるに従い、ピルブアルデヒドの生成量が増加した。触媒の金属組成比がW₂Nb_2.7V_1.2O_xのとき、ピルブアルデヒドの収率が19 %であった。, 公益社団法人 石油学会, 日本語

種結晶添加法による結晶性MoVO複合酸化物触媒の合成と低級アルカン選択酸化反応
田代雅也, 石川理史, 村山徹, 上田渉, 石油・石油化学討論会講演要旨, 44th, 0, 357, 2014年10月16日
結晶性MoVO複合酸化物は低級アルカンの選択酸化反応に高い活性を示す触媒である。前駆体溶液のpHを調整することで斜方晶、三方晶などの結晶相が作り分けられる。今回、種結晶添加法をMoVO合成に応用することにより、広いpH領域において容易に触媒の作り分けが可能となった。得られた触媒のキャラクタリゼーションや反応活性試験から、種結晶を用いて合成した試料も種結晶と同様に高い活性を示すことが明らかとなった。, 公益社団法人 石油学会, 日本語

水熱合成W-V-O複合酸化物触媒によるピコリンのアンモ酸化
後藤文倫, 村山徹, 清水研一, 上田渉, 石油・石油化学討論会講演要旨, 44th, 143, 2014年10月16日
日本語

水熱合成W-V-O複合酸化物触媒によるピコリンのアンモ酸化
後藤文倫, 村山徹, 清水研一, 上田渉, 触媒討論会討論会A予稿集, 114th, 0, 126, 2014年09月18日
当研究室では水熱法により合成した結晶性層状構造複合酸化物触媒を報告してきた。一連の触媒はその構造に由来した高い活性を有している。本研究では同様の構造を有するW-V-O複合酸化物がピコリンのアンモ酸化反応において高収率でシアノピリジンを与えることを見出した。各組成の触媒性能の違いから活性要因についても考察する。, 公益社団法人 石油学会, 日本語

水素移行脱水反応機構によるV₂O₃およびMoO₂上でのアルコールからのアルカン,アルデヒド同時生成
中村陽一, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 114th, 424, 2014年09月18日
日本語

4,5族元素とWからなる複合酸化物の水熱合成と酸触媒機能
村山徹, 平田純, 上田渉, 触媒討論会討論会A予稿集, 114th, 183, 184, 2014年09月18日
日本語

種結晶添加による斜方晶MoOx酸化物の水熱合成
田代雅也, 石川理史, 坂口紀史, 村山徹, 清水研一, 上田渉, 触媒討論会討論会A予稿集, 114th, 150, 2014年09月18日
日本語

4,5,6族遷移金属元素を用いた複合酸化物触媒の合成とその固体酸性質
村山徹, 東京工業大学応用セラミックス研究所共同利用研究報告書, 2013, 113, 2014年06月30日
日本語

斜方晶Mo₃₀V₁₀O₁₁₂複合酸化物触媒の酸化還元処理に伴うミクロ細孔径制御およびそのエタン選択酸化触媒活性
石川理史, 小林大地, 紺谷岳史, 大村俊平, 村山徹, 定金正洋, 上田渉, 触媒討論会講演予稿集, 113th, 32, 34, 2014年03月10日
日本語

Effects of W on the selective oxidation of acrolein to acrylic acid over orthorhombic and trigonal Mo-V-W-O
Qiu Chuntian, 石川 理史, 村山 徹, 上田 渉, 石油学会要旨集, 2014, 0, 2014年
Orthorhombic and trigonal phase Mo-V-W-O complex oxides were synthesized with one-step hydrothermal method. And their catalytic activity for selective oxidation of acrolein to acrylic acid was investigated. The results showed that both of orthorhombic and trigonal phase Mo-V-W-O complex oxides are excellent catalysts for acrolein oxidation to acrylic acid especially under low water partial pressure.&nbsp;, 公益社団法人 石油学会, 日本語

W複合酸化物触媒によるグリセロールからのアクリル酸合成
小俣香織, 松本慶江子, 村山徹, 上田渉, 酸化反応討論会講演要旨集, 46th, 109, 111, 2013年11月15日
日本語

層構造を有するW系複合酸化物の水熱合成およびその固体酸性質
平田純, 小俣香織, 倉又望, 村山徹, 上田渉, 石油・石油化学討論会講演要旨, 43rd, 0, 25, 2013年11月14日
我々はこれまで水熱合成法により合成したW-M-O酸化物(M=Zr,Ti,Nb,V,Ta)が固体酸性質を有しており、フリーデル・クラフツアルキル化反応に高い活性を示すことを報告してきた。今回、種々の水熱合成条件の検討を行い、調製したW-M-O複合酸化物触媒の結晶構造、細孔特性，酸触媒性能の評価を行った。その結果、XRDにおいて積層構造を示す23&deg;にピークを与える物質が高い固体酸触媒性質を有していることが分かった。, 公益社団法人 石油学会, 日本語

複雑結晶構造を持った選択酸化用複合酸化物触媒 (特集 次世代型触媒開発の新潮流)
上田 渉, 村山 徹, 石川 理史, 化學工業, 64, 10, 785, 791, 2013年10月01日
小峰工業出版, 日本語

複雑結晶構造を持った選択酸化用複合酸化物触媒 (特集 次世代型触媒開発の新潮流)
上田 渉, 村山 徹, 石川 理史, 化學工業, 64, 10, 785, 791, 2013年10月
小峰工業出版, 日本語

三方晶Mo‐V‐M‐O(M=Fe,Cu,Nb,Ta,W)の合成および低級アルカン選択酸化触媒活性
石川理史, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 112th, 274, 2013年09月11日
日本語

還元VおよびMo酸化物を用いたエタノール転換反応
中村陽一, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 112th, 486, 2013年09月11日
日本語

種結晶を用いた結晶性Mo‐V‐O複合酸化物の調製と水熱下生成機構
田代雅也, 石川理史, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 112th, 487, 2013年09月11日
日本語

水熱合成法により調製したW‐Ta‐O複合酸化物の構造と固体酸性質
村山徹, 倉又望, 上田渉, 触媒討論会討論会A予稿集, 112th, 159, 2013年09月11日
日本語

W複合酸化物触媒の表面機能とグリセロール転換反応の選択性との関連
小俣香織, 松本慶江子, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 112th, 210, 2013年09月11日
日本語

結晶性Mo-V-O複合酸化物を用いた低級アルカン選択酸化反応
村山 徹, 上田 渉, 觸媒 = Catalyst, 55, 3, 148, 153, 2013年06月10日
触媒学会, 日本語

エタノールからのエタン生成におけるバナジウム酸化物触媒の還元種の影響
中村 陽一, 村山 徹, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2013, 38, 38, 2013年05月28日
バナジウム酸化物触媒を用いてエタノール転換反応にて触媒性能を検討したところ、エタンおよびアセトアルデヒドが各々収率約30 %で生成した。バナジウム酸化物によるエタノールの選択酸化反応では、生成物としてアセトアルデヒドやエチレンが生成するという報告例は多数あるが、エタン生成に関する報告例はない。そこで本研究では、バナジウム酸化物の新たな触媒性能を検討するために、バナジウム酸化物におけるアルコールからのアルカン生成についての詳細な検討を行った。, 公益社団法人 石油学会, 日本語

層構造を有するW-Ti-O複合酸化物の水熱合成およびその酸触媒活性
平田 純, 村山 徹, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2013, 0, 37, 37, 2013年05月28日
硫酸チタン(III)、メタタングステン酸アンモニウムおよびシュウ酸の混合水溶液を175 ℃で24時間水熱合成を行い、複合酸化物を調製した。前駆体のW/Tiモル比および、前駆体濃度およびシュウ酸の添加量を変化させることにより、積層構造を有するW-Ti-O複合酸化物触媒が得られた。合成したW-Ti-O複合酸化物触媒は、ピリジン吸着IRおよびアンモニアTPDにより固体酸性質を有することが分かった。種々の基質を用いてフリーデルクラフツ・アルキル化反応を検討したところ、既報の固体酸触媒と比較し高い反応活性を示した。, 公益社団法人 石油学会, 日本語

グリセロールからのアクリル酸一段階合成のためのW複合酸化物触媒の開発
小俣香織, 松本慶江子, 村山徹, 上田渉, 触媒討論会講演予稿集, 111th, 14, 16, 2013年03月11日
日本語

固体酸化物触媒の真髄に迫る 複雑結晶構造が生みだす触媒機能
上田渉, 村山徹, 化学, 68, 2, 70, 71, 2013年02月01日
日本語

三方晶Mo‐V‐O複合酸化物触媒の酸化活性に対する酸化還元処理効果
小林大地, 村山徹, 上田渉, 酸化反応討論会講演要旨集, 45th, 191, 193, 2012年11月16日
日本語

界面活性剤を添加して合成した斜方晶Mo₃VO_xの低級アルカン選択酸化活性
石川理史, 村山徹, 上田渉, 酸化反応討論会講演要旨集, 45th, 188, 190, 2012年11月16日
日本語

複合酸化物型固体酸触媒を用いたアルコールの転換反応
村山 徹, 中村 陽一, 倉又 望, 平田 純, 小俣 香織, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2012, 0, 166, 166, 2012年10月11日
複合酸化物型固体酸触媒を合成し、アルコールの転換反応を検討した。触媒はタングステン、モリブデン、バナジウム、ニオブ、タンタルの5，6族元素を用いて水熱処理により種々の複合酸化物を合成した。調製した固体酸触媒は、XRD、NH₃-TPD、STEMでキャラクタリゼーションを行った。また、得られた生成物を比較検討することで、触媒の持つ酸性質を検討した。, 公益社団法人 石油学会, 日本語

水熱法によるW-Ti-O複合酸化物の合成とその酸触媒特性
平田純, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 110th, 168, 2012年09月14日
日本語

W複合酸化物触媒の合成とグリセロール転換反応への応用
小俣香織, 泉彰子, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 110th, 207, 2012年09月14日
日本語

Mo‐Zr‐O層状複合酸化物触媒の合成と構造解析
安藤雅朗, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 110th, 411, 2012年09月14日
日本語

結晶性W(Mo)‐Ta‐O複合酸化物の結晶構造と固体酸性質
倉又望, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 110th, 169, 2012年09月14日
日本語

三方晶Mo‐V‐O複合酸化物の構造解析と酸化触媒活性
小林大地, 石川理史, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 110th, 391, 2012年09月14日
日本語

界面活性剤を用いた結晶性Mo‐V‐O複合酸化物の合成および低級アルカン選択酸化活性
石川理史, XI Xiaodong, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 110th, 390, 2012年09月14日
日本語

水熱合成法を用いたW‐V‐Sb‐O複合酸化物系触媒の合成とその酸化触媒活性
後藤文倫, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 110th, 395, 2012年09月14日
日本語

複合酸化物型固体酸触媒を用いたアルコールの転換反応
村山 徹, 中村 陽一, 倉又 望, 平田 純, 小俣 香織, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2012, 0, 166, 166, 2012年
複合酸化物型固体酸・塩基触媒を合成し，アルコールの転換反応を検討した．触媒はW，Mo，Zrなどの遷移金属およびSi，Mgの組み合わせを水熱条件下または固相法にて複合化し調製した．調製した固体酸・塩基触媒は，XRD，NH₃-TPD，CO₂-TPD，SEM，元素分析でキャラクタリゼーションを行った．合成した触媒の活性および生成物選択性を基に，触媒の構造と構成元素の役割および固体酸・塩基性質の解明を試みた．, 公益社団法人 石油学会, 日本語

Epoxidation of olefin catalyzed by a new microporous material based on molybdenum, vanadium, and bismuth
Zhang Zhenxin, 泉 彰子, 村山 徹, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2012, 0, 122, 122, 2012年
A novel microporous complex metal oxide based on molybdenum, vanadium, and bismuth (Mo-V-Bi oxide) was synthesized by hydrothermal method and characterized by STEM, TEM, XRD, FT-IR, Raman, TPD, NH₃-TPD, and N₂ adsorption. The results showed that Mo-V-Bi oxide was crystalline material with high porosity and surface area. The single crystal of Mo-V-Bi oxide was obtained for single crystal analysis to gain full structural information of this material. This material was used as a heterogeneous catalyst for olefin epoxidation with TBHP. The stable catalyst could be reused for several times without loss of activity., 公益社団法人 石油学会, 日本語

W-Nb-O複合酸化物の合成と酸触媒機能
小俣香織, 泉彰子, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 109th, 2012年

水熱合成法によるMo-(Nb,Ta)-O複合酸化物触媒の合成と酸触媒能の評価
村山徹, 倉又望, 泉彰子, 上田渉, 触媒討論会討論会A予稿集, 109th, 2012年

5,6族元素を用いた複合酸化物の合成と固体酸性質評価
村山徹, YI Xiaodong, 高玉峻介, 泉彰子, 上田渉, 触媒討論会討論会A予稿集, 107th, 2011年

Pd(0)ナノ粒子担持炭素触媒によるフェノールの電解カルボニル化
村山徹, 林外茂彦, 山中一郎, 触媒討論会討論会A予稿集, 108th, 2011年

低級アルカン酸化反応におけるMo₃VO_xの触媒性能と活性点について
紺谷岳史, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 108th, 2011年

各種有機アンモニウムモリブデン酸塩を用いたMo-V-O複合酸化物の合成および低級アルカン酸化活性
石川理史, 紺谷岳史, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 108th, 2011年

熱活性化Fe-TPP/C触媒による炭化水素の選択部分酸化
柳下亮, 越智紀明, 村山徹, 上田渉, 山中一郎, 触媒討論会討論会A予稿集, 108th, 2011年

熱活性活性化Co-TPP/C電極触媒による過酸化水素の選択合成
岩崎達也, 西村直也, 村山徹, 上田渉, 山中一郎, 触媒討論会討論会A予稿集, 108th, 2011年

水熱合成法によるW-Zr-O複合酸化物の合成と酸触媒特性
安藤雅郎, 泉彰子, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 108th, 2011年

種々の水熱条件で合成した多孔性W-Ta-O複合酸化物の結晶構造および酸触媒能
倉又望, 泉彰子, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 108th, 2011年

Mo-Nb-O複合酸化物を用いた酸触媒能の評価
村山徹, 泉彰子, YI Xiaodong, 上田渉, 触媒討論会討論会A予稿集, 108th, 2011年

低級アルカン酸化反応におけるMo₃VO_x触媒の還元度の影響
紺谷岳史, 村山徹, 上田渉, 酸化反応討論会講演要旨集, 44th, 2011年

水熱合成法による5族6族元素を用いた固体酸触媒合成
村山 徹, Yi Xiaodong, 倉又 望, 泉 彰子, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2011, 0, 9, 9, 2011年
既に我々は、水熱合成により細孔を有する結晶性Mo-V-O触媒の合成に成功し報告した。この手法を応用し、5、6族元素をベースとした新規結晶性複合金属酸化物触媒の合成に展開した。実際に水熱合成法を用いてMoVO、MoNbO、MoTaO、WVO、WNbO、WTaOを合成し、合成した酸化物の固体酸性質をフリーデル・クラフツアルキル化反応を用いて評価した。, 公益社団法人 石油学会, 日本語

The propane ammoxidation over trigonal Mo-V-Te-O catalysts
Yi Xiaodong, 村山 徹, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2011, 0, 8, 8, 2011年
The selective oxidation of propane to oxygenates has attracted a lot of attention. Among the catalysts that has been tested for propane oxidation so far, MoVTeNbO is the most active and selective catalyst for the oxidation of propane. Our group have succeeded in synthesizing monophasic orthorhombic MoVO with or without other element(Te, Sb or Nb) under hydrothermal conditions. In the present study, we tried to synthesize single-phase MoVTeO with trigonal structure and tested its catalytic activity by propane ammoxidation., 公益社団法人 石油学会, 日本語

高難度フェノールの電解カルボニル化によるノンホスゲンＤＰＣ合成
山中 一郎, 村山 徹, 林 外茂彦, 兼賀 量一, 石油学会 年会・秋季大会講演要旨集, 2011, 0, 186, 186, 2011年
既に我々は、PdCl2/ACアノードがフェノールの酸化的カルボニル化による炭酸ジフェニル合成に活性を示すことを報告している。今回アノード触媒の適切化を行ったところ、Pdナノ金属粒子を炭素上に担持した触媒が炭酸ジフェニル合成に高活性を示すことを見出した。Pd粒子径とカルボニル化活性の間には強い依存性があることを見出した。, 公益社団法人 石油学会, 日本語

W-Nb複合酸化物触媒によるグリセロールからのアクロレイン合成
小俣 香織, 泉 彰子, 村山 徹, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2011, 0, 52, 52, 2011年
水熱合成法により調製したWとNb複合酸化物は、層構造に起因するXRDパターンを有する。このW-Nb複合酸化物をグリセロール転換反応に用いたところ、脱水により高選択的にアクロレインが得られることが分かった。発表では、W-Nb複合酸化物の調製条件や、種々の金属添加が、生成物分布に与える影響について述べる。, 公益社団法人 石油学会, 日本語

三方晶Mo-V-(Nb,Te)-O複合酸化物触媒を用いたプロパンのアンモ酸化
Yi Xiaodong, 小林 大地, 紺谷 岳史, 村山 徹, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2011, 0, 95, 95, 2011年
プロパンのアンモ酸化反応には、MoVNbTeO複合酸化触媒が高い活性を示すと数多くの報告がある。しかしながら、それぞれの金属元素の役割につては明確ではない。これまで我々は、Mo、Vのみを構成元素に用いた三方晶Mo-V-Oを合成し報告を行ってきた。今回、三方晶Mo-V-Oおよび、第三成分としてNbまたはTeを添加した三方晶MoV(Nb,Te)O複合酸化触媒を調製し、アンモ酸化反応，プロパン酸化，エタン酸化，メタン酸化により活性を評価することにより、触媒の結晶構造および金属成分の役割の解明を検討した。, 公益社団法人 石油学会, 日本語

北海道での研究が Kick Off
村山 徹, 觸媒 = Catalyst, 52, 8, 600, 601, 2010年12月10日
日本語

Pd電極触媒による炭酸ジフェニル(DPC)の常温常圧合成
村山 徹, 林外 茂彦, 荒井 悠二, 山中 一郎, 觸媒 = Catalyst, 52, 6, 405, 407, 2010年09月04日
触媒学会, 日本語

Direct Synthesis of Diphenyl Carbonate by Electrocarbonylation at a Pd2+-supported Anode
Toru Murayama, Yuji Arai, Tomohiko Hayashi, Ichiro Yamanaka, CHEMISTRY LETTERS, 39, 4, 418, 419, 2010年04月
The first electrochemical synthesis of diphenyl carbonate was accomplished using triethylamine/tetrabutylammonium perchlorate/phenol/dichloromethane or sodium phenoxide/phenol/acetonitrile electrolyte at a [PdCl2/activated carbon and vapor grown carbon fiber] anode, 1 atm CO and 25 degrees C. Sodium phenoxide functioned as a promoter, triethylamine, and a supporting electrolyte, tetrabutylammonium perchlorate, for the carbonylation., CHEMICAL SOC JAPAN, 英語

CoPc/CカソードによるCO₂の気相電解
田端恭介, 村山徹, 加藤之貴, 小原徹, 山中一郎, 電気化学会大会講演要旨集, 77th, 2010年

フェノールの電解カルボニル化による炭酸ジフェニル直接合成
林外茂彦, 村山徹, 山中一郎, 電気化学会大会講演要旨集, 77th, 2010年

酸触媒アシル化反応からのピルビン酸エチルからα-アセトキシアクリル酸エチルの合成
中村陽一, 村山徹, 二宮航, 安川隼也, 大谷内健, 定金正洋, 上田渉, 触媒討論会討論会A予稿集, 106th, 2010年

水熱合成法による5,6族元素を用いた多孔性固体酸複合酸化物の合成
村山徹, 陳俊利, 高玉峻介, 泉彰子, 上田渉, 触媒討論会討論会A予稿集, 106th, 2010年

Mo₃VO_x酸化物における細孔構造と選択酸化反応
紺谷岳史, 村山徹, 上田渉, 触媒討論会討論会A予稿集, 106th, 2010年

Mo₃VOx触媒の構造特性および炭化水素選択酸化反応
村山徹, 中谷浩介, 紺谷岳史, 上田渉, 酸化反応討論会講演要旨集, 43rd, 2010年

Mo-V-O系複合金属酸化物触媒を用いたアクロレイン選択酸化反応
中谷 浩介, 村山 徹, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2010, 0, 46, 46, 2010年
当研究室では結晶性Mo-V-O複合金属酸化物の合成に成功し、アクロレインの選択酸化反応触媒として非常に高い活性と選択性を有することを報告してきた。今回，種々の結晶構造を有するMo-V-O酸化物を触媒として用いることにより、構造の担う役割を明らかにすることを目的とした。それに加え、他の金属元素を添加し触媒性能との相関を調べることで、各金属元素の担う役割の解明および触媒性能の改良を検討した。, 公益社団法人 石油学会, 日本語

水熱合成法を用いたメソ孔を有するMo-Nb-O複合酸化物の合成
村山 徹, 高玉 峻介, 泉 彰子, 上田 渉, 石油学会 年会・秋季大会講演要旨集, 2010, 0, 57, 57, 2010年
我々はこれまで水熱合成法による結晶性Mo-V-O複合金属酸化物の合成に成功し、アルコールやアルカンの選択酸化触媒として高い活性を有することを報告してきた。今回，水熱合成法による複合酸化物調製を応用し，MO-Nb-O複合酸化物触媒の合成に展開した．調整した触媒について，詳細にキャラクタリゼーションを行った結果，MoNbOxのメソ孔構造は棒状の粒子が不規則に積み重なり形成されていることが示唆された．, 公益社団法人 石油学会, 日本語

CoN_2C_x/炭素電極による中性H_2O_2水の触媒的合成
山中 一郎, 田澤 慧, 村山 徹, 竹中 壮, 觸媒 = Catalyst, 51, 6, 420, 422, 2009年09月10日
触媒学会, 日本語

熱処理活性化Co-TPP/GCF電極触媒による高濃度中性H_2O_2水の直接合成
山中 一郎, 田澤 慧, 村山 徹, 市橋 亮, 花泉 紀子, 觸媒 = Catalyst, 51, 2, 96, 98, 2009年03月10日
触媒学会, 日本語

Pdアノード上での電解酸化カルボニル化によるDPCの直接合成-アルキルアミン添加効果-
村山徹, 荒井悠二, 山中一郎, 触媒討論会討論会A予稿集, 104th, 2009年

Pdアノード上での電解カルボニル化反応によるDPCの直接合成-ナトリウムフェノキシド添加効果-
林外茂彦, 村山徹, 荒井悠二, 山中一郎, 触媒討論会討論会A予稿集, 104th, 2009年

熱処理活性化Co(NO₃)₂(phen)/XC72電極による触媒的中性H₂O₂合成
岩崎達也, 田澤慧, 村山徹, 山中一郎, 触媒討論会討論会A予稿集, 104th, 2009年

燃料電池反応法を用いた中性H₂O₂水の合成
田澤慧, 村山徹, 市橋亮, 山中一郎, 電気化学会大会講演要旨集, 75th, 2008年

SPE電解法を利用したCO₂還元反応
古澤崇, 村山徹, 山中一郎, 触媒討論会討論会A予稿集, 102nd, 2008年

膜触媒を用いたO₂とH₂からのH₂O₂の直接合成
平木大介, 田澤慧, 村山徹, 山中一郎, 触媒討論会討論会A予稿集, 102nd, 2008年

水と空気の電気分解による中性過酸化水素水の一段合成
村山 徹, 山中 一郎, 触媒 = Catalysts & Catalysis, 49, 6, 453, 455, 2007年09月05日
触媒学会, 日本語

中性過酸化水素の電解合成 (3)
村山徹, 山田淳, 井関正博, 山中一郎, 触媒討論会討論会A予稿集, 99th, 2007年

燃料電池反応法を用いた中性H₂O₂水の合成
田澤慧, 村山徹, 市橋亮, 山中一郎, 触媒討論会討論会A予稿集, 100th, 2007年

中性H2O2水の電解合成
村山 徹, 山中 一郎, 化学工学会 研究発表講演要旨集, 2007, 0, 742, 742, 2007年
公益社団法人 化学工学会, 日本語

中性過酸化水素水の電解合成
村山徹, 山中一郎, 山田淳, 井関正博, 触媒討論会討論会A予稿集, 98th, 2006年

固体高分子電解質膜を用いた中性過酸化水素水の電解合成
村山徹, 山中一郎, 触媒討論会討論会A予稿集, 96th, 2005年

2020年04月 - 現在
日本化学会　　　　　　　　　　　　　　　

カチオン欠陥サイトを導入した酸化物担体へのAuシングルアトム調製と触媒反応
科学研究費助成事業
2024年02月28日 - 2027年03月31日
村山 徹
日本学術振興会, 基盤研究(B), 東京都立大学, 23K26456

原子間力顕微鏡によるナノ構造体を担持した金属酸化物表面の電荷状態と触媒反応の解明
科学研究費助成事業
2022年04月01日 - 2025年03月31日
李 艶君, 菅原 康弘, 村山 徹
日本学術振興会, 基盤研究(A), 大阪大学, 22H00282

水熱合成による４，５，６族を用いた固体酸複合酸化物の合成
科学研究費助成事業
2012年04月01日 - 2015年03月31日
村山 徹
４，５，６族の遷移金属元素（Ti,Zr,V,Nb,Ta,Mo,W）を用いて，水熱合成法によりオクタヘドラル積層構造を有する多孔性複合酸化物の合成を行った．特にW-M-O（M=Ti，Zr，Nb，Ta）複合酸化物においては，基本的な結晶構造が同じまま元素組成比を変化することができた．この触媒を利用することにより，複合酸化物触媒における構成元素の種類と構成比が触媒活性に与える関係性を明らかにした．この複合酸化物触媒は，多量の水存在下においても固体酸性能を示し，アルコールの脱水反応および水和反応に高い活性を示した．
日本学術振興会, 若手研究(B), 北海道大学, 研究代表者, 競争的資金, 24760635

ユニットネットワーク固体の構築工学展開による新機能触媒物質群形成
科学研究費助成事業
2011年04月01日 - 2014年03月31日
上田 渉, 竹口 竜弥, 清水 研一, 村山 徹, 定金 正洋, 神谷 裕一
ユニットが平面性および球状のポリ酸を合成系中で発生させ、水熱条件下でそれぞれ2次元平面ネットワーク構造、３次元立体ネットワーク構造を構築した。前者は６族、５族、４族のほとんどの元素の組み合わせが可能となり、ナノレベルで5員環状ポリ酸ユニットのネットワーク化を達成し、合成を一般化した。後者の３次元構造形成では、ε型ケギンユニットと金属酸素八面体リンカーが三次元的にネットワーク化した新しいゼオライト様の結晶物質の合成に成功し、構造の確定、対象元素の拡張、ミクロ細孔特性の解析を進めた。二酸化炭素やエタンに対する特異的な親和性を示した。得られた物質の非対称性ミクロ細孔場は新しい触媒機能を示した。
日本学術振興会, 基盤研究(A), 北海道大学, 23246135

窒素化合物変換装置および窒素化合物変換方法
特許権, 村山 徹, 猪俣 雄介, 石田 玉青, 竹歳 絢子, 東京都公立大学法人
特願2020-106393, 2020年06月19日
特開2022-001558, 2022年01月06日
特許第7511877号, 2024年06月28日
202403011202440112

金担持触媒
特許権, 村山 徹, 春田 正毅, 武井 孝, 朱 倩倩, 井上 泰徳, 内田 文生, 前田 憲二, 松尾 寛, 芝崎 靖雄, 東京都公立大学法人, 富士化学株式会社, 芝崎 靖雄
JP2019035138, 2019年09月06日
特許第7457984号, 2024年03月21日
202403003976092980

燃焼システム
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 秦 慎一, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2020009543, 2020年03月05日
特許第7445925号, 2024年02月29日
202403007681453293

脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 秦 慎一, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2020009542, 2020年03月05日
特許第7429012号, 2024年01月30日
202403020958659044

脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 秦 慎一, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2019009201, 2019年03月07日
特許第7388653号, 2023年11月20日
202303019394568820

燃焼システム
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 秦 慎一, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2019009200, 2019年03月07日
特許第7315921号, 2023年07月19日
202303016895506140

燃焼システム
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 秦 慎一, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2019009204, 2019年03月07日
特許第7315922号, 2023年07月19日
202303019149505405

排ガスの脱硝方法
特許権, 清永 英嗣, 吉田 和広, 迫谷 聡介, 盛田 啓一郎, 村山 徹, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2022018036, 2022年04月18日
特許第7278555号, 2023年05月12日
202303002566282176

脱硝触媒及びその製造方法、並びに脱硝方法
特許権, 清永 英嗣, 吉田 和広, 迫谷 聡介, 盛田 啓一郎, 村山 徹, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2022018035, 2022年04月18日
特許第7216975号, 2023年01月25日
202303004051090226

脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 秦 慎一, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2019009199, 2019年03月07日
特許第7209299号, 2023年01月12日
202303017135973918

二酸化炭素還元触媒、及び二酸化炭素還元方法
特許権, 村山 徹, 石田 玉青, 望月 ちひろ, アリ エム. アブデル メイジド, ロルフ ユルゲン ベーム, 中国電力株式会社
JP2021015916, 2021年04月19日
特許第7193037号, 2022年12月12日
202203019967170489

脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 秦 慎一, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2019009203, 2019年03月07日
特許第7193089号, 2022年12月12日
202203001631133180

アミン系化合物の分解方法及びアミン系化合物分解触媒
特許権, 新見 奈央, 直原 洋平, 中山 鶴雄, 村山 徹, 春田 正毅, 武井 孝, 宍戸 哲也, 林 明月, 安 宝祥, 株式会社NBCメッシュテック, 東京都公立大学法人
特願2018-131725, 2018年07月11日
特開2020-006342, 2020年01月16日
特許第7165345号, 2022年10月26日
202203013267229379

ガスセンサ
特許権, 長瀬 徳美, 澁田 夕佳里, 村山 徹, 春田 正毅, 武井 孝, 富士電機株式会社, 東京都公立大学法人
特願2018-188574, 2018年10月03日
特開2020-056726, 2020年04月09日
特許第7158680号, 2022年10月14日
202203016261359873

脱硝触媒及びその製造方法
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2021002436, 2021年01月25日
特許第7050244号, 2022年03月31日
202203005328736730

脱硝触媒成型体及びその製造方法
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2021002437, 2021年01月25日
特許第7050243号, 2022年03月31日
202203015354788271

金複合材料、その製造方法及び金ナノ触媒
特許権, 春田正毅, 村山徹, 吉田拓也, 東京都公立大学法人
JP2017009072, 2017年03月07日
特許第7043072号, 2022年03月18日
202203017231777081

窒素化合物変換装置および窒素化合物変換方法
特許権, 村山 徹, 猪俣 雄介, 石田 玉青, 竹歳 絢子, 東京都公立大学法人
特願2020-106393, 2020年06月19日
特開2022-001558, 2022年01月06日
202203018952471745

脱硝触媒塗布液
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
特願2020-570591, 2020年09月08日
特許第6956988号, 2021年10月08日
202103009857811290

脱硝触媒成型体及び脱硝触媒成型体の製造方法
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
特願2020-570584, 2020年09月08日
特許第6956987号, 2021年10月08日
202103021317327798

正極活物質、リチウムイオン電池用正極及び、リチウムイオン電池
特許権, 村山徹, 石田 玉青, ル-ン スオン ディエン, 春田 正毅, 東京都公立大学法人
特願2019-082603, 2019年04月24日
特開2020-181659, 2020年11月05日
202003015625212953

燃焼システム
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2019004519, 2019年02月07日
WO2020-161875, 2020年08月13日
202103000015406500

燃焼システム
特許権, 清永 英嗣, 吉田 和広, 盛田 啓一郎, 村山 徹, 春田 正毅, 猪股 雄介, 中国電力株式会社, 東京都公立大学法人
JP2019004518, 2019年02月07日
WO2020-161874, 2020年08月13日
202103003547089596

ガスセンサ
特許権, 長瀬 徳美, 澁田 夕佳里, 村山 徹, 春田 正毅, 武井 孝, 富士電機株式会社, 公立大学法人首都大学東京
特願2018-188574, 2018年10月03日
特開2020-056726, 2020年04月09日
202003011106212185

金担持触媒
特許権, 村山 徹, 春田 正毅, 武井 孝, 朱 倩倩, 井上 泰徳, 内田 文生, 前田 憲二, 松尾 寛, 芝崎 靖雄, 東京都公立大学法人, 富士化学株式会社, 芝崎 靖雄
JP2019035138, 2019年09月06日
WO2020-054597, 2020年03月19日
202103017693265119

メタクリル酸製造用触媒及びその製造方法、並びにメタクリル酸の製造方法
特許権, 村山 徹, 張 禎シン, 酒井 秀臣, 福永 誠一郎, 国立大学法人北海道大学, 日本化薬株式会社
特願2016-046697, 2016年03月10日
特開2016-168591, 2016年09月23日
特許第6653871号, 2020年01月31日
202003010838468372

アミン系化合物の分解方法及びアミン系化合物分解触媒
特許権, 新見 奈央, 直原 洋平, 中山 鶴雄, 村山 徹, 春田 正毅, 武井 孝, 宍戸 哲也, 林 明月, 安 宝祥, 株式会社NBCメッシュテック, 公立大学法人首都大学東京
特願2018-131725, 2018年07月11日
特開2020-006342, 2020年01月16日
202003009732563351

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特許権, ポール,セバスティアン, デュメニル,フランク, カトリニョク,バンジャマン, アラク マラン,マルシア, 村山 徹, 上田 渉, サントレ ナティオナル ド ラ ルシェルシェ シアンティフィク, ユニヴェルシテ デ シヨンス エ テクノロジー ド リール - リール1, エコール サントラル ド リール, 国立大学法人北海道大学
特願2017-565846, 2015年06月18日
特表2018-519284, 2018年07月19日
特表2018-519284, 2018年07月19日
特許第6602401号, 2019年10月18日
201803010399318271

不飽和アルコールから不飽和カルボン酸への酸化触媒としてのモリブデンとバナジウムの混合酸化物の使用
特許権, ポール,セバスティアン, デュメニル,フランク, カトリニョク,バンジャマン, アラク マラン,マルシア, 村山 徹, 上田 渉, サントレ ナティオナル ド ラ ルシェルシェ シアンティフィク, ユニヴェルシテ デ シヨンス エ テクノロジー ド リール - リール1, エコール サントラル ド リール, 国立大学法人北海道大学
特願2017-565846, 2015年06月18日
特許第6602401号, 2019年10月18日
201903002003178850

触媒反応装置
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 吉河 敏和, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
特願2018-533707, 2017年03月07日
特許第6558560号, 2019年07月26日
201903015177919004

脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
特願2018-533851, 2017年03月07日
特許第6489597号, 2019年03月08日
201903004551325294

脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
特願2018-533706, 2017年03月07日
特許第6489596号, 2019年03月08日
201903017904205870

脱硝触媒を用いる排ガス浄化方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 吉河 敏和, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
特願2018-533852, 2017年03月07日
特許第6489598号, 2019年03月08日
201903019634020530

船舶用燃焼システム
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 中村 明博, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2017009050, 2017年03月07日
WO2018-047383, 2018年03月15日
WO2018-047383, 2018年03月15日
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脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2016076870, 2016年09月12日
WO2018-047356, 2018年03月15日
WO2018-047356, 2018年03月15日
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脱硝触媒の再生方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 吉河 敏和, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2017009047, 2017年03月07日
WO2018-047380, 2018年03月15日
201803002655919854

脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2017009046, 2017年03月07日
WO2018-047379, 2018年03月15日
201803008005680634

燃焼システム
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2017009049, 2017年03月07日
WO2018-047382, 2018年03月15日
201803020576354688

脱硝触媒の再生方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 吉河 敏和, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2017009048, 2017年03月07日
WO2018-047381, 2018年03月15日
201803006540092137

燃焼システム
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2017009044, 2017年03月07日
WO2018-047377, 2018年03月15日
201803010818481919

イソブチレンの製造方法
特許権, 上田 渉, 村山 徹, 大谷内 健, 二宮 航, 安川 隼也, 国立大学法人北海道大学, 三菱ケミカル株式会社
特願2014-536870, 2013年09月18日
特許第6300726号, 2018年03月09日
2018年03月09日
201803007068046572

金複合材料、その製造方法及び金ナノ触媒
特許権, 春田正毅, 村山徹, 吉田拓也, 公立大学法人首都大学東京
JP2017009072, 2017年03月07日
WO2017-154927, 2017年09月14日
201903009968215302

火力発電システム
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2015075515, 2015年09月08日
WO2017-042895, 2017年03月16日
WO2017-042895, 2017年03月16日
201703001245699578

排ガス浄化方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
JP2015075516, 2015年09月08日
WO2017-042896, 2017年03月16日
WO2017-042896, 2017年03月16日
201703006707793054

脱硝触媒、及びその製造方法
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
特願2016-560930, 2016年09月12日
WO2018-047378, 2018年03月15日
特許第6093101号, 2017年02月17日
2017年02月17日
201703009719744686

火力発電システム
特許権, 清永 英嗣, 引野 健治, 盛田 啓一郎, 春田 正毅, 村山 徹, 美濃 真, 中国電力株式会社, 公立大学法人首都大学東京
特願2016-550662, 2015年09月08日
特許第6077190号, 2017年01月20日
2017年01月20日
201703009567886803

メタクリル酸製造用触媒及びその製造方法、並びにメタクリル酸の製造方法
特許権, 村山 徹, 張 禎シン, 酒井 秀臣, 福永 誠一郎, 国立大学法人北海道大学, 日本化薬株式会社
特願2016-046697, 2016年03月10日
特開2016-168591, 2016年09月23日
201603002825276886

イソブチレン製造用触媒、および、それを用いたイソブチレンの製造方法
特許権, 上田 渉, 村山 徹, 大谷内 健, 二宮 航, 安川 隼也, 国立大学法人北海道大学, 三菱レイヨン株式会社
JP2013075130, 2013年09月18日
WO2014-046118, 2014年03月27日
WO2014-046118, 2014年03月27日
201603021121385080