Researcher Profile and Settings

Master

Affiliation (Master)

• Faculty of Engineering　Applied Chemistry　Chemical Engineering

Affiliation (Master)

• Faculty of Engineering　Applied Chemistry　Chemical Engineering

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Profile and Settings

Affiliation

• Yonsei University, Department of Chemical and Biomolecular Engineering, Adjunct Professor (1/1/2013-12/31/2013)

Degree

• Ph.D. in Chemical Engineering (Advisor, Distinguished Professor Bruce C. Gates)（University of California, Davis）

Profile and Settings

• Name (Japanese)

  OGINO

• Name (Kana)

  Isao

• Name

  201301009973830684

Alternate Names

https://pubs.rsc.org/en/content/ebook/978-1-78801-454-0

Affiliation

• Yonsei University, Department of Chemical and Biomolecular Engineering, Adjunct Professor (1/1/2013-12/31/2013)

Achievement

Research Interests

• Reaction kinetics   Supported catalysts   Microwave   Zeolites   Carbon catalysts   

Research Areas

• Manufacturing technology (mechanical, electrical/electronic, chemical engineering) / Transfer phenomena and unit operations
• Manufacturing technology (mechanical, electrical/electronic, chemical engineering) / Catalytic processes and resource chemistry
• Manufacturing technology (mechanical, electrical/electronic, chemical engineering) / Chemical reaction and process system engineering

Research Experience

• 2011 北海道大学 工学(系)研究科(研究院) 准教授

Published Papers

• Benefits of Using Rapid Microwave Heating in the Synthesis of Metal-Free Carbon Electrocatalysts

  Kodai Satoh, Takumi Odawara, Yusaku Yamazaki, Takatoshi Murakami, Hironobu Ono, Shinichiroh Iwamura, Shin R. Mukai, Isao Ogino

  Industrial and Engineering Chemistry Research 63 (11) 4825 - 4837 0888-5885 2024/03/07
• Cover Feature: Enhanced Dry Reforming of Methane Catalysis by Ni at Heterointerfaces between Thin MgAlO_x and Bulk ZrO₂ (ChemCatChem 19/2023)

  Jin Wang, Gbolade O. Kayode, Yuki Hirayama, Dina Shpasser, Isao Ogino, Matthew M. Montemore, Oz M. Gazit

  ChemCatChem 15 (19) 1867-3880 2023/09/18
• Enhanced Dry Reforming of Methane Catalysis by Ni at Heterointerfaces between Thin MgAlO_x and Bulk ZrO₂

  Jin Wang, Gbolade O. Kayode, Yuki Hirayama, Dina Shpasser, Isao Ogino, Matthew M. Montemore, Oz M. Gazit

  ChemCatChem 15 (19) 1867-3880 2023/08/21 

  Abstract The catalytic performance of supported metals is greatly influenced by the interaction with the support material. The role of the support becomes even more important when dealing with metal nanoparticles and high reaction temperatures. Herein, we show that interfacial sites between two metal oxides, MgAlO_x and ZrO₂ can bestow high stability as well as enhanced reactivity to nickel (Ni) nanoparticles. We use the MgAlO_x as thin oxides on an underlying bulk ZrO₂. We demonstrate the effect of the metal‐support interactions (MSI) in different support locations on the performance in dry reforming of methane (DRM). We find that the rate of DRM catalysis produces a concave‐down trend with respect to Ni loading with a maximum at ~0.8–1.1 % wt Ni. Measuring the Ni2p_3/2 binding energy (BE), we find a similar concave‐down trend whereas for the Mg2p BE we find a concave‐up trend with respect to the Ni loading both with the maximum and minimum centered at 0.8–1.1 % wt Ni, respectively. These trends were correlated with the stability of Ni calculated by DFT. Overall, our results suggest that heterointerfacial sites can be used to tailor moderate MSI, which can be used in the design of DRM catalyst with significantly increased activity and high stability.
• Enhancing the efficiency of gas-liquid-solid reactions using a monolithic microhoneycomb catalyst

  Hiroyuki Mega, Shunpei Takahashi, Takuya Aihara, Seiichiro Yoshida, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  Catalysis Today 407 244 - 251 0920-5861 2023/01
• Solution-mediated transformation of natural zeolite to ANA and CAN topological structures with altered active sites for ethanol conversion

  Mutjalin Limlamthong, Minseong Lee, Bunjerd Jongsomjit, Isao Ogino, Shusheng Pang, Jungkyu Choi, Alex C.K.Yip

  Advanced Powder Technology Elsevier BV 0921-8831 2021/09 [Refereed][Not invited]
  
• Mo–V–O Nanocrystals Synthesized in the Confined Space of a Mesoporous Carbon

  Ryo Obunai, Keisuke Tamura, Isao Ogino, Shin R. Mukai, Wataru Ueda

  Applied Catalysis A: General Elsevier BV 624 118294 - 118294 0926-860X 2021/08/25 [Refereed][Not invited]
  
• Size-activity threshold of titanium dioxide-supported Cu cluster in CO oxidation

  Wasim Ullah Khan, Iris K.M. Yu, Yuqing Sun, Matthew I.J. Polson, Vladimir Golovko, Frank L.Y. Lam, Isao Ogino, Daniel C.W. Tsang, Alex C.K. Yip

  Environmental Pollution Elsevier BV 279 (15) 116899 - 116899 0269-7491 2021/06 [Refereed][Not invited]
  
• Conversion of Carbohydrates to High Value Products

  Isao Ogino

  Heterogeneous Catalysts 617 - 632 2021/03/22 [Refereed]
  
• Genesis of Micropores by Thermal Activation of Mg-Al Layered Double Hydroxides Possessing Interlayer Organic Sulfonates under Oxygen-free Environments

  Isao Ogino, Rei Tanaka, Shin R. Mukai

  Catalysis Today Elsevier 356 (1) 11 - 17 0920-5861 2020/10 [Refereed][Not invited]
  
• Bruce Gates: A Career in Catalysis

  Cawas Cooper, Kerry M. Dooley, Juan C. Fierro-Gonzalez, Javier Guzman, Rolf Jentoft, H. Henry Lamb, Isao Ogino, Ron C. Runnebaum, Ajit Sapre, Alper Uzun

  ACS Catalysis American Chemical Society (ACS) 11912 - 11935 2155-5435 2020/09/10 [Refereed][Invited]
   

  On the occasion of his 80th birthday, we take stock of the remarkable and ongoing career of Professor Bruce C. Gates. This Account highlights his key scientific achievements in three areas of significance: supported metal clusters and atomically dispersed metal complexes, hydroprocessing reaction networks and catalysts, and strong acid catalysis. His contributions in all three areas are noteworthy and have been sustained over 50 years. The work of his group evolved from mainly catalyst synthesis and reaction studies to also incorporate sophisticated characterization techniques based on X-ray absorption spectroscopies and improved scanning transmission electron microscopic examination of catalytic surfaces. In the course of this work, he has addressed, and contributed to the solutions of some of the most significant and challenging problems in catalysis of the last half century.
• Intercalation Chemistry and Thermal Characteristics of Layered Double Hydroxides Possessing Organic Phosphonates and Sulfonates (selected as inside front cover)

  Isao Ogino, Yuki Hirayama, Shin R. Mukai

  New Journal of Chemistry Royal Society of Chemistry 44 (24) 10002 - 10010 1144-0546 2020/06/28 [Refereed][Not invited]
   

  The distinct roles of organic sulfonates that enable delamination in water and formation of microporous structures via thermal activation are elucidated.

• Efficient microwave-assisted annealing of reduced graphene oxides in an up-flow reactor

  Konosuke Minakami, Isao Ogino, Shinichiro Iwamura, Hironobu Ono, Shin R. Mukai

  AIChE Annual Meeting, Conference Proceedings 2020-November 2020
• Understanding Atomically Dispersed Supported Metal Catalysts: Structure and Performance of Active Sites (in SPR Catalysis Volume 31)

  Isao Ogino, edited by James Spivey, Yi-Fan Han, Dushyant Shekhawat

  The Royal Society of Chemistry 31 166 - 197 2019/02 [Refereed][Invited]
   

  Catalysts are required for a variety of applications and industrialists and academics are increasingly challenged to find cost effective and environmentally benign catalysts to use. This volume looks at modern approaches to catalysis and reviews the extensive literature including direct methane conversion, nanocomposite catalysts for transformation of biofuels into syngas and hydrogen and catalytic wet air oxidation technology for industrial wastewater treatment.
• Continuous-flow Separation of Cesium Ion by Ammonium Molybdophosphate Immobilized in a Silica

  Seiichiro Yoshida, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  Adsorption 25 (6) 1089 - 1098 0929-5607 2019 [Refereed][Not invited]
   

  Monolithic cesium ion (Cs+) adsorbents were synthesized via the directional freezing of a silica hydrogel containing ammonium molybdophosphate (AMP) particles, followed by freeze-drying. The adsorbents have a honeycomb-like structure with nearly straight microchannels (approximately 21 mu m in diameter) running through them and with AMP particles partially embedded intact within the channel walls. Because of its honeycomb-like structure, the adsorbent, denoted as AMP silica microhoneycomb (AMP-SMH), achieves a significantly lower pressure drop than a typical column packed with spherical particles with similar diffusion path lengths for Cs+ when water was passed through it (about 35-times lower). Comparison of breakthrough curves between the AMP-SMH and columns packed with particles by numerical simulation also indicates that AMP-SMH shows shorter length of unused bed values. These results demonstrate that the AMP-SMH shows a high performance in the continuous separation of Cs+ due to their unique microhoneycomb structure.
• Catalytic Activity for Oxygen Reduction Reaction of Ni-Mn-Fe Layered Double Hydroxide-Carbon Gel Composite

  Yu Iwai, Takuya Ikka, Akira Miura, NC Rosero-Navarro, Shinichiroh Iwamura, Isao Ogino, Shin R Mukai, Kiyoharu Tadanaga

  Chemistry Letters 48 (7) 696 - 699 0366-7022 2019 [Refereed][Not invited]
  
• Carbon Gel Monoliths with Introduced Straight Microchannels for Phenol Adsorption

  Kazuya Takahashi, Seiichiro Yoshida, Kasama Urkasame, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  Adsorption 25 (6) 1241 - 1249 0929-5607 2019 [Refereed][Not invited]
   

  Adsorption of phenol using carbon adsorbents in the form of a packed bed of particles inherently suffers from the incompatibility between low hydraulic resistance and short diffusion path length. In this work, carbon gel monoliths made from resorcinol-formaldehyde gels with introduced straight microchannels in the range of 60-160 mu m were successfully synthesized using polyesters fibers as templates. The advantage of this synthesis method is that both channel size and channel density can be tuned independently. Introduced microchannels were effective in minimizing the pressure drop of a fluid flowing through the sample to less than a hundredth of beds packed with particles having the same diffusion path length. Synthesized monoliths also possess sufficient mechanical strength (more than 12 kg per monolith) to be activated to increase their adsorption capacity. Adsorption experiments of phenol in a continuous flow system show that synthesized monoliths can be used as effective adsorbents for phenol removal. The tunable channel size and channel density of the proposed synthesis method has the potential for the synthesis of monoliths which could be used to fulfill various process demands.
• Synthesis of Mg–Al Mixed Oxides with Markedly High Surface Areas from Layered Double Hydroxides with Organic Sulfonates

  Rei Tanaka, Isao Ogino, Shin R. Mukai

  ACS Omega 3 (12) 16916 - 16923 2018/12 [Refereed][Invited]
  
• Development of TiO2-SiO2 Photocatalysts Having a Microhoneycomb Structure by the Ice Templating Method.

  Kasama Urkasame, Seiichiro Yoshida, Taihei Takanohashi, Shinichiroh Iwamura, Isao Ogino, Shin R Mukai

  ACS omega 3 (10) 14274 - 14279 2018/10/31 [Refereed][Not invited]
   

  Immobilization of TiO2-based photocatalysts usually suffers from lowered surface area and mass transfer limitation compared with their suspended counterpart. In this work, TiO2-SiO2 monolithic photocatalysts having straight macropores, called microhoneycombs, were synthesized. The obtained samples had straight macropores with a diameter in the range of 15-40 μm formed by walls having a thickness up to 5 μm. The samples also contain micropores and small mesopores inside their walls, which contribute to high surface areas of more than 500 m2 g-1. Synthesized photocatalysts were tested in a continuous flow system using the decolorization of methylene blue as a model reaction. It was found that the unique morphology of the samples can be used to promote the uniform distribution of the target fluid while reducing the pressure drop across the photocatalyst to less than a hundredth compared with a packed bed system. In addition, calcination at 600-800 °C improved the strength and photocatalytic activity of the monoliths while preserving the high surface area of the samples.
• Esterification of levulinic acid with ethanol catalyzed by sulfonated carbon catalysts: Promotional effects of additional functional groups

  Isao Ogino, Yukei Suzuki, Shin R. Mukai

  Catalysis Today 314 (15) 62 - 69 0920-5861 2018/09/15 [Refereed][Not invited]
   

  Analysis of literature data on acid-catalyzed esterification reaction of levulinic acid (LA) with ethanol (EtOH) has suggested that some sulfonated carbon catalysts exhibit higher active-site performance than other solid acid catalysts such as macroreticular resins bearing sulfonic acid groups, zeolites, mesoporous silica functionalized with alkyl- and arene-sulfonic acid groups. To elucidate factors that enable the higher performance of sulfonated carbon catalysts, a series of sulfonated carbon catalysts was synthesized by sulfonating various carbon materials whose concentrations of surface oxygen-containing functional groups, porous structure, and swelling ability differ significantly. The catalysts were tested not only in the liquid-phase esterification reaction of LA with EtOH but also in the reaction of acetic acid (AcA) with EtOH because the latter reaction serves as a test reaction to probe the performance of –SO3H sites with minimal influence by mass transfer limitation and to provide an insight into a role of γ-keto group of LA in catalysis. The results show that all catalysts exhibit nearly the same turnover frequency per –SO3H site in the esterification reaction of AcA with EtOH despite widely different structural properties. In contrast, the data indicate that neighboring functional groups such as –COOH and –OH facilitate the reaction of LA with EtOH presumably through hydrogen-bonding interaction between these surface functional groups and γ-keto group of LA. These results suggest a general design strategy to improve the performance of solid acid catalysts further by precisely tuning the distance between –SO3H sites and neighboring functional groups.
• The Critical Role of Bulk Density of Graphene Oxide in Tuning its Defect Concentration through Microwave-driven Annealing (invited)

  Isao Ogino, Go Fukazawa, Shunsuke Kamatari, Shinichiroh Iwamura, Shin R. Mukai

  Journal of Energy Chemistry 27 (5) 1468 - 1474 2095-4956 2018/09 [Refereed][Invited]
  
• The impact of thermal activation conditions on physicochemical properties of nanosheet-derived Mg-Al mixed oxides

  Isao Ogino, Rei Tanaka, Shuichiroh Kudo, Shin R. Mukai

  Microporous and Mesoporous Materials 263 181 - 189 1387-1811 2018/06/01 [Refereed][Not invited]
   

  Mg-Al mixed oxides with highly accessible basic sites were synthesized from Mg-Al layered double hydroxides bearing interlayer isethionates (Ise). Anion-exchange of interlayer carbonates in synthetic hydrotalcites with Ise induces stacking disorders in layered structure, and subsequent delamination in water followed by drying causes further disordering as characterized by X-ray diffraction technique. However, thermal activation of these materials in air formed Mg-Al mixed oxides with low surface area and low CO2 adsorption capacity. In contrast, thermal activation in N2 or N2 followed by air formed materials exhibiting marked increases in CO2 adsorption capacity up to ∼800% relative to those obtained by thermal activation in air. Thermogravimetric and elemental analyses and IR spectroscopy characterization indicate that thermal activation in N2 enables removal of sulfur species formed from Ise at ∼400 °C, and limits the formation of sulfate species that bridge nanosheets and cause irreversible stacking of them. The proper thermal activation procedure in addition to disordered structure of aggregates of Mg-Al double hydroxide nanosheets enabled the formation of Mg-Al mixed oxides with higher surface area and larger micropore volume than those obtained from the initial hydrotalcites. These results highlight the critical importance of thermal activation steps for such materials, and demonstrate a prospective route to synthesize new porous materials based on Mg-Al mixed oxides.
• Effects of thermal activation conditions on physicochemical properties of nanosheet-derived Mg-AI mixed oxides

  I. Ogino, R. Tanaka, S. R. Mukai

  2nd Natural Gas Utilization Workshop 2018 26  2018
• グラフェン系材料の欠陥低減による耐酸化性と電気伝導性の向上

  荻野勲, 深澤剛, 鎌足俊輔, 岩村振一郎, 向井紳

  月刊Material Stage 17 (12) 1346-3926 2018
• Carbon paper with a high surface area prepared from carbon nanofibers obtained through the liquid pulse injection technique

  Kazuki Sakai, Shinichiroh Iwamura, Ryo Sumida, Isao Ogino, Shin R Mukai

  ACS Omega 3 (1) 691 - 697 2470-1343 2018 [Refereed][Not invited]
   

  To improve the performance of carbon paper used for applications such as electrodes for electrochemical devices and air filters, two types of long carbon nanofibers (CNFs) with average diameters of 20 and 49 nm were prepared by the liquid pulse injection (LPI) technique by adjusting reaction conditions. Carbon paper was made from the CNFs through a simple filtration process. The paper prepared from the CNFs with an average diameter of 20 nm (LPI-CNF(20) paper) was firm and flexible even though it was prepared without using any binders. LPI-CNF(20) paper also had a high surface area and showed a high electrical conductivity and a moderate gas permeability according to its void size. These properties are required for cathodes in the latest battery systems such as lithium−air batteries. In electrochemical experiments conducted to evaluate the performance of LPI-CNF(20) paper as a cathode, the paper showed a larger discharge capacity on the basis of the cathode weight than a conventional cathode (a commercially available carbon paper combined with a porous carbon), which indicated that it has a high potential to be used as a cathode in lithium−air batteries.
• Cost-effective synthesis of activated carbons with high surface areas for electrodes of non-aqueous electric double layer capacitors

  Takeshi Mori, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  Separation and Purification Technology 214 174 - 180 1873-3794 2018 [Refereed][Not invited]
   

  Activated carbons for electrodes of non-aqueous electric double layer capacitors were prepared from composites of poly(methymethacrylate) particles and phenolic resins. Their surface areas can be increased up to 3000 m2 g−1 through simple CO2 activation. Through the characterization of pore properties of the resulting carbons, it was found that the activation process appears to be composed of two steps. The pore properties of the activated carbons were optimized to maximize their performances as electrodes for non-aqueous electric double layer capacitor electrodes.
• Optimization of practical activation depth for effective CO2 activation using PMMA-templated carbons with a tailorable pore system of meso- and macropores

  Takeshi Mori, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  JOURNAL OF POROUS MATERIALS 24 (6) 1497 - 1506 1380-2224 2017/12 [Refereed][Not invited]
   

  For the preparation of physically-activated carbons with ultra-high surface areas that are comparable to those of chemically-activated carbons, we synthesized meso-, macroporous carbons from phenolic resins using poly(methylmethacrylate) particles as a template and activated them using CO2. Our aim was to achieve uniform activation by reducing the practical depth within the carbon which needs to be activated. Our results show that the shorter the practical depth becomes, the higher the achievable BET surface area becomes. Extremely high BET surface areas (similar to 3000 m(2) g(-1)) can be attained by reducing this depth to the order of a few tens of nanometers. We also relate the practical length of the developed nanopores with the practical depth through the results obtained from EDLC measurements. The results reveal that the shortening of the practical activation depth also leads to the shortening of the lengths of the nanopores introduced during activation.
• X-ray absorption spectroscopy for single -atom catalysts: Critical importance and persistent challenges

  Isao Ogino

  CHINESE JOURNAL OF CATALYSIS 38 (9) 1481 - 1488 0253-9837 2017/09 [Refereed][Invited]
  
• Supported Catalysts (in Handbook of Solid State Chemistry) (invited)

  Isao Ogino, Pedro Serna, Bruce C. Gates, edited, by, R. Dronskowski, S. Kikkawa, A. Stein

  Wiley-VCH 313 - 337 2017/08 [Refereed][Invited]
   

  Catalysts make chemical reactions go faster, often by many orders of magnitude in comparison with purely thermal processes. The dominant technological catalysts are solids, which offer the important practical benefit of being readily separated from fluid‐phase products. Solid catalysts are usually porous, having high internal surface areas and therefore high numbers of catalytically active species per unit of reactor volume to facilitate high rates of catalytic reaction. The preparation of common supported catalysts involves support synthesis, deposition of catalyst precursor components, and treatment to convert the supported species into catalytically active species. Industrial catalysts are also subjected to additional processing to control the sizes and shapes of the final product. The effect of the structure of a crystal face on catalysis is typically diagnosed in experiments with single crystals exposing various faces and often rationalized on the basis of relationships between the crystallographic orientations and the adsorbate‐adsorbent (reactant‐catalyst) binding energies.
• PMMA-Templated Carbon Gel Monoliths with Independently Tunable Micro-, Meso-, and Macropores

  Takeshi Mori, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  JOURNAL OF CHEMICAL ENGINEERING OF JAPAN 50 (4) 315 - 323 0021-9592 2017/04 [Refereed][Not invited]
   

  Independent controlling of micro-(< 2 nm), meso-(2-50 nm) and macropore (> 50 nm) structures in monolithic carbon gels (CGs) was achieved by simply adjusting three independent synthetic parameters. Monolithic composites of resorcinol- formaldehyde (RF) gel and poly(methylmethacrylate) (PMMA) particles were prepared and subsequently carbonized yielding carbonized monoliths. Macropores were successfully introduced as traces of the PMMA particles without hardly affecting the structures of the micro-and mesopores of CGs. The size of the macropores can be controlled in the range of 0.05-1.0 mu m by adjusting the size of the PMMA particles. The size of the mesopores can also be controlled in the range of a few to a few tens of nanometers by adjusting the concentration of the catalyst in the starting RF solution. Micropores can be efficiently developed by activating the CG monoliths with CO2 gas yielding monoliths having extremely high BET surface areas up to similar to 3000 m(2) g(-1).
• CO2 Separation in a Flow System by Silica Microhoneycombs Loaded with an Ionic Liquid Prepared by the Ice-Templating Method

  Seiichiro Yoshida, Kazuya Takahashi, Shuichiro Kudo, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 56 (10) 2834 - 2839 0888-5885 2017/03 [Refereed][Not invited]
   

  Silica microhoneycombs (SMHs) loaded with an ionic liquid (IL) (IL-SMHs) were successfully synthesized by impregnating SMHs with an IL bearing an amino group, trihexyl(tetradecyl)-phosphonium alanate ([P-66614][Ala]). SMHs can incorporate at least 50 wt % [P-66614] [Ala] without its straight channels being clogged as demonstrated by a low pressure drop when He was passed through the material. The IL-SMH containing 50 wt % [P-66614] [Ala] shows a CO2 capacity of similar to 0.26 mmol-CO2.g(-1) in a CO2 33%-N-2 67% atmosphere at 303 K IL-SMHs can be readily regenerated by heating them at 393 K and can be reused at least three times without losing the CO2 absorption ability. IL-SMH can also effectively separate CO2 in a flow system. The length of unused bed was very short (only 19 mm). These results demonstrate the high potential of IL-SMHs to be used for effective CO2 separation in flow systems.
• Adsorption of phenol in flow systems by a monolithic carbon cryogel with a microhoneycomb structure

  Seiichiro Yoshida, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY 22 (8) 1051 - 1058 0929-5607 2016/11 [Refereed][Not invited]
   

  Adsorption of phenol from an aqueous solution in batch and continuous flow systems using carbon gels with a microhoneycomb structure (carbon gel microhoneycombs, CMHs) was studied. The obtained monolithic CMHs had fairly straight channels, 25-45 mu m in diameter, and the thickness of the walls which form the channels was around 5 mu m. The CMHs showed 370 times lower hydraulic resistance when compared with a column packed with particles having the same diffusion path length as it. The obtained CMHs have a hierarchical micro-meso porous structure giving BET surface area in the range of 513-1070 m(2)center dot g(-1).When used for phenol adsorption from an aqueous solution, the CMHs quickly adsorbed phenol at first, and then, the uptake gradually increased, which indicates that the adsorption mechanism is based on not only simple physisorption. The phenol adsorption capacity increased with the increase in carbonization temperature of the CMH and the decrease in its hydrophilicity. CMHs carbonized at temperatures higher than 1073 K showed the highest phenol adsorption capacity which was around 160 mg center dot g(-1). The CMHs could continuously adsorb phenol from aqueous solutions, and their length of unused bed (LUB) values depended on operation conditions but were in the range of 0.3-0.7 cm. The experimental results indicated that carbon cryogels with a microhoneycomb structure have a high potential to be used for effective separation of phenol.
• New method for introducing mesopores into carbon microhoneycombs using dextran

  Shinichiroh Iwamura, Kohei Kitano, Isao Ogino, Shin R. Mukai

  MICROPOROUS AND MESOPOROUS MATERIALS 231 171 - 177 1387-1811 2016/09 [Refereed][Not invited]
   

  Carbon microhoneycombs (CMHs), which can be prepared from a resorcinol formaldehyde (RF) hydrogel using ice crystals as a template, are attractive materials for industrial applications such as solid catalysts and adsorbents in flow system reactors. For such applications, pores in a material are important for mass transfer, but the mesopore volumes of CMHs are smaller than that of typical RF-derived carbons because ice crystals compress RF gels during freezing, and mesopores partly collapse. The introduction of mesopores into CMHs requires an additional step such as HCl treatment in the preparation process, and this increases the preparation time. In this work, we developed a convenient method for introducing mesopores into CMHs, in which dextran was added to the initial RF solution. This simple step increased the mesopore volume from 0.015 to 0.191 cm(3)/g. We investigated the porous structure of the sample at each step in the preparation, and found that dextran protected the porous structure of the RF hydrogel from growth of ice crystals, enabling mesopore introduction. A combination of dextran addition and HCl treatment further increased the mesopore volume to 0.753 cm3/g; this cannot be achieved using HCl treatment alone. This may be because the HCl solution can diffuse through the mesopores introduced by dextran addition, and this promotes pore formation. (C) 2016 Elsevier Inc. All rights reserved.
• Effect of the mesopores of carbon supports on the CO tolerance of Pt2Ru3 polymer electrolyte fuel cell anode catalyst

  Napan Narischat, Tatsuya Takeguchi, Takeshi Mori, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai, Wataru Ueda

  INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 41 (31) 13697 - 13704 0360-3199 2016/08 [Refereed][Not invited]
   

  To investigate the effects of the porous structure of carbon support for bimetallic PtRu PEFC anode catalysts on their CO tolerance, a series of Resorcinol-formaldehyde carbon gels with different resorcinol to catalyst (R/C) ratios (i.e., 200, 800 and 1000) were synthesized and used to support Pt2Ru3 nanoparticles. Synthesized catalysts were characterized by powder X-ray diffraction, N-2 gas adsorption/desorption experiments, and scanning transmission electron microscopy. CO tolerances were evaluated by using a single cell in a H-2 feed in the presence of CO ranging from 100 to 2000 ppm. The potential difference of the cell using Pt2Ru3/RC1000ac58 anode catalyst was 0.655 V whereas the cell using a commercial Pt2Ru3/C catalyst showed a voltage of 0.570 V in the presence of 500 ppm CO. The results reveal that high modal size and volume of mesopore enhance diffusivity of CO resulted in effectively oxidization of CO. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
• 次世代社会を支えるエネルギー技術 酸化グラフェン由来の多孔質炭素の合成

  荻野勲, 向井紳

  ケミカルエンジニヤリング 61 (5) 0387-1037 2016
• Flexible film-type catalysts encapsulating urease within kappa-carrageenan hydrogel network

  Sohei Yamazaki, Takeshi Mori, Isao Ogino, Shin R. Mukai

  CHEMICAL ENGINEERING JOURNAL 278 (15) 122 - 128 1385-8947 2015/10 [Refereed][Not invited]
   

  Flexible film-type catalysts were synthesized by encapsulating urease within a kappa-carrageenan gel network supported on a cellulose-acetate membrane filter. Synthesized film-type catalysts are flexible and can be easily formed into a shape that is suitable for a specific process configuration. The filter membrane has macropores about 200 nm, which are formed by interconnected bead-shaped membrane material. Scanning electron microscopy shows that the surface of the membrane material is coated homogeneously with the kappa-carrageenan hydrogel. Urease entrapped within the gel network hardly leaches out during urea hydrolysis catalysis conducted at 310 K in a batch reactor and exhibits high catalytic performance. Analysis of the reaction data by the Michaelis-Menten equation shows that the film-type catalyst shows kinetic parameters (K-M and V-max) and apparent activation energy (24 kJ mol(-1)), which are all similar to those found for free urease. Estimation of the mass transfer rate of urea within the kappa-carrageenan network and the urea hydrolysis rate show that the diffusion rate of urea within the thin film is five orders of magnitude higher than the reaction rate. The film catalyst can be recycled at least 7 times with <20% decrease in activity. High flexibility as well as high catalytic performance of the film catalyst shows prospective features of this catalyst for future applications. (C) 2014 Elsevier B.V. All rights reserved.
• Tuning the Pore Structure and Surface Properties of Carbon-Based Acid Catalysts for Liquid-Phase Reactions

  Isao Ogino, Yukei Suzuki, Shin R. Mukai

  ACS CATALYSIS 5 (8) 4951 - 4958 2155-5435 2015/08 [Refereed][Not invited]
   

  A series of sulfonic-acid-containing carbon catalysts were synthesized through the pyrolyzation of resorcinol-formaldehyde resins and subsequent sulfonation to investigate the tunability of their pore structure and surface properties. These catalysts were characterized by nitrogen gas adsorption, water vapor adsorption, elemental analysis, Boehm titration, and IR spectroscopy. Catalytic consequences of these properties were examined using two esterification reactions in which reactants of substantially different sizes (oleic acid vs acetic acid) are involved as well as the condensation of furfural with 2-methylfuran. The esterification of acetic acid with ethanol proceeded at nearly the same activity (TOF similar to 0.02 s(-1)) for all synthesized catalysts regardless of the variation of their surface and pore properties. Poisoning experiments of acid groups in the synthesized catalysts with NaCl indicate that nearly all -SO3H groups are accessible to the reactants. However, the esterification of oleic acid with methanol requires a large volume of mesopores (>0.4 cm(3) g(-1)) to proceed as efficiently as that using p-toluenesuffonic acid (p-TSA) as the catalyst. The condensation reaction requires both hydrophobic surfaces and a large volume of mesopores. A synthesized carbon-based catalyst having a large mesopore volume (1.1 cm(3) g(-1)) and surfaces with a relatively high hydrophobicity catalyzes this reaction at a much higher rate and higher selectivity (>90%) than Amberlyst-15. The results reported here show that the pore structure and surface properties of phenolic-resin-derived carbon catalysts can be easily tuned to maximize their catalytic performance in the reaction for which they are intended.
• Genesis of De laminated-Zeolite Morphology: 3-D Characterization of Changes by STEM Tomography

  Ilke Arslan, John D. Roehling, Isao Ogino, K. Joost Batenburg, Stacey I. Zones, Bruce C. Gates, Alexander Katz

  JOURNAL OF PHYSICAL CHEMISTRY LETTERS 6 (13) 2598 - 2602 1948-7185 2015/07 [Refereed][Not invited]
   

  Zeolite delamination increases the external surface area available for catalyzing the conversion of bulky molecules, but a fundamental understanding of the delamination process remains unknown. Here we report morphological changes accompanying delamination on the length scale of individual zeolite clusters determined by 3-D imaging in scanning transmission electron microscopy. The results are tomograms that demonstrate delamination as it proceeds on the nanoscale through two distinct key steps: a chemical treatment that leads to a swelled material and a subsequent calcination that leads to curling and peeling off of delaminated zeolite sheets over hundreds of nanometers. These results characterize the direct, local, 3-D morphological changes accompanying delaminated materials synthesis and, with corroboration by mercury porosimetry, provide unique insight into the morphology of these materials, which is difficult to obtain with any other technique.
• Sonication-Free Exfoliation of Graphite Oxide via Rapid Phase Change of Water

  Isao Ogino, Yuya Yokoyama, Shin R. Mukai

  TOPICS IN CATALYSIS 58 (7-9) 522 - 528 1022-5528 2015/05 [Refereed][Invited]
   

  Efficacy of a new approach for the synthesis of graphene oxide (GO) nanosheets that has been recently reported (Ogino et al. in Chem Mater 26:3334-3339, 2014) was investigated further using graphite oxides with various degrees of oxidation and average particle sizes. The approach consists of rapid freeze-thaw cycles of water containing graphite oxide, which enables the efficient exfoliation of graphite oxide layers with the minimal fragmentation of GO sheets. The method is effective for the exfoliation of graphite oxides with C/O atomic ratios <= 2.6 as shown by experiments with various degrees of oxidation of graphite oxides. When this method was tested for large particle-size graphite oxide that had been prepared from graphite with the average particle size of 60 mu m, it formed approximately tenfold larger GO sheets than those prepared using sonication. Exfoliation experiments conducted at different freezing rates of water demonstrate that a faster freezing rate of water yielded a higher concentration of a dispersed GO solution. Thus, the results support the hypothesis that rapid phase change enables efficient layer exfoliation.
• Carbon Nanotube Synthesis via the Calciothermic Reduction of Carbon Dioxide with Iron Additives

  Tatsuya Kikuchi, Ryoma Ishida, Shungo Natsui, Takehiko Kumagai, Isao Ogino, Norihito Sakaguchi, Mikito Ueda, Ryosuke O. Suzuki

  ECS SOLID STATE LETTERS 4 (9) M19 - M22 2162-8742 2015 [Refereed][Not invited]
   

  The novel fabrication of multi-walled carbon nanotube (MWCNT)/cementite (Fe3C) nanocomposites was demonstrated via the calciothermic reduction of carbon dioxide (CO2) through electrolysis in molten CaCl2/CaO with iron additives at 1173 K. In this technique, CO2 generated from a graphite anode is reduced to carbon with a metallic calcium reductant formed on a graphite cathode via electrolysis in molten salt. Calciothermic reduction without iron additives resulted in the formation of onion-like carbons (OLCs) with spherical graphite layers and thin graphite sheets. In contrast, MWCNT/Fe3C nanocomposites and OLCs were successfully fabricated via calciothermic reduction with iron additives through their catalytic activities. (C) The Author(s) 2015. Published by ECS. All rights reserved.
• Development of a novel cesium adsorbent which causes minimal hydraulic resistance through the immobilization of Prussian blue analogues in a monolithic silica-alumina microhoneycomb

  Shin R. Mukai, Yoshinao Kimura, Seiichiro Yoshida, Isao Ogino

  Chemical Engineering Transactions 42 181 - 186 2283-9216 2014/12/01 [Refereed][Not invited]
   

  Prussian blue analogues (PBAs) such as K2[CuFe(CN)6] are expected to become the key material for efficient cesium recovery. However to use this material efficiently, it must have a morphology that doesn't cause a severe hydraulic resistance, as a high throughput is required during recovery. This is very difficult, as this material is usually obtained in the form of small particles. In this work, we developed a cesium adsorbent with a low hydraulic resistance using PBAs as the adsorption sites. Silica-alumina was selected as the substrate. As for the morphology of the adsorbent, we adopted a microhoneycomb structure, which can be obtained by the Ice Templating Method, a new micromolding method developed in our laboratory. The obtained adsorbent showed a significantly lower hydraulic resistance than conventional adsorbents in the particle form, and could be used to continuously remove ppm-ordered cesium from solutions.
• Zeolite-supported Molecular Metal Complex Catalysts (in Atomically-Precise Methods for Synthesis of Solid Catalysts)

  Isao Ogino, Sophie Hermans, Thierry Visart, de Bocarme Ed

  The Royal Society of Chemistry 27 - 54 2014/11 [Refereed][Invited]
  
• Effect of Activation Degree of Resorcinol-Formaldehyde Carbon Gels on Carbon monoxide Tolerance of Platinum-Ruthenium Polymer Electrolyte Fuel Cell Anode Catalyst

  Napan Narischat, Tatsuya Takeguchi, Takanori Tsuchiya, Takeshi Mori, Isao Ogino, Shin R. Mukai, Wataru Ueda

  JOURNAL OF PHYSICAL CHEMISTRY C 118 (40) 23003 - 23010 1932-7447 2014/10 [Refereed][Not invited]
   

  Resorcinol-formaldehyde carbon gels (RFCs) show several advantageous properties as a catalyst support over other carbons, as their pore volume and pore size can be readily tailored, for example, via CO2 activation. In this study, RFCs were synthesized with various activation degrees (burn-off) as 0, 37, 58, and 88% and used as the support for a PtRu anode electrode; a commercial Pt2Ru3/C anode catalyst was used as a reference. The catalysts were characterized by powder X-ray diffraction (PXRD), BET surface area, transmission electron microscopy (TEM), and scanning transmission electron microscopy (STEM). The performance and CO tolerance of the obtained catalysts were tested through single cell performance analysis with CO contaminations ranging from 100 to 2000 ppm. The prepared Pt2Ru3/RFC catalysts showed superior CO tolerance. Especially Pt2Ru3/RFC prepared using an RFC with a burn-off of 58% (RC1000Ac58) showed the highest performance and best CO tolerance. The activation degree could affect the volumes and sizes of mesopores and micropores, resulting in differences in size and dispersion of PtRu particles, and accessibility to the particles both of which govern the performance and CO tolerance of the catalysts. Pt2Ru3/RC1000Ac58 showed the highest cell voltage of 0.787 V and highest CO tolerance at 2000 ppm of CO (0.655 V, only 16.8% overvoltage. Supporting PtRu particles by using a carbon support with an optimum activation degree could be a practical method to improve the performance and CO tolerance of a PtRu electrocatalyst.
• Binderfree synthesis of high-surface-area carbon electrodes via CO2 activation of resorcinol-formaldehyde carbon xerogel disks: Analysis of activation process

  Takanori Tsuchiya, Takeshi Mori, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  CARBON 76 240 - 249 0008-6223 2014/09 [Refereed][Not invited]
   

  High-surface-area carbon xerogels were prepared in the form of disks via carbonization of precursor resorcinol-formaldehyde (RP) polymer disks and subsequent activation of the resultant RF carbon xerogels by CO2. RF carbon xerogels allow the preparation of a set of pre-activated carbon disks having different mesopore volumes. Analysis of the relationship between the mesopore volume of the samples and their CO2 activation efficiency showed that the presence of mesopores is crucial for obtaining a high-surface-area carbon with minimal burn-off of carbon atoms. Activation of an RF carbon disk with a mesopore volume of 1.0 cm(3) g(-1) up to a bum-off of 81% yielded an activated carbon disk with a high BET surface area of similar to 3000 m(2) g(-1). Such disks could be readily used as electrode materials for an electric double layer capacitor without filler or binder addition and exhibited competitive EDLC performance against other electrode materials previously reported. (C) 2014 Elsevier Ltd. All rights reserved.
• Exfoliation of Graphite Oxide in Water without Sonication: Bridging Length Scales from Nanosheets to Macroscopic Materials

  Isao Ogino, Yuya Yokoyama, Shinichiro Iwamura, Shin R. Mukai

  CHEMISTRY OF MATERIALS 26 (10) 3334 - 3339 0897-4756 2014/05 [Refereed][Not invited]
   

  Dispersed graphene oxide (GO) nanosheets in water were synthesized via a new approach involving sonication-free exfoliation, as promoted by repetitive simple freeze-thaw cycles. These cycles consist of rapid freezing of an aqueous solution containing graphite oxide and subsequent thawing of the resultant solid. This approach is effective for exfoliation of graphite oxide and yields approximately 80% GO after six repetitive freeze-thaw cycles. The GO synthesized by the new method experiences minimal fragmentation during the exfoliation process and has a lateral size at least 3-fold larger than that of GO prepared by using sonication, as evidenced by atomic force microscopy and dynamic light scattering. We also demonstrate use of the resulting exfoliated GO that is synthesized using this approach as a building block for the synthesis of a low-density (approximate to 0.02 g cm(-3)) macroporous monolithic material, using directional freezing, which forms ice rods within the solution that served as the template to direct the assembly of the solution-dispersed GO nanosheets into a honeycomb-like morphology with a 10 mu m macropore opening and sheet-like walls. Such a unique morphology of the synthesized monolith has broad applicability for advanced functional materials that allow extremely high throughput with minimal pressure drop as well as electronic and energy storage materials.
• Marked Increase in Hydrophobicity of Monolithic Carbon Cryogels via HCI Aging of Precursor Resorcinol-Formaldehyde Hydrogels: Application to 1-Butanol Recovery from Dilute Aqueous Solutions

  Isao Ogino, Sakai Kazuki, Shin R. Mukai

  JOURNAL OF PHYSICAL CHEMISTRY C 118 (13) 6866 - 6872 1932-7447 2014/04 [Refereed][Not invited]
   

  Monolithic carbon cryogels having a honeycomb structure with pore openings a few tens of micrometers in diameter (Carbon Micro Honeycomb, CMH) were synthesized by directional freezing of precursor resorcinol formaldehyde (RF) hydrogels and subsequent carbonization at temperatures >= 674 K. Aging of precursor RF monoliths with 1 N HCl aq. was found to markedly increase the hydrophobicity of the corresponding CMHs as characterized by water vapor adsorption experiments conducted at 298 K. Analysis of the water vapor adsorption data indicates that levels of hydrophobicity of CMHs are similar to those exhibited by other types of highly hydrophobic adsorbents, such as a coal-derived activated carbon and a defect-free pure silica zeolite Beta. HCl aging also drastically changes the porous structure of CMHs from microporous to micro/mesoporous as characterized by nitrogen adsorption/desorption experiments. Because of significantly enhanced hydrophobicity of CMHs as well as hierarchical pore structure (straight macropores connected with micro/mesopores), CMHs can readily separate 1-butanol molecules from a diluted aqueous solution at 310 K and demonstrate high capacities (up to approximate to 3.13 mol kg(-1) at a 1-butanol concentration of 135 mM). The unique morphology of CMHs, consisting of straight macropores coupled with micro/mesopores embedded within honeycomb walls, and the highly hydrophobic surface properties offer future prospects of CMHs in various applications that require fast separation of hydrophobic molecules from a large volume of aqueous solutions.
• Continuous cesium separation using a silica microhoneycomb supporting ammonium molybdophosphate

  Seiichiro Yoshida, Yoshinao Kimura, Isao Ogino, Shin R. Mukai

  Separations Division 2014 - Core Programming Area at the 2014 AIChE Annual Meeting 2 520  2014
• Development of a Novel Cesium Adsorbent which Causes Minimal Hydraulic Resistance through the Immobilization of Prussian Blue Analogues in a Monolithic Silica-Alumina Microhoneycomb

  Shin R. Mukai, Yoshinao Kimura, Seiichiro Yoshida, Isao Ogino

  SDEWES: THE 8TH CONFERENCE ON SUSTAINABLE DEVELOPMENT OF ENERGY, WATER AND ENVIRONMENT SYSTEMS 42 181 - 186 1974-9791 2014 [Refereed][Not invited]
   

  Prussian blue analogues (PBAs) such as K-2[CuFe(CN)(6)] are expected to become the key material for efficient cesium recovery. However to use this material efficiently, it must have a morphology that doesn't cause a severe hydraulic resistance, as a high throughput is required during recovery. This is very difficult, as this material is usually obtained in the form of small particles. In this work, we developed a cesium adsorbent with a low hydraulic resistance using PBAs as the adsorption sites. Silica-alumina was selected as the substrate. As for the morphology of the adsorbent, we adopted a microhoneycomb structure, which can be obtained by the Ice Templating Method, a new micromolding method developed in our laboratory. The obtained adsorbent showed a significantly lower hydraulic resistance than conventional adsorbents in the particle form, and could be used to continuously remove ppm-ordered cesium from solutions.
• Synthesis of Sulfonic Acid Functionalized Silica Honeycombs

  Yoshitaka Satoh, Yuya Yokoyama, Isao Ogino, Shin R. Mukai

  INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 52 (44) 15293 - 15297 0888-5885 2013/11 [Refereed][Not invited]
   

  A honeycomb-type silica monolith was functionalized with sulfonic acid groups to synthesize a solid acid catalyst for flow reaction systems. The sulfonic acid groups were introduced via anchoring of 3-mercaptopropyltrimethoxysilane (MPTS) on the silica surface and subsequent oxidation using a H2O2 solution. The honeycomb-type monolith used as the substrate was prepared using ice crystals as a template and was found to have a high open frontal area of approximate to 85% and flow-through macropores (approximate to 27 mu m in diameter) that are surrounded by silica walls (approximate to 2 mu m in thickness). The catalyst was tested by the liquid phase esterification of ethanol with acetic acid at 333 K in a batch reactor as well as a flow reactor. The catalyst was found to exhibit about 2-fold higher catalytic activity than Amberlyst-15 in a batch reactor. The catalyst also showed a stable catalytic activity for 24 h in a flow reactor.
• Analysis of the Growth Behavior of Carbon Nanofibers Synthesized Using the Liquid Pulse Injection Technique

  Shin R. Mukai, Yuusuke Rikima, Riku Furukawa, Isao Ogino

  INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 52 (44) 15281 - 15286 0888-5885 2013/11 [Refereed][Not invited]
   

  In this work, the growth behavior of carbon nanofibers synthesized using the liquid pulse injection technique was clarified by analyzing samples collected at different growth stages. It was confirmed that, due to the high catalytic activity of the ultrafine metal catalyst particles generated through this technique, the fibers elongate at an extremely high rate during the initial stage of growth, which leads to the high efficiency of carbon nanofiber production. Owing to this high elongation rate, the elongation process and thickening process can be practically considered as two consecutive processes. This allows the modification of the production sequence, resulting in a significant enhancement in production efficiency.
• Synthesis of a Monolithic Carbon-Based Acid Catalyst with a Honeycomb Structure for Flow Reaction Systems

  Kazuhiro Murakami, Yoshitaka Satoh, Isao Ogino, Shin R. Mukai

  INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 52 (44) 15372 - 15376 0888-5885 2013/11 [Refereed][Not invited]
   

  A carbon-based monolithic acid catalyst with a honeycomb structure (CMHC) was synthesized via carbonization of a resorcinol-formaldehyde resin and subsequent sulfonation using sulfuric acid. The CMHC has nearly straight flow-through macropores (e.g., 47-78 mu m) formed by the directional freezing of the resin precursor. These macropores are surrounded by thin carbon walls of approximately 6-mu m thickness that are micro- and mesoporous as characterized by nitrogen adsorption experiments. The straight macropores enable a low hydraulic resistance to a liquid flow as demonstrated by >1000-fold less pressure drops of water flowing through the CMHC than those calculated for a packed bed of spherical particles with the same diameter as the approximate wall thickness of the CMHC. The CMHC shows a stable catalytic activity in the liquid-phase esterification of acetic acid with ethanol at 333 K in a flow reaction system for 50 h of operation. These results show prospective features of the CMHC for applications in flow reaction systems.
• Heteroatom-Tolerant Delamination of Layered Zeolite Precursor Materials

  Isao Ogino, Einar A. Eilertsen, Son-Jong Hwang, Thomas Rea, Dan Xie, Xiaoying Ouyang, Stacey I. Zones, Alexander Katz

  CHEMISTRY OF MATERIALS 25 (9) 1502 - 1509 0897-4756 2013/05 [Refereed][Not invited]
   

  The synthesis of the first delaminated borosilicate layered zeolite precursor is described, along with its aluminosilicate analogue, which consists of Al-containing UCB-3 and B-containing UCB-4 from as-made SSZ-70. In addition, the delamination of PREFER (which is the precursor to ferrierite zeolite) under similar conditions yields delaminated layered zeolite precursors consisting of Al-containing UCB-5 and Ti-containing UCB-6. Multinuclear solid-state NMR spectroscopy (B-11 and Al-27), diffuse-reflectance UV-vis spectroscopy, and heteroatom/Si ratios measured via elemental analysis are consistent with a lack of heteroatom leaching from the framework following delamination. Such mild delamination conditions are achieved by swelling the zeolite precursor in a fluoride/chloride surfactant mixture in DMF solvent, followed by sonication. Powder X-ray diffraction, argon gas physisorption, and chemisorption of bulky base probes strongly suggest delamination, and demonstrate a 1.5-fold increase in the number density of external acid sites and surface area of calcined UCB-3, relative to calcined Al-SSZ-70. The synthesis of microporous pockets in materials UCB-3-UCB-5 suggests the possibility of interlayer porosity in SSZ-70, which is a layered zeolite precursor material whose structure remains currently unknown. The mildness of the delamination method presented here, as well as the lack of need for acidification in the synthesis procedure, enables the delamination of heteroatom-containing zeolites while preserving the framework integrity of labile heteroatoms, which could otherwise be leached under harsher conditions.
• Optimizing the dimensions of magnesium ammonium phosphate to maximize its ammonia uptake ability

  Takanobu Masuda, Isao Ogino, Shin R. Mukai

  ADVANCED POWDER TECHNOLOGY 24 (2) 520 - 524 0921-8831 2013/03 [Refereed][Not invited]
   

  Magnesium ammonium phosphate (MgNH4PO4.6H(2)O:MAP) releases approximately 70% of its ammonia at a mild temperature of 378 K. The resultant material (magnesium hydrogen phosphate (MgHPO4:MHP)-like material), which appears to be an amorphous phase, to remove ammonia from wastewater was investigated. Because the original size of MAP crystals was found to critically affect the kinetics of ammonia uptake by the corresponding MHP-like material, MAP with different sizes were synthesized by changing concentration, pH and temperature of the synthesis solution. The variation in the synthesis concentration was found to change the size of MAP as well as the aspect ratio of the long-axis to the short-axis. The rate of ammonia uptake depends primarily on the dimension of the short-axis of the corresponding MAP crystals. Furthermore, analysis of ammonia uptake using a method similar to the shrinking-core model shows approximately 0.5 mu m from the surface is effectively used for ammonia uptake over a period of a realistic process time. Thus, the results suggest it is crucial to synthesize small MAP crystals with the size of short-axis less than 11 mu m. Our results also show that small MAP crystals can be used at least four times repeatedly for ammonia uptake. (C) 2012 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder Technology Japan. All rights reserved,
• Synthesis of a microhoneycomb-type silica-supported ammonium molybdophosphate for cesium separation

  Seiichiro Yoshida, Yoshinao Kimura, Isao Ogino, Shin R. Mukai

  Journal of Chemical Engineering of Japan 46 (9) 616 - 619 0021-9592 2013 [Refereed][Not invited]
   

  The present study investigates a monolithic silica microhoneycomb including ammonium molybdophosphate (AMPSMH) that was synthesized for cesium separation in a continuous flow system. The honeycomb structure of the AMP-SMH causes significantly less hydraulic resistance to a liquid flow than a conventional bed of particles as demonstrated by pressure-drop measurements using water. AMP particles were dispersed as small particles ≈10 μm in diameter on or within the microchannels of the silica microhoneycomb as characterized by SEM. These AMP particles function as effective sorbents to remove ppm-level cesium ions effectively from a solution, as shown by the breakthrough curve. These data suggest the potential features of the AMP-SMH for processing a large volume of a solution containing radioactive cesium. © 2013 The Society Of Chemical Engineers, Japan.
• Immobilization of magnesium ammonium phosphate crystals within microchannels for efficient ammonia removal

  Takanobu Masuda, Isao Ogino, Shin R. Mukai

  WATER SCIENCE AND TECHNOLOGY 67 (2) 359 - 365 0273-1223 2013 [Refereed][Not invited]
   

  Magnesium ammonium phosphate was formed in flow-through microchannels of silica monoliths using two different methods to fabricate materials that show efficient ammonia adsorption performance from wastewater with low hydraulic resistance. Magnesium ammonium phosphate crystals in these materials release ammonia when heated at 378 K, yielding primarily magnesium hydrogen phosphate. When this material was used for ammonia removal from an aqueous solution containing 100 ppm ammonia in a flow system, the material readily removed ammonia, decreasing the ammonia concentration to 25 ppm. The material can be reactivated by the same procedure and used again for ammonia removal. Hydrodynamic resistance through the lengths of the materials depend on the shape of the immobilized crystals, showing that needle-like crystals are more effective to cause less resistance than plate-like particles. The material containing needle-like crystals causes only approximately one-eighth of the hydraulic resistance that a packed column consisted of spherical particles with a typical bed porosity of 0.5 does. Thus, these results demonstrate the high applicability of the material for ammonia removal from wastewater in a continuous process.
• Nonaqueous Fluoride/Chloride Anion-Promoted Delamination of Layered Zeolite Precursors: Synthesis and Characterization of UCB-2

  Einar A. Eilertsen, Isao Ogino, Son-Jong Hwang, Thomas Rea, Sheila Yeh, Stacey I. Zones, Alexander Katz

  CHEMISTRY OF MATERIALS 23 (24) 5404 - 5408 0897-4756 2011/12 [Refereed][Not invited]
   

  The delamination of layered zeolite precursor PREFER is demonstrated under mild nonaqueous conditions using a mixture of cetyltrimethylammonium bromide, tetrabutylammonium fluoride, and tetrabutylammonium chloride in N,N-dimethylformamide (DMF) as solvent. The delamination proceeds through a swollen material intermediate which is characterized using powder X-ray diffraction (PXRD). Subsequent addition of concentrated HCl at room temperature leads to synthesis of UCB-2 via delamination of the swollen PREFER material and is characterized using PXRD, transmission electron microscopy (TEM), and argon gas physisorption, which shows lack of microporosity in UCB-2. (29)Si magic angle sinning (MAS) NMR spectroscopy indicates lack of amorphization during delamination, as indicated by the entire absence of Q(2) resonances, and (27)Al MAS NMR spectroscopy shows exclusively tetrahedral aluminum in the framework following delamination. The delamination process requires both chloride and fluoride anions and is sensitive to solvent, working well in DMF. Experiments aimed at synthesizing UCB-2 using aqueous conditions previously used for UCB-1 synthesis leads to partial swelling and lack of delamination upon acidification. A similar lack of delamination is observed upon attempting synthesis of UCB-1 under conditions used for UCB-2 synthesis. The delamination of PREFER is reversible between delaminated and swollen states in the following manner. Treatment of as-made UCB-2 with the same reagents as used here for the swelling of PREFER causes the delaminated UCB-2 material to revert back to swollen PREFER. This causes the delaminated UCB-2 material to revert back to swollen PREFER. Altogether, these results highlight delamination as the reverse of zeolite synthesis and demonstrate the crucial role of noncovalent self-assembly involving the zeolitic framework and cations/anions/structure-directing agent and solvent during the delamination process.
• Delamination of Layered Zeolite Precursors under Mild Conditions: Synthesis of UCB-1 via Fluoride/Chloride Anion-Promoted Exfoliation

  Isao Ogino, Michael M. Nigra, Son-Jong Hwang, Jeong-Myeong Ha, Thomas Rea, Stacey I. Zones, Alexander Katz

  JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 133 (10) 3288 - 3291 0002-7863 2011/03 [Refereed][Not invited]
   

  New material UCB-1 is synthesized via the delamination of zeolite precursor MCM-22 (P) at pH 9 using an aqueous solution of cetyltrimethylammonium bromide, tetrabutylammonium fluoride, and tetrabutylammonium chloride at 353 K. Characterization by powder X-ray diffraction, transmission electron microscopy, and nitrogen physisorption at 77 K indicates the same degree of delamination in UCB-1 as previously reported for delaminated zeolite precursors, which require a pH of greater than 13.5 and sonication in order to achieve exfoliation. UCB-1 consists of a high degree of structural integrity via Si-29 MAS NMR and Fourier transform infrared spectroscopies, and no detectable formation of amorphous silica phase via transmission electron microscopy. Porosimetry measurements demonstrate a lack of hysteresis in the N-2 adsorption/desorption isotherms and macroporosity in UCB-1. The new method is generalizable to a variety of Si:Al ratios and leads to delaminated zeolite precursor materials lacking amorphization.
• A bioinspired approach for controlling accessibility in calix[4]arene-bound metal cluster catalysts

  Namal de Silva, Jeong-Myeong Ha, Andrew Solovyov, Michael M. Nigra, Isao Ogino, Sheila W. Yeh, Kathleen A. Durkin, Alexander Katz

  NATURE CHEMISTRY 2 (12) 1062 - 1068 1755-4330 2010/12 [Refereed][Not invited]
   

  In enzymes, the electronic and steric environments of active centres, and therefore their activity in biological processes, are controlled by the surrounding amino acids. In a similar manner, organic ligands have been used for the 'passivation' of metal clusters, that is, inhibition of their aggregation and control of their environment. However, the ability of enzymes to maintain large degrees of accessibility has remained difficult to mimic in synthetic systems in which little room, if any, is typically left to bind to other species. Here, using calix[4]arene macrocycles bearing phosphines as crude mimics of the rigid backbones of proteins, we demonstrate the synthesis of gold clusters and the control of their accessibility through an interplay between the sizes of the calixarene ligands and metal cores. For 0.9-nm cores, 25% of all the gold atoms within the cluster bind to the chemisorption probe 2-naphthalenethiol. This accessibility dramatically decreases with 1.1-nm and 4-nm gold cores.
• Reactions of Highly Uniform Zeolite H-beta-Supported Rhodium Complexes: Transient Characterization by Infrared and X-ray Absorption Spectroscopies

  Isao Ogino, Bruce C. Gates

  JOURNAL OF PHYSICAL CHEMISTRY C 114 (18) 8405 - 8413 1932-7447 2010/05 [Refereed][Not invited]
   

  A zeolite H-beta-supported mononuclear rhodium diethene complex (Rh(C(2)H(4))(2){O(2)Al}, where the braces indicate a part of the zeolite) was formed by the reaction of Rh(acac)(eta(2)-C(2)H(4))(2) (acac = acetylacetonate, C(5)H(7)O(2)(-)) with the zeolite. Transient characterization of the sample by X-ray absorption near edge structure (XANES) and infrared (IR) spectroscopies (combined with mass spectrometry of the effluent gas) while the sample was in contact with flowing CO indicates a simple stoichiometric conversion of the supported metal complex into another species, identified by the spectra as the zeolite-supported rhodium gem-dicarbonyl (Rh(CO)(2){O(2)Al}). The sharpness of the nu(CO) bands in the IR spectrum indicates a high degree of uniformity of the supported rhodium gem-dicarbonyl, and isosbestic points in the XANES spectra as the transformation was occurring imply that the rhodium diethene complex was also highly uniform. Spectra similarly show that treatment of the supported rhodium gem-dicarbonyl with flowing C(2)H(4) resulted in another stoichiometrically simple transformation, giving a species suggested to be Rh(C(2)H(4))(CO)(2){O(2)Al}. The intermediate was ultimately transformed when the sample was purged with helium into another highly uniform supported species, inferred on the basis of IR spectra to be Rh(C(2)H(4))(CO){O(2)Al}. Extended X-ray absorption fine structure spectra characterizing the supported rhodium diethene complex and the species formed from it show how the Rh-O bond distance at the Rh-support interface varied in response to the changes in the ligands bonded to the rhodium.
• Essentially Molecular Metal Complexes Anchored to Zeolite beta: Synthesis and Characterization of Rhodium Complexes and Ruthenium Complexes Prepared from Rh(acac)(eta(2)-C2H4)(2) and cis-Ru(acac)(2)(eta(2)-C2H4)(2)

  Isao Ogino, Bruce C. Gates

  JOURNAL OF PHYSICAL CHEMISTRY C 114 (6) 2685 - 2693 1932-7447 2010/02 [Refereed][Not invited]
   

  Mononuclear complexes of rhodium and of ruthenium, Rh(acac)(eta(2)-C2H4)(2) and cis-Ru(acac)(2)(eta(2)-C2H4)(2) (acac = C5H7O2-), were used as precursors to synthesize metal complexes bonded to zeolite beta. Infrared (IR) and extended X-ray absorption fine structure (EXAFS) spectra show that the species formed from Rh(acac)(eta(2)- C2H4)(2) was Rh(eta(2) -C2H4)(2)(+), which was bonded to the zeolite at aluminum sites via two Rh-O bonds. Reaction of this supported rhodium complex with CO gave the supported rhodium gem-dicarbonyl Rh(CO)(2)(+), which was characterized by two nu(co) bands in the IR spectrum, at 2048 and 2115 cm(-1), that were sharp (fwhm of 2115-cm(-1) band = 5 cm(-1)), indicating a high degree of uniformity of the supported species. Nearly the same result was observed (Liang, A. et al. J. Am. Chem. Soc. 2009, 131, 8460) for the isostructural rhodium complex supported on dealuminated MY zeolite, which was characterized by frequencies of the vco bands that were 4 and 2 cm(-1), respectively, greater than those characterizing the zeolite beta-supported complex. This comparison indicates that the Rh atoms in Rh(eta(2)-C2H4)(2)(+) anchored on zeolite beta were slightly more electron-rich than those on zeolite Y. This inference is supported by EXAFS results showing shorter Rh-C bonds in the zeolite beta-supported rhodium ethene complex than in the zeolite Y-supported rhodium ethene complex. In contrast to these supported rhodium complexes, the zeolite beta-supported ruthenium samples were shown by IR and EXAFS spectroscopies to consist of mixtures of mononuclear ruthenium complexes with various numbers of acac ligands; when CO reacted with the supported ruthenium complexes, the resultant ruthenium carbonyls were characterized by vco spectra characteristic of both ruthenium dicarbonyls and ruthenium tricarbonyls.
• Zeolite-supported metal complexes of rhodium and of ruthenium: a general synthesis method influenced by molecular sieving effects

  Isao Ogino, Cong-Yan Chen, Bruce C. Gates

  DALTON TRANSACTIONS 39 (36) 8423 - 8431 1477-9226 2010 [Refereed][Invited]
   

  A general method for synthesis of supported metal complexes having a high degree of uniformity is presented, whereby organometallic precursors incorporating acetylacetonate (C(5)H(7)O(2)(-), acac) ligands react with zeolites incorporating OH groups near Al sites. The method is illustrated by the reactions of Rh(acac)(CO)(2) and of cis-Ru(acac)(2)(eta(2)-C(2)H(4))(2) with zeolites slurried in n-pentane at room temperature. The zeolites were H-Beta, H-SSZ-42, H-Mordenite, and HZSM-5. Infrared (IR) and extended X-ray absorption fine structure spectra of the zeolites incorporating rhodium complexes indicate the formation of Rh(CO)(2)(+) bonded near Al sites; similar results have been reported for the formation of zeolite-supported Rh(eta(2)-C(2)H(4))(2+) from Rh(acac)(eta(2)-C(2)H(4))(2). IR spectra of the supported rhodium gem-dicarbonyls include sharp, well-resolved nu(CO) bands, demonstrating that the sites surrounding each metal complex are nearly equivalent. The frequencies of the nu(CO) bands show how the composition of the zeolite influences the bonding of the supported species, demonstrating subtle differences in the roles of the zeolite as ligands. When the zeolite has pore openings larger than the critical diameter of the precursor organometallic compound, the latter undergoes facile transport into the interior of the zeolite, so that a uniform distribution of the supported species results, but when the precursors barely fit through the zeolite apertures, the mass transport resistance is significant and the supported metal complexes are concentrated near the pore mouths.
• A Zeolite-Supported Molecular Ruthenium Complex with eta(6)-C6H6 Ligands: Chemistry Elucidated by Using Spectroscopy and Density Functional Theory

  Isao Ogino, Mingyang Chen, Jason Dyer, Philip W. Kletnieks, James F. Haw, David A. Dixon, Bruce C. Gates

  CHEMISTRY-A EUROPEAN JOURNAL 16 (25) 7427 - 7436 0947-6539 2010 [Refereed][Not invited]
   

  An essentially molecular ruthenium-benzene complex anchored at the aluminum sites of dealuminated zeolite Y was formed by treating a zeolite-supported mononuclear ruthenium complex, [Ru(acac)(eta(2)-C2H4)(2)](+) (acac = acetylacetonate, C5H7O2-), with (C6H6)-C-13 at 413 K. IR, C-13 NMR, and extended X-ray absorption fine structure (EXAFS) spectra of the sample reveal the replacement of two ethene ligands and one acac ligand in the original complex with one (C6H6)-C-13 ligand and the formation of adsorbed protonated acac (Hacac). The EXAFS results indicate that the supported [Ru(eta(6)-C6H6)](2+) incorporates an oxygen atom of the support to balance the charge, being bonded to the zeolite through three Ru-O bonds. The supported ruthenium benzene complex is analogous to complexes with polyoxometalate ligands, consistent with the high structural uniformity of the zeolite-supported species, which led to good agreement between the spectra and calculations at the density functional theory level. The calculations show that the interaction of the zeolite with the Hacac formed on treatment of the original complex with (C6H6)-C-13 drives the reaction to form the ruthenium-benzene complex.
• Transient Spectroscopic Characterization of the Genesis of a Ruthenium Complex Catalyst Supported on Zeolite Y

  Isao Ogino, Bruce C. Gates

  JOURNAL OF PHYSICAL CHEMISTRY C 113 (46) 20036 - 20043 1932-7447 2009/11 [Refereed][Not invited]
   

  A mononuclear ruthenium complex anchored to dealuminated zeolite HY, Ru(acac)(C(2)H(4))(2)(+) (acac = acetylacetonate, C(5)H(7)O(2)(-)), was characterized in flow reactors by transient infrared (IR) spectroscopy and Ru K edge X-ray absorption spectroscopy. The combined results show how the supported complex was converted into a form that catalyzes ethene conversion to butene. The formation of these species resulted from the removal of acac ligands from the ruthenium (as shown by IR and extended X-ray absorption fine structure (EXAFS) spectra) and the simultaneous decrease in the symmetry of the ruthenium complex, with the ruthenium remaining mononuclear and its oxidation state remaining essentially unchanged (as shown by EXAFS and X-ray absorption near-edge structure spectra). The removal of anionic acac ligands from the ruthenium was evidently compensated by the bonding of other anionic ligands, such as hydride from H(2) in the feed stream, to form species suggested to be Ru(H)(C(2)H(4))(2)(+), which is coordinatively unsaturated and inferred to react with ethene, leading to the observed formation of butene in a catalytic process.
• Role of the Support in Catalysis: Activation of a Mononuclear Ruthenium Complex for Ethene Dimerization by Chemisorption on Dealuminated Zeolite Y

  Isao Ogino, Bruce C. Gates

  CHEMISTRY-A EUROPEAN JOURNAL 15 (28) 6827 - 6837 0947-6539 2009 [Refereed][Not invited]
   

  A set of supported ruthenium complexes with systematically varied ratios of chemisorbed to physisorbed species was formed by contacting cis-[Ru(acac)(2)(C(2)H(4))(2)] (I; acac = C(5)H(7)O(2)(-)) with dealuminated zeolite Y. Extended X-ray absorption fine structure (EXAFS) spectra used to characterize the samples confirmed the systematic variation in the loadings of the two supported species and demonstrated that removal of bidentate acac ligands from I accompanied chemisorption to form [Ru(acac)(C(2)H(4))(2)](+) attached through two Ru-O bonds to the Al sites of the zeolite. A high degree of uniformity in the chemisorbed species was demonstrated by sharp bands in the infrared (IR) spectrum characteristic of ruthenium dicarbonyls that formed when CO reacted with the anchored complex. When the ruthenium loading exceeded 1.0 wt% (Ru/Al approximate to 1:6), the additional adsorbed species were simply physisorbed. Ethene ligands on the chemisorbed species reacted to form butenes when the temperature was raised to approximately 393 K: acac ligands remained bonded to Ru. In contrast, ethene ligands on the physisorbed complex simply desorbed under the same conditions. The chemisorption activated the ruthenium complex and facilitated dimerization of the ethene, which occurred catalytically. IR and EXAFS spectra of the supported samples indicate that 1) Ru centers in the chemisorbed species are more electron deficient than those in the physisorbed species and 2) Ru-ethene bonds in the chemisorbed species are less symmetric than those in the physisorbed species, which implies the presence of a preferred configuration for the catalytic dimerization.
• Molecular chemistry in a zeolite: Genesis of a zeolite Y-supported ruthenium complex catalyst

  Isao Ogino, Bruce C. Gates

  JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 130 (40) 13338 - 13346 0002-7863 2008/10 [Refereed][Not invited]
   

  Dealuminated zeolite Y was used as a crystalline support for a mononuclear ruthenium complex synthesized from cis-Ru(acac)(2)(C2H4)(2). Infrared (IR) and extended X-ray absorption fine structure spectra indicated that the surface species were mononuclear ruthenium complexes, Ru(acac)(C2H4)(2)(2+), tightly bonded to the surface by two Ru-O bonds at Al3+ Sites of the zeolite. The maximum loading of the anchored ruthenium complexes was one complex per two Al3+ sites; at higher loadings, some of the cisRu(acac)(2)(C2H4)(2) was physisorbed. In the presence of ethylene and H-2, the surface-bound species entered into a catalytic cycle for ethylene dimerization and operated stably. IR data showed that at the start of the catalytic reaction, the acac ligand of the Ru(acac)(C2H4)(2)(2+) species was dissociated and captured by an Al3+ site. Ethylene dimerization proceeded similar to 600 times faster with a cofeed of ethylene and H2 than without H-2. These results provide evidence of the importance of the cooperation of the Al3+ sites in the zeolite and the H-2 in the feed for the genesis of the catalytically active species. The results presented here demonstrate the usefulness of dealuminated zeolite Y as a nearly uniform support that allows precise synthesis of supported catalysts and detailed elucidation of their structures.
• Structure-directing agent location and non-centrosymmetric structure of fluoride-containing zeolite SSZ-55

  A Burton, RJ Darton, ME Davis, SJ Hwang, RE Morris, Ogino, I, SI Zones

  JOURNAL OF PHYSICAL CHEMISTRY B 110 (11) 5273 - 5278 1520-6106 2006/03 [Refereed][Not invited]
   

  Single crystals Of pure silica zeolite SSZ-55 were prepared using the fluoride route. Single-crystal X-ray diffraction at a synchrotron source revealed the framework structure of the material, but the unit cell (orthorhombic a = 12.905(2) angstrom, b = 21.344(4) angstrom, c = 5.1279(10)) is too small to accommodate ordered arrays of the organic structure-directing agent. Molecular modeling was used to simulate the docking of the structure-directing agent in the channels of the material, and this revealed a strong space-filling interaction with a number of possible orientations of the organic cation. The overall non-centrosymmetric structure of the solid (spacegroup C222(1)) was confirmed using second harmonic generation experiments.
• The fluoride-based route to all-silica molecular sieves; a strategy for synthesis of new materials based upon close-packing of guest-host products

  SI Zones, SJ Hwang, S Elomari, Ogino, I, ME Davis, AW Burton

  COMPTES RENDUS CHIMIE 8 (3-4) 267 - 282 1631-0748 2005/03 [Refereed][Not invited]
   

  This study surveys the use of a range of structure-directing agents (SDA) in zeolite synthesis experiments under the conditions using HE The studies made are all for systems containing only silica as the inorganic component. Key points to emerge from the study are a reinforcement of the concept of more open-framework host structures forming when the reactions are more concentrated (lower H(2)O/SiO(2) ratios). This discovery had been reported previously from the research group at ITQ in Valencia, Spain. Our studies show that some novel all-silica compositions have been achieved using this route for synthesis. Two new relationships we explore are whether the use of fluoride anion in synthesis has different nucleation selectivities as a function of dilution, and whether guest molecules can achieve tighter packing in the host structures using the fluoride route as contrasted with the hydroxide route. We explore this with MAS NMR studies. We find that some large organo-cations, which produce no products in alkaline media, give interesting host structure in the fluoride reactions. (c) 2005 Published by Elsevier SAS on behalf of Academie des sciences.
• Molecular sieve synthesis using alkylated sparteine derivatives as structure-directing agents

  Ogino, I, ME Davis

  MICROPOROUS AND MESOPOROUS MATERIALS 67 (1) 67 - 78 1387-1811 2004/01 [Refereed][Not invited]
   

  (-)-Sparteine is alkylated to prepare a series of compounds that are used as structure-directing agents (SDAs) to specifically crystallize large pore molecular sieves. Two new sparteine derivatives, N-ethylsparteinium (EtSPA) and N,N'-dimethylsparteinium (Me(2)SPA), are synthesized and their single crystal X-ray structures obtained. The results from molecular sieve syntheses using EtSPA and Me(2)SPA are compared to previously reported preparations that employed N (16)-methylsparteinium (MeSPA). In general, crystalline phases obtained with MeSPA, e.g., SSZ-24, CIT-5, ITQ-21, can also be prepared using EtSPA and Me(2)SPA. However, Me(2)SPA did produce what appears to be a new phase from a reaction mixture containing Zn2+. (C) 2003 Elsevier Inc. All rights reserved.
• A stable "ship in the bottle" type 12-molybdophosphoric acid encaged Y-type zeolite catalyst for liquid phase reactions

  Shin R. Mukai, Isao Ogino, Litsu Lin, Yumi Kondo, Takao Masuda, Kenji Hashimoto

  Reaction Kinetics and Catalysis Letters 69 (2) 253 - 258 0133-1736 2000 [Refereed][Not invited]
   

  The stability of a "ship in the bottle" type 12-molybdophosphoric acid encaged catalyst was drastically enhanced by stabilizing the acidic species of the catalyst by partial exchange of its protons with cesium cations. This catalyst practically acted as a solid catalyst in the esterification of acetic acid with ethanol.
• Preparation of encaged heteropoly acid catalyst by synthesizing 12-molybdophosphoric acid in the supercages of Y-type zeolite

  Mukai, SR, T Masuda, Ogino, I, K Hashimoto

  APPLIED CATALYSIS A-GENERAL 165 (1-2) 219 - 226 0926-860X 1997/12 [Refereed][Not invited]
   

  12-molybdophosphoric acid encaged in the supercages of Y-type zeolite was synthesized from molybdenum oxide and phosphoric acid, in a slurry mixture of Y-type zeolite crystals and deionized water. After thorough washing in hot water, the 12-molybdophosphoric acid was found to remain in the Y-type zeolite, at an amount estimated to be 0.09 g (g-support)(-1). Catalysts thus obtained were found to show activity for the esterification of acetic acid with ethanol, indicating that this catalyst could be used as a solid acid catalyst in various liquid phase reactions which involve water. (C) 1997 Elsevier Science.

MISC

• マクロ孔を活用した窒素ドープグラフェンの迅速マイクロ波改質

  小田原匠, 荻野勲, 岩村振一郎, 小野博信, 向井紳  化学工学会大会(Web)  2021-  2021
• 水素の層間アニオン脱離促進効果を利用した層状複水酸化物の熱処理

  平山雄大, 荻野勲, 岩村振一郎, 向井紳  化学工学会大会(Web)  2021-  2021
• マイクロ波改質による窒素ドープ炭素のORR活性向上

  菅田輝, 荻野勲, 岩村振一郎, 向井紳  化学工学会年会研究発表講演要旨集(CD-ROM)  86th-  2021
• Cu⁺/Cu⁰比の制御を目指したゼオライト担持触媒の開発とアセトアルデヒド選択合成への利用

  樋口友輔, 荻野勲, 岩村振一郎, 向井紳  化学工学会年会研究発表講演要旨集(CD-ROM)  86th-  2021
• マイクロ波処理による炭素系触媒の酸素還元反応活性の向上

  荻野勲, 一家拓矢, 岩村振一郎, 小野博信, 向井紳  化学工学会年会研究発表講演要旨集(CD-ROM)  84th-  2019
• ゼオライト層状前駆体の欠陥サイトを利用した金属担持触媒の合成

  菊原一将, 荻野勲, 向井紳  ゼオライト研究発表会講演予稿集  35th-  2019
• ファイバーテンプレート法によりマイクロ流路を導入したモノリス状Pt/C触媒の開発

  女鹿浩幸, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  50th-  2018
• メソポーラスカーボン細孔内でのMoVO複合酸化物触媒の合成と選択酸化反応への利用

  佐藤裕貴, 田邑圭介, 小船井諒, 荻野勲, 上田渉, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  50th-  2018
• LPI-CNFを用いたリチウム空気電池正極用シート状電極の開発

  住田稜, 牛島啓太, 坂井一樹, 岩村振一郎, 荻野勲, 向井紳  化学工学会大会(Web)  2018-  2018
• マイクロ波加熱による酸化グラファイト由来グラフェン系炭素材料の低欠陥化

  深澤剛, 皆上昂ノ介, 荻野勲, 岩村振一郎, 向井紳  化学工学会大会(Web)  2018-  2018
• ナノシートを利用した高表面積Mg-Al複合酸化物の合成

  田中怜, 荻野勲, 向井紳  日本吸着学会研究発表会講演要旨集  32nd-  2018
• メソ孔性炭素材料の細孔内を利用した結晶性MoVO複合酸化物の合成と選択酸化反応での評価

  田邑圭介, 小船井諒, 荻野勲, 上田渉, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  49th-  2017
• カーボンゲルの細孔構造がPt担持に及ぼす影響

  相原拓哉, 佐藤耕大, 岩村振一郎, 荻野勲, 向井紳  炭素材料学会年会要旨集  44th-  2017
• 炭素材料の構造と表面特性のリチウム空気電池充放電特性への影響

  藤田和樹, 岩村振一郎, 荻野勲, 向井紳  炭素材料学会年会要旨集  44th-  2017
• ファイバーテンプレート法により直状流路を導入した高表面積なモノリス状吸着剤の開発

  高橋和也, 吉田誠一郎, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  49th-  ROMBUNNO.EA115  2017  [Not refereed][Not invited]
  
• マイクロハニカム構造を有するカーボンクライオゲルによるフェノールと色素の連続分離

  吉田誠一郎, 岩村振一郎, 荻野勲, 向井紳  化学工学会年会研究発表講演要旨集(CD-ROM)  81st-  ROMBUNNO.ZAA333  2016/03/13  [Not refereed][Not invited]
  
• 長尺カーボンナノファイバーから作製したシート電極のリチウム空気電池空気極特性

  岩村振一郎, 住田稜, 坂井一樹, 荻野勲, 向井紳  電池討論会講演要旨集  57th-  2016
• 混合溶媒を用いたゼオライト層状前駆体の層剥離に関する詳細検討

  白部大知, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  48th-  2016
• 液パルスインジェクション法による電極材料用TiO₂/Cナノ複合体の高効率製造

  岩村振一郎, 藤田和樹, 岩城凌, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  48th-  2016
• 炭素系固体酸触媒の液相反応への利用:表面の親疎水性と細孔構造が触媒活性へ与える影響

  鈴木佑啓, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  48th-  2016
• カーボンゲルマイクロハニカムを用いたフェノールの連続分離

  吉田誠一郎, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  ROMBUNNO.L124  2015/09/09  [Not refereed][Not invited]
  
• リチウム空気電池正極細孔構造がLi₂O₂析出量に与える影響

  坂井一樹, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• 液パルスインジェクション法によるリチウムイオン電池負極用シリコン/炭素ナノ複合材料の製造

  岩城凌, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• 細孔内合成による微小なα-MnO₂とカーボンゲルの複合化

  梅津僚太郎, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• PMMA鋳型によるフェノール樹脂由来多孔質炭素の合成とガス賦活による高表面積化

  森武士, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• カーボンゲル-カーボンナノファイバー複合体の高レートEDLC電極への応用

  大西健太, 鎌足俊輔, 森武士, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• 長尺カーボンナノファイバーを用いた導電性シートの開発

  住田稜, 岩城凌, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• 液パルスインジェクション法によるSi/Cナノ複合体の効率的製造とリチウムイオン電池負極特性

  岩村振一郎, 岩城凌, 荻野勲, 向井紳  電池討論会講演要旨集  56th-  2015
• 酸化グラフェン由来の多孔質炭素の合成

  深澤剛, 北野耕平, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• 酸化グラフェンを利用したPt/C触媒の合成

  北野耕平, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• 凍結乾燥操作を利用した水分散Mg-Al系複水酸化物ナノシートの再構築

  工藤修一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• 混合溶媒を用いたゼオライト層状前駆体の層剥離

  白部大知, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• スルホ基導入カーボンゲルを担体に用いた燃料電池用Pt/C触媒の開発

  佐藤耕大, 岩村振一郎, 荻野勲, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  47th-  2015
• 液パルスインジェクション法によるシリコン/炭素ナノ複合体の製造とリチウムイオン電池負極材料への応用

  岩城凌, 住田稜, 岩村振一郎, 荻野勲, 向井紳  炭素材料学会年会要旨集  42nd-  2015
• 液パルスインジェクション法により製造される炭素ナノ粒子の構造解析

  岩村振一郎, 岩城凌, 藤田和樹, 荻野勲, 向井紳  炭素材料学会年会要旨集  42nd-  2015
• CO₂賦活カーボンゲルの細孔構造がリチウム空気電池特性に与える影響

  坂井一樹, 梅津僚太郎, 岩村振一郎, 荻野勲, 向井紳  炭素材料学会年会要旨集  42nd-  2015
• カーボンゲルを利用したα-MnO₂の粒子径制御

  梅津僚太郎, 岩村振一郎, 荻野勲, 向井紳  炭素材料学会年会要旨集  42nd-  2015
• Pt担持カーボンゲルへのスルホ基導入

  佐藤耕大, 岩村振一郎, 荻野勲, 向井紳  炭素材料学会年会要旨集  42nd-  2015
• 酸化グラフェンを利用したPt/C触媒の合成と応用

  北野耕平, 岩村振一郎, 荻野勲, 向井紳  炭素材料学会年会要旨集  42nd-  2015
• Synthesis and catalytic consequences of delaminated layered zeolite precursors

  Richard Ouyang, Ron Runnebaum, Isao Ogino, Son-Jong Hwang, Dan Xie, Stacey Zones, Alexander Katz  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY  247-  2014/03  [Not refereed][Not invited]
  
• Synthesis of a non-conventional monolithic catalyst for continuous flow reaction systems

  Isao Ogino, Daiki Ando, Yoshitaka Satoh, Shunpei Takahashi, Shin R. Mukai  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY  247-  2014/03  [Not refereed][Not invited]
  
• Efficient cesium recovery from fluid flows using a silica-alumina microhoneycomb including Prussian Blue analog nanoparticles

  Shin Mukai, Yoshinao Kimura, Seiichiro Yoshida, Isao Ogino  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY  247-  2014/03  [Not refereed][Not invited]
  
• ジルコニアと溶融塩を用いたCO2の分解

  鈴木亮輔, 菊地竜也, 坂口紀史, 上田幹人, 熊谷剛彦, 夏井俊悟, 荻野 勲, 内山拓也, 若松貴文, 石田龍馬, 北村三佳, 松浦史弥, 羽田大将  炭素循環型製鉄研究会最終報告会「炭素循環型スマート製鉄(iACRES)による低炭素化への貢献」  27-  31  2014/03  [Not refereed][Not invited]
  
• セシウムの連続分離に適したマイクロハニカム状ヘテロポリ酸塩・シリカ複合体の開発

  吉田誠一郎, 木村佳直, 荻野勲, 向井紳  化学系学協会北海道支部冬季研究発表会講演要旨集(CD-ROM)  2014-  ROMBUNNO.2B04  2014/01/28  [Not refereed][Not invited]
  
• 凍結操作を利用した水分散Mg-Al金属水酸化物ナノシートの再構築

  工藤修一郎, 荻野勲, 岩村振一郎, 向井紳  化学工学会秋季大会研究発表講演要旨集(CD-ROM)  46th-  2014
• 新規層剥離法による酸化グラフェン調製

  荻野勲, 横山裕也, 北野耕平, 岩村振一郎, 向井紳  触媒討論会討論会A予稿集  114th-  2014
• Enhanced CO Tolerance of PEFC Anode Catalyst by Optimized Degree of Activation of Resorcinol-Formaldehyde Carbon Support

  N. Narischat, T. Takeguchi, T. Mori, I. Ogino, S. R. Mukai, W. Ueda  POLYMER ELECTROLYTE FUEL CELLS 14  64-  (3)  145  -150  2014  [Not refereed][Not invited]
   

  In this study, a series of resorcinol-formaldehyde carbons (RFCs) were prepared by varying the degree of activation such as 0, 42, and 58, in order to control their surface areas and porosity. Then, these RFCs were used as supports to prepare Pt2Ru3 anode catalysts. These catalysts were characterized by many techniques including BET, DH calculation, XRD, STEM and CO tolerant by polymer electrolyte fuel cell (PEFC) single cell analysis. It was found that higher degree of activation of RFCs (i.e. rc1400ac42 and rc1400ac58) have larger micropore and mesopore volume. In case of CO tolerant by PEFC single cell unit, Pt2Ru3/rc1400ac58 showed the same performance as the commercial Pt2Ru3/C in pure H-2 (0.76 V at 0.2 A/cm(2)), but Pt2Ru3/rc1400ac58 showed superior performance at 2000 ppm CO contamination. Nafion dispersion of Pt2Ru3/rc1400ac58 was also found to be better than that of the Pt2Ru3/C, since pore structure was optimized by degree of activation.
• 12‐モリブドリン酸三アンモニウムを固定化シリカマイクロハニカムによるセシウムの連続処理

  吉田誠一郎, 木村佳直, 荻野勲, 向井紳  日本吸着学会研究発表会講演要旨集  27th-  19  2013/11/21  [Not refereed][Not invited]
  
• マイクロリアクター型固体触媒の合成-シリカマイクロハニカム流路表面へのMg/Alナノシートの集積固定化-

  安藤大輝, 荻野勲, 向井紳  触媒討論会討論会A予稿集  112th-  2013
• 不溶性フェロシアン化物のシリカ‐アルミナマイクロハニカムへの包含によるセシウム吸着剤の創製

  木村佳直, 吉田誠一郎, 荻野勲, 向井紳  日本吸着学会研究発表会講演要旨集  26th-  31  2012/11/14  [Not refereed][Not invited]
  
• Synthesis of Zeolite Nanosheets via Delamination of Layered Zeolite Precursors

  荻野 勲  ゼオライト  29-  (4)  127  -134  2012
• New class of delaminated zeolite precursors for selective conversion of heavy hydrocarbons

  Isao Ogino, Michael M. Nigra, Sonjong Hwang, Thomas Rea, Stacey I. Zones, Alexander Katz  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY  241-  2011/03  [Not refereed][Not invited]
  
• Factors in the zeolite synthesis selectivity in using large organo-cations in HF-based reactions.

  S Zones, ME Davis, SJ Hwang, Ogino, I, A Burton, R Morris  ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY  227-  U870  -U870  2004/03  [Not refereed][Not invited]
  

Books etc

• Conversion of Carbohydrates to High Value Products (in Heterogeneous Catalysts: Emerging Techniques for Design, Characterization and Applications)

  Isao Ogino, edited, by Wey, Yang Teoh, Atsushi Urakawa, Yun Hau Ng, Patrick Si (Contributor)
  Wiley-VCH 2021/03
• Understanding Atomically Dispersed Supported Metal Catalysts: Structure and Performance of Active Sites (in SPR Catalysis Volume 31)

  Isao Ogino, edited by James Spivey, Yi-Fan Han, Dushyant Shekhawat (Contributor)
  The Royal Society of Chemistry 2019 (ISBN: 9781788014540) 

  Catalysts are required for a variety of applications and industrialists and academics are increasingly challenged to find cost effective and environmentally benign catalysts to use. This volume looks at modern approaches to catalysis and reviews the extensive literature including direct methane conversion, nanocomposite catalysts for transformation of biofuels into syngas and hydrogen and catalytic wet air oxidation technology for industrial wastewater treatment.
• Supported Catalysts (in Handbook of Solid State Chemistry)

  Isao Ogino, Pedro Serna, Bruce C. Gates, edited, by, R. Dronskowski, S. Kikkawa, A. Stein (Contributor)
  Wiley-VCH 2017/08 (ISBN: 9783527325870) 

  Catalysts make chemical reactions go faster, often by many orders of magnitude in comparison with purely thermal processes. The dominant technological catalysts are solids, which offer the important practical benefit of being readily separated from fluid‐phase products. Solid catalysts are usually porous, having high internal surface areas and therefore high numbers of catalytically active species per unit of reactor volume to facilitate high rates of catalytic reaction. The preparation of common supported catalysts involves support synthesis, deposition of catalyst precursor components, and treatment to convert the supported species into catalytically active species. Industrial catalysts are also subjected to additional processing to control the sizes and shapes of the final product. The effect of the structure of a crystal face on catalysis is typically diagnosed in experiments with single crystals exposing various faces and often rationalized on the basis of relationships between the crystallographic orientations and the adsorbate‐adsorbent (reactant‐catalyst) binding energies.
• Synthesis of 2D Zeolites (Zeolite Nanosheets)

  Isao Ogino (Contributor)
  CMC 2015/11 (ISBN: 9784781310954) 11 

  Leading Edge Technology of High Functional Zeolite Editorial Supervisor: Toshihide Baba
• Zeolite-supported Molecular Metal Complex Catalysts (in Atomically-Precise Methods for Synthesis of Solid Catalysts)

  Isao Ogino, Sophie Hermans, Thierry Visart, de Bocarme Ed (Contributor)
  The Royal Society of Chemistry 2014/11 (ISBN: 9781849738293) 

  There is much interest in preparing catalysts with specific structures for a desired catalytic activity. Although there has been a great amount of research into correlating particles sizes and microstructure to catalytic activity, knowledge about practical catalysts still remain ill-defined. The current challenge is now to understand atomic control.
• Ice Templating Method (Handbook of Gel Technology)

  Isao Ogino, Shin R. Mukai (Contributor)
  NTS 2014

Presentations

• マイクロ波加熱を利用した窒素ドープ炭素系触媒の高性能化  [Invited]

  荻野勲

  第 3 回 ワークショップ  2021/07
• Efficient Microwave-Assisted Annealing of Reduced Graphene Oxides in an up-Flow Reactor

  Konosuke Minakami, Isao Ogino, Shinichiroh Iwamura, Hironobu Ono, Shin R. Mukai

  2020 Virtual AIChE Annual Meeting  2020/11
• Scalable Synthesis of Metal Oxide Supports with High Surface Area and Basic Site Density from Mg-Al Layered Double Hydroxides

  Isao Ogino, Rei Tanaka, Kudo Suichiroh, Shin R. Mukai

  26th North American Catalysis Society Meeting  2019/06
• Enhancing Oxygen Reduction Reaction Performance of Nitrogen-doped Carbon through Microwave-assisted Annealing in NH3

  Isao Ogino, Takuya Ikka, Shinichiroh Iwamura, Hironobu Ono, Shin R. Mukai

  26th North American Catalysis Society Meeting  2019/06
• Confined-Space Synthesis of Nanocrystalline Mo-VO Mixed Oxides Using a Mesoporous Carbon

  Ryo Obunai, Keisuke Tamura, Isao Ogino, Shin Mukai, Wataru Ueda

  2019 North American Catalysis Society Meeting  2019/06
• Control of crystallinity and defect concentration of graphene-based materials through microwave annealing  [Invited]

  Isao Ogino

  Seminar on functional nanomaterials (Department of Applied Chemistry & Biochemistry, Kumamoto University)  2018/09
• Locations of Defective SiO– Sites in Lamellar Precursors of Pure-Silica MWW-Type Molecular Sieves

  Isao Ogino, Taichi Shirobe, Shin Mukai

  25th North American Catalysis Society Meeting  2017/06
• On the Influence of Mass Transport in Sulfonated Carbon Catalysts Derived from Various Carbon Sources on Liquid-Phase Esterification Reactions

  Isao Ogino, Yukei Suzuki, Shin R. Mukai

  2016 AIChE Annual Meeting  2016/11
• A Mixed-Solvent Approach to Delaminate Layered Zeolitic Precursors

  Isao Ogino, Taichi Shirobe, Shin R. Mukai

  2016 AIChE Annual Meeting  2016/11
• Adsorption of Water Contaminants in Continuous Flow Systems Using Carbon Cryogels with a Microhoneycomb Structure

  Seiichiroh Yoshida, Shinichiroh Iwamura, Isao Ogino, Shin R. Mukai

  2016 AIChE Annual Meeting  2016/11
• Synthesis of a Non-Conventional Monolithic Catalyst by Immobilizing Mg/Al Layered Double Hydroxides within Microchannels of a Silica Monolith

  Isao Ogino, Daiki Andoh, Shin R. Mukai

  2013 AIChE Annual Meeting  2016/11
• Sulfonated carbon catalysts synthesized from various carbon sources

  Yukei Suzuki, Isao Ogino, Shin R. Mukai

  The 16th International Congress on Catalysis  2016/07
• The Society of Chemical Engineers, Japan, Autumn Meeting, Sapporo, Japan, September 9, 2015  [Invited]

  Isao Ogino

  2015/09
• Synthesis of Graphene Oxide Via Sonication-Free Exfoliation of Graphite Oxide

  Isao Ogino, Yuya Yokoyama, Shinchiroh Isamura, Shin R. Mukai

  2014 AIChE Annual Meeting  2014/11
• Synthesis of Graphene Oxide Via Sonication-Free Exfoliation of Graphite Oxide

  Isao Ogino, Yuya Yokoyama, Shinichiroh Iwamura, Shin R. Mukai

  2014 AIChE Annual Meeting  2014/11
• Synthesis of Carbon Nanofibers from Light Liquid Paraffins Using the Liquid Pulse Injection Technique

  Shin R. Mukai, Ryoto Hirahashi, Riku Furukawa, Yuusuke Rikima, Shinichiro Iwamura, Isao Ogino

  2014 AIChE Annual Meeting  2014/11
• Continuous Cesium Separation Using a Silica Microhoneycomb Supporting Ammonium Molybdophosphate

  Seiichiroh Yoshida, Shin R. Mukai, Kimura Yoshinao, Isao Ogino

  2014 AIChE Annual Meeting (ISBN: 978-0-8169-1086-1)  2014/11
• ISC Seminar, National Institute of Advanced Industrial Science and Technology (AIST), Japan, October 8, 2014  [Invited]

  Isao Ogino

  2014/10
• Nagoya Univ.-Tsinghua Univ.-Toyota Motor Corp.-Hokkaido Univ. Joint Symposium, Sapporo, Japan, July 22, 2014  [Invited]

  Isao Ogino

  2014/07
• 247th ACS National Meeting & Exposition, Gabor A. Somorjai Award for Creative Research in Catalysis: Symposium in Honor of Mark E. Davis, Dallas, Texas, March 17, 2014  [Invited]

  Isao Ogino

  2014/03
• The Japan Petroleum Institute Seminar, Sapporo, Japan, January 25, 2013  [Invited]

  Isao Ogino

  2013/01
• Electrochemistry Seminar, Nogata, Japan, September 6, 2012  [Invited]

  Isao Ogino

  2012/09
• Catalysis Seminar, Tokachi, Japan, August 8, 2012  [Invited]

  Isao Ogino

  2012/08
• 10th Biomass Conversion Seminar, Sapporo, Hokkaido, February 24, 2012  [Invited]

  Isao Ogino

  2012/02

Teaching Experience

Chemical engineering laboratory (015160)Chemical engineering laboratory (015160) Hokkaido University
Separation process engineering (CHEM_ELMOL 6112)Separation process engineering (CHEM_ELMOL 6112) Hokkaido university
Transport phenomena (015209)Transport phenomena (015209) Hokkaido university
Chemical kinetics (015239)Chemical kinetics (015239) Hokkaido university

Research Projects

• マイクロ波を用いた高性能炭素系非白金触媒合成プロセスの創出

  科学技術振興機構：A-STEP機能検証フェーズ

  -2021/03 

  Author : 荻野勲, 岩村振一郎, 向井紳
• Synthesis of supported catalysts using zeolitic nanosheets

  Japan Society for the Promotion of Science：Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (B)

  Date (from‐to) : 2017/04 -2020/03 

  Author : Ogino Isao

   

  Atomically-dispersed metals on oxide supports have attracted significant interest as catalytic materials for energy and environmental applications. In this work, we aimed to develop a synthetic method to confine small metal species within zeolitic materials using layered zeolitic precursors. We studied the synthesis conditions of layered zeolitic precursors, extraction methods of organic structure-directing agents from interlayer spaces of layered precursors, the type and composition of amino alcohols and metal complexes, and thermal activation conditions of synthesized samples. We found that supported catalysts with highly dispersed metal species can be synthesized through a proper choice of amino alcohol and metal complex and adjustment of thermal activation condition. We found further that the synthesized catalyst exhibits significantly higher activity than other catalysts in a test reaction.
• Development of Long Functional Nanofibers for Performance Improvement of Various Energy Storage Devices

  Japan Society for the Promotion of Science：Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (B)

  Date (from‐to) : 2016/04 -2019/03 

  Author : Mukai Shin

   

  Previously, we developed an original method to efficiently produce long carbon nanofibers at extremely high growth rates, the Liquid Pulse Injection Technique. In this study, we expanded this method to incorporate new functions into the nanofibers. Methods to cast the resulting fibers into sheets, and also methods to mold the fibers into monoliths were developed in order to make the use of such nanofibers easier. Sheets and monoliths of functional fibers obtained through the developed methods were used to improve the performance of energy storage devices such as electric double layer capacitors.
• Development of nanofiborous CO2 sorbents for sorption-enchanced production of hydrogen

  Japan Society for the Promotion of Science：Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Exploratory Research

  Date (from‐to) : 2016/04 -2018/03 

  Author : Mukai Shin

   

  In this work, we aimed at the synthesis of high-temperature CO2 adsorbents from nanosheets derived from MgAl double layered hydroxides, which will be potentially used to intensify the existing hydrogen production processes. In addition, we aimed at the synthesis of fiborous CO2 sorbents that can be readily molded into filters. As a result, we succeeded in preparing nanofiborous materials a few hundreds nm in diameter. In addition, through CO2 sorption experiments conducted in both batch and flow systems, we found that Mg/Al mixed oxides obtained by heat treatment in flowing nitrogen adsorbed CO2 up to 8-times higher than those obtained by heat treatment in flowing air. This research has brought important insights into how to improve the performance of Mg/Al mixed oxides as high-temperature adsorbents.
• Synthesis of new porous materials and thin films through delamination of layered materials and reconstruction of nanosheets

  Japan Society for the Promotion of Science：Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (C)

  Date (from‐to) : 2014/04 -2017/03 

  Author : Ogino Isao

   

  This research aimed to synthesis new porous materials and thin films, which will be potentially used as catalysts, adsorbents, and electrode materials, through delamination of layered materials and reconstruction of resultant nanosheets. Several important results were obtained as listed below: 1. Graphene-like materials with large lateral sizes were successfully obtained through a new delamination method that relies on fast phase change of slurry containing dispersed graphene oxides. 2. High purity graphene-like materials with low defect sites were obtained by microwave-driven annealing of graphene oxides. 3. Nanofiborous solid acid-base materials were obtained by fast freezing of aqueous dispersions containing Mg/Al double hydroxide nanosheets.
• Synthesis of supported ionic liquid catalysts with microhoneycomb structure

  Japan Society for the Promotion of Science：Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Exploratory Research

  Date (from‐to) : 2014/04 -2016/03 

  Author : Mukai Shin, OGINO Isao, IWAMURA Shinichiro

   

  In this research, as a first step to synthesize supported ionic liquid catalysts, we aimed to prepare CO2 absorbents by coating the surface of microchannels of silica microhoneycombs (SMHs) with ionic liquid (IL) that bears an amino group. We found that as much as 55 wt % of the IL can be coated on a SMH without clogging its microchannels. The resultant material caused low pressure drop like the original SMH when helium was passed through it and enabled fast CO2 uptake both in bath and flow absorption systems. The prepared absorbent can be reused at least 4 times without loss in performance by regenerating it by heat treatment at 393 K in flowing nitrogen. Collectively, the results show promising properties of the prepared material for CO2 separation.
• Development and Morphology Controlling of a Solid Acid for the Fast and Selective Separation of Cesium

  Japan Society for the Promotion of Science：Grants-in-Aid for Scientific Research Grant-in-Aid for Scientific Research (B)

  Date (from‐to) : 2012/04 -2015/03 

  Author : MUKAI Shin, OGINO Isao, IWAMURA Shinichiro

   

  In this work, heteropoly acids which form insoluble salts with Cs+ and Prussian blue analogues which selectively adsorb Cs+ were respectively dispersed and immobilized in silica gels and silica-alumina gels using freezing in order to obtain materials which allow the selective recovery of Cs+ existing in an extremely dilute state. Such materials were also molded into the form of microhoneycombs by controlling the direction of freezing in order to reduce the resistance they cause against fluid flows, and to significantly enhance their response speed towards Cs+ recovery.
• Synthesis of new porous materials via reconstruction of funcitonal nanosheets obtained by freeze-thaw exfoliation method

  Japan Society for the Promotion of Science：Grants-in-Aid for Scientific Research Grant-in-Aid for Challenging Exploratory Research

  Date (from‐to) : 2012/04 -2014/03 

  Author : MUKAI Shin, OGINO Isao

   

  This research aims to develop a new exfoliation method that relies on phase-change of water and can exfoliate layered materials to obtain nanosheets. The research also aims to reconstruct the resultant nanosheets into functional materials via phase-change of water. (1) We have successfully exfoliated graphite oxide in water to obtain dispersed graphene oxide nanosheets with high efficiency via rapid freezing-thawing cycle of the solution.(2) We have also succeeded in the reconstruction of the resultant graphene oxide into a 3D macroporous monolith using ice crystals as the template.
• Preparation of microreactor-type solid catalysts via immobilization of zeolite nanosheets

  Japan Society for the Promotion of Science：Grants-in-Aid for Scientific Research Grant-in-Aid for Young Scientists (B)

  Date (from‐to) : 2012/04 -2014/03 

  Author : OGINO Isao

   

  This research aims to synthesize high-performance solid catalysts via immobilization of zeolite nanosheets or nanocrystals, which exhibit molecular recognition properties, on the microchannels of a solid support. We investigated the pre-treatment conditions of the solid support as well as immobilization methods and successfully prepared a solid catalyst, which potentially exhibits the aimed catalytic properties.

Industrial Property Rights

• 特開2021-006497:低欠陥化炭素材料の製造方法  

  向井紳, 荻野勲, 岩村振一郎, 皆上昂ノ介, 小野博信
• 特開2020-090409:低欠陥化含窒素炭素材料の製造方法  

  向井紳, 荻野勲, 岩村振一郎, 一家拓矢, 小野博信
• WO2018105570:低欠陥化グラフェン系炭素材料及びその製造方法  

  向井紳, 荻野勲, 岩村振一郎, 深澤剛
• 特許6569101:カーボンナノファイバーの製造方法  

  向井 紳、荻野 勲、岩村 振一郎、鎌足 俊輔、山口 東吾、西川 翔悟
• 特開2015-026482:多孔質炭素材料及びその製造方法  

  向井 紳, 荻野 勲, 森 武士, 広瀬 寛, 錦織 英孝
• 特許6214028:酸化グラフェン含有液の製造方法及びその利用  

  向井 紳, 荻野 勲, 横山 裕也
• 特開2013-159515:メソポーラスカーボンゲルとその製造方法  

  向井 紳, 三浦 雄一郎, 荻野 勲

Social Contribution

• Board Member, The Society of Chemical Engineers for Japan, Hokkaido Region

  Date (from-to) : 2015-Today

  Role : Others
• Member, National Advisory Board, International Symposium on Zeolite and Microporous Crystals 2018, August 5–9

  Date (from-to) : 2018/08/05-2018/08/08

  Role : Organizing member
• Session Chair, International Symposium on Zeolite and Microporous Crystals 2018, August 5–9

  Date (from-to) : 2018/08/06-2018/08/06

  Role : Others
• Member, Organizing Committee, Catalysis Seminar in Hokkaido, Catalysis Society of Japan, July 8–9

  Date (from-to) : 2018/07/08-2018/07/09

  Role : Organizing member
• Organizing Committee, The 5th International Symposium on Ambitious Leader’s Program Fostering Future Leaders to Open New Frontiers in Materials Science, Hokkaido University, November 21–22

  Date (from-to) : 2017/11/21-2017/11/22

  Role : Organizing member
• Session Chair, the 17th Asia Pacific Confederation of Chemical Engineers Congress (APCChE 2017), August 23–27

  Date (from-to) : 2017/08/23-2017/08/27

  Role : Others
• Session Chair, Hokkaido University – University of California, Berkeley, Joint Symposium on Chemical Sciences and Engineering, January 7

  Date (from-to) : 2017/01/06-2017/01/08

  Role : Others
• Member, Organizing Committee, Hokkaido University – University of California, Berkeley, Joint Symposium on Chemical Sciences and Engineering, January 7

  Date (from-to) : 2017/01/06-2017/01/08

  Role : Organizing member
• Secretary, The Society of Chemical Engineers for Japan, Hokkaido Region

  Date (from-to) : 2015-2016

  Role : Others
• Session Chair, 5th German-Japanese Joint Symposium “Development and Technology of Carbon Materials,” July 20–21, 2015, TU Bergakademie Freiberg Reiche Zeche, IEC-Haus1 Fuchsmühlenweg 9, 09599, Germany

  Date (from-to) : 2015/07/20-2015/07/21

  Role : Others
• Member, Organizing Committee, International Symposium on Zeolite and Microporous Crystals 2015, June 28–July 2

  Date (from-to) : 2015/06/28-2015/07/02

  Role : Organizing member
• Chair, Department Seminar (Speaker, Distinguished Prof. Bruce C. Gates)

  Date (from-to) : 2013/09/06-2013/09/06

  Role : Others
• Member, Organizing Committee, 22th Chemical Engineering and Particle Engineering Research Conference, The Society of Chemical Engineers for Japan, Hokkaido Region, February 1–2

  Date (from-to) : 2013/02/01-2013/02/02

  Role : Others