研究者データベース

HOURDET DOMINIQUE(ウルデ ドミニク)
国際連携研究教育局 ソフトマターグローバルステーション
教授

基本情報

所属

  • 国際連携研究教育局 ソフトマターグローバルステーション

職名

  • 教授

J-Global ID

研究キーワード

  • hybrid hydrogels   responsive copolymers   associating polymers   macromolecular assemblies   

研究分野

  • ナノテク・材料 / 高分子材料 / from synthesis to properties

職歴

  • 2016年06月 - 現在 University of Hokkaido Global Station for Soft Matter Professor
  • 2010年10月 - 現在 UPMC-Paris 6 Material Chemistry Professor
  • 2000年10月 - 2010年09月 UPMC-Paris 6 Material Chemistry Associate professor
  • 1990年10月 - 2000年09月 UPMC-Paris 6 Material Chemistry Assistant Professor

学歴

  •         - 1989年05月   UPMC-Paris 6 / France   Polymer chemistry and physics   PhD
  •         - 1984年06月   UPMC-Paris 6 / France   Polymer chemistry and physics   Master of science

研究活動情報

論文

  • Hui Guo, Nicolas Sanson, Dominique Hourdet, Alba Marcellan
    ADVANCED MATERIALS 28 28 5857 - 5864 2016年07月 [査読有り][通常論文]
     
    A novel mode of gel toughening displaying crack bifurcation is highlighted in phase-separated hydrogels. By exploring original covalent network topologies, phase-separated gels under isochoric conditions demonstrate advanced thermo responsive mechanical properties: excellent fatigue resistance, self-healing, and remarkable fracture energies. Beyond the phase-transition temperature, the fracture proceeds by a systematic crack-bifurcation process, unreported so far in gels.
  • Hui Guo, Cecile Mussault, Annie Brulet, Alba Marcellan, Dominique Hourdet, Nicolas Sanson
    MACROMOLECULES 49 11 4295 - 4306 2016年06月 [査読有り][通常論文]
     
    The challenge of this work was to investigate the role of topology in LOST hydrogels that strongly and reversibly thermo-reinforce their mechanical strength under isochoric conditions. To achieve this, two different hydrogels with opposite topologies were designed on the basis of grafted architectures using equal amounts of water-soluble chains (poly(N,N-dimethylacrylamide) = PDMA) and LOST polymer chains (poly(N-isop' ropylacrylainide) = PNIPA). By working under isochoric conditions, with almOst 85 wt % of water in the whole temperature range (20-60 degrees C), we were able to clearly highlight the impact of the phase transition of PNIPA on the mechanical reinforcement of the gel without any interference of the volume transition. These graft hydrogels, designed with PNIPA in the backbone (GPN-D) or as pendant chains (G-15D-N), have been studied more specifically by tensile tests and 2D neutron scattering at rest and under deformation. From these complementary techniques, we show that PNIPA side-chains in GPD-N self-assemble above their transition temperature into a micellar network "greatly interfering with the covalent PDMA frame. While the elastic modulus increases reversibly more than ten times throughout the phase transition, other properties-like elongation at break and fracture resistance are greatly enhanced with temperature. At high temperature and under extension, SANS data highlight the affine deformation of PNIPA domains. By comparison, the opposite topology with PNIPA forming the cross-linked backbone undergoes a similar phase separation with temperature and gives rise to a bicontinuous structure that aligns under loading. The collapsed phase being topologically defined as the load" bearing phase, GPN-D displays remarkable fracture toughening with crack bifurcation at high temperature whereas GPD-N gels fracture in a more conventional way.
  • Hui Guo, Annie Brulet, Pattuparambil R. Rajamohanan, Alba Marcellan, Nicolas Sanson, Dominique Hourdet
    POLYMER 60 164 - 175 2015年03月 [査読有り][通常論文]
     
    This work, based on structure/properties relationships of associating polymers, aims to investigate the role of topology in the self-assembling behavior of responsive graft copolymers. For that purpose, two graft copolymers with inverse topologies were prepared with similar amounts of water-soluble chains (poly(N,N-dimethylacrylamide) = PDMA) and LCST polymer chains (poly(N-isopropylacrylamide) = PNIPA). In pure water, and above 3 wt%, PNIPA-g-PDMA and PDMA-g-PNIPA exhibit very similar macroscopic properties with a sol/gel transition above 35 degrees C related to the microphase separation of PNIPA sequences. From complementary experiments, performed by DSC, H-1 NMR and small angle neutron scattering, we show that the phase transition of PNIPA is more abrupt when NIPA units are located within the backbone, compared to side-chains. Nevertheless, well above their transition temperature, the two copolymers display very similar bicontinuous structures where PNIPA sequences self aggregate into concentrated percolating domains (about 70 wt% at 60 degrees C) characterized by a frozen dynamics. On the other hand, when salt or surfactant molecules are added into unentangled semi-dilute aqueous solution, the PNIPA-g-PDMA sample does not percolate anymore above the transition temperature while PDMA-g-PNIPA still demonstrate thermothickening properties that are correlated to the ability of water-soluble PDMA chains to bridge PNIPA aggregates. (C) 2015 Elsevier Ltd. All rights reserved.
  • Nivika R. Gupta, Arun A. T. Torris, Prakash P. Wadgaonkar, P. R. Rajamohanan, Guylaine Ducouret, Dominique Hourdet, Costantino Creton, Manohar V. Badiger
    CARBOHYDRATE POLYMERS 117 331 - 338 2015年03月 [査読有り][通常論文]
     
    New thermo associating polymers were designed and synthesized by grafting amino terminated poly(ethylene oxide-co-propylene oxide) (PEPO) onto carboxymethyl guar (CMG) and carboxymethyl tamarind (CMT). The grafting was performed by coupling reaction between-NH2 groups of PEPO and -COOH groups of CMG and CMT using water-soluble EDC/NHS as coupling agents. The grafting efficiency and the temperature of thermo-association, T-assoc in the copolymer were studied by NMR spectroscopy. The graft copolymers, CMG-g-PEPO and CMT-g-PEPO exhibited interesting thermo-associating behavior which was evidenced by the detailed rheological and fluorescence measurements. The visco-elastic properties (storage modulus, G'; loss modulus, G") of the copolymer solutions were investigated using oscillatory shear experiments. The influence of salt and surfactant on the T-assoc was also studied by rheology, where the phenomenon of "Salting out" and "Salting in" was observed for salt and surfactant, respectively, which can give an easy access to tunable properties of these copolymers. These thermo-associating polymers with biodegradable nature of CMG and CMT can have potential applications as smart injectables in controlled release technology and as thickeners in cosmetics and pharmaceutical formulations. (C) 2014 Elsevier Ltd. All rights reserved.
  • Severine Rose, Alba Marcellan, Tetsuharu Narita, Francois Boue, Fabrice Cousin, Dominique Hourdet
    SOFT MATTER 11 29 5905 - 5917 2015年 [査読有り][通常論文]
     
    Nano-hybrid hydrogels were prepared by cross-linking polymerization of N,N-dimethylacrylamide (DMA) within a dispersion of silica nano-particles. Working at constant polymer/water ratio, the mechanical properties of hydrogels can be finely tuned by changing either the level of covalent cross-linker and/or the amount of particles that act as physical cross-linkers through specific adsorption of PDMA chains. Whatever is the cross-linking ratio (from 0 to 1 mol%), the introduction of silica nano-particles dramatically improves the mechanical behavior of hydrogels with a concomitant increase of stiffness and nominal strain at failure. The physical interactions being reversible in nature, the dynamics of the adsorption/desorption process of PDMA chains directly controls the time-dependence of the mechanical properties. Small angle neutron scattering experiments, performed in contrast matching conditions, show that silica particles, which repel themselves at short range, remain randomly dispersed during the formation of the PDMA network. Although PDMA chains readily interact with silica particles, no significant variation of the polymer concentration was observed in the vicinity of silica surfaces. Together with the time dependence of physical interactions pointed out by mechanical analyses, this result is attributed to the moderate adsorption energy of PDMA chains with silica surfaces at pH 9. From 2D SANS experiments, it was shown that strain rapidly gives rise to a non affine deformation of the hybrid network with shearing due to the transverse compression of the particles. After loading at intermediate deformation, the particles recover their initial distribution due to the covalent network that is not damaged in these conditions. That is no longer true at high deformation where residual anisotropy is observed.
  • Guillaume Sudre, Dominique Hourdet, Costantino Creton, Fabrice Cousin, Yvette Tran
    LANGMUIR 30 32 9700 - 9706 2014年08月 [査読有り][通常論文]
     
    We investigated the effect of specific interactions on the structure of interfaces between a brush and a hydrogel on the polymer chain length scale. We used a model system for which the interactions between the brush and the gel are switchable. We synthesized weak polyelectrolyte brushes of poly(acrylic acid) and hydrogels of polyacrylamide and poly(N,N-dimethylacrylamide) which interact solely when the poly(acrylic acid) is mainly in its acidic form. The monomer density profiles of the poly(acrylic acid) brush immersed in pure deuterium oxide (D2O) or in contact with a D2O-swollen gel were determined by neutron reflectivity. At pH 2 when the brush is in its neutral form, it interacts with the gel by hydrogen bonds while at pH 9 when the brush is a polyelectrolyte it is not interacting with the gel. Our results show that the presence of interactions with the gel at pH 2 increases the swelling ratio of the brush relative to that in pure D2O, meaning that the brushes exhibit conformations which are more extended from the surface than in the absence of interactions.
  • Laurence Petit, Linn Carlsson, Severine Rose, Alba Marcellan, Tetsuharu Narita, Dominique Hourdet
    MACROMOLECULAR SYMPOSIA 337 1 58 - 73 2014年03月 [査読有り][通常論文]
     
    Based on specific interactions taking place between poly(N,N-dimethylacrylamide) [PDMA] and silica nanoparticles, two strategies were used to improve the viscoelastic properties of aqueous formulations. First, PDMA oligomers were grafted onto a non-adsorbing poly(acrylamide-co-sodium acrylate) backbone. With this architecture, the binding process of PDMA side-chains with silica nanoparticles was shown to proceed very similarly to free PDMA chains and to promote the formation of hybrid physical networks. The viscoelastic properties of these systems are controlled by the concentration of inorganic cross-links and the fraction of adsorbing grafts involved in the formation of bridges between particles. An optimum weight ratio between silica and grafts was found for the viscoelastic properties, in agreement with the saturation of silica beads by the PDMA precursor. While the homogeneous formation of such hybrid assemblies remains limited to mixtures involving low polymer concentrations (<= 2wt%), we show that homogeneous hybrid networks can be readily prepared by direct polymerization of DMA monomer (>= 5wt%), with or without chemical cross-linker, in a suspension of silica nanoparticles. In this case, the specific interactions taking place between the silica filler and the whole polymer network give rise to a very unusual combination of properties where elasticity, dissipation, strength and strain at failure are enhanced simultaneously. While the intrinsic structure of the network can be controlled by the level of chemical cross-linking, physical interactions dominate the dissipation process with a dramatic time dependence of the mechanical properties.
  • Severine Rose, Alexandre Prevoteau, Paul Elziere, Dominique Hourdet, Alba Marcellan, Ludwik Leibler
    NATURE 505 7483 382 - + 2014年01月 [査読有り][通常論文]
     
    Adhesives are made of polymers(1) because, unlike other materials, polymers ensure good contact between surfaces by covering asperities, and retard the fracture of adhesive joints by dissipating energy under stress(2,3). But using polymers to 'glue' together polymer gels is difficult, requiring chemical reactions, heating, pH changes, ultraviolet irradiation or an electric field(4-7). Here we show that strong, rapid adhesion between two hydrogels can be achieved at room temperature by spreading a droplet of a nanoparticle solution on one gel's surface and then bringing the other gel into contact with it. The method relies on the nanoparticles' ability to adsorb onto polymer gels and to act as connectors between polymer chains, and on the ability of polymer chains to reorganize and dissipate energy under stress when adsorbed onto nanoparticles. We demonstrate this approach by pressing together pieces of hydrogels, for approximately 30 seconds, that have the same or different chemical properties or rigidities, using various solutions of silica nanoparticles, to achieve a strong bond. Furthermore, we show that carbon nanotubes and cellulose nanocrystals that do not bond hydrogels together become adhesive when their surface chemistry is modified. To illustrate the promise of the method for biological tissues, we also glued together two cut pieces of calf's liver using a solution of silica nanoparticles. As a rapid, simple and efficient way to assemble gels or tissues, this method is desirable for many emerging technological and medical applications such as microfluidics, actuation, tissue engineering and surgery.
  • Severine Rose, Alba Marcellan, Dominique Hourdet, Tetsuharu Narita
    MACROMOLECULES 46 13 5329 - 5336 2013年07月 [査読有り][通常論文]
     
    Nanohybrid gels based on poly(acrylamide-co-N,N-dimethylacrylamide), P(AAm-co-DMA), and colloidal silica nanoparticles were synthesized by radical polymerization, and the influence of hydrogen bonding between DMA and silica nanoparticles on the dynamics of the network and the nanoparticles were studied by dynamic light scattering. As previously reported, in the case of polyacrylamide homopolymer, PAAm, which have no hydrogen bonding with silica, we observed two decay modes in the hybrid gels, a gel mode and a Brownian diffusion mode of silica nanoparticles. When we increased the DMA weight fraction (or physical cross-link density), we observed (1) a higher scattered light intensity than the silica suspension and the gel without silica, (2) an increased plateau value of the autocorrelation function, (3) a slowing down of the silica diffusion mode, and (4) no influence on the gel mode. These results, compared with those of the mixtures of the linear PDMA and silica nanoparticles in solution (showing an increase in the scattered light intensity and in the hydrodynamic radius), indicate that the P(AAm-co-DMA) hybrid gels have a more heterogeneous structure due to the adsorption of the polymer on the silica nanoparticles, and that the silica nanoparticles, trapped in the network due to the adsorption of the polymer, show a cage dynamics in the network. The local viscoelastic properties probed by the bound nanoparticles are discussed.
  • Dominique Hourdet, Guylaine Ducouret, Sony Varghese, Manohar V. Badiger, Prakash P. Wadgaonkar
    POLYMER 54 11 2676 - 2689 2013年05月 [査読有り][通常論文]
     
    Two series of Hydrophobically Modified Polyacrylamides (HMPAMs) were prepared by free radical copolymerization of trimethylsilylacrylamide with 3-pentadecylcyclohexylacrylamide (PDCAM) or dodecylacrylamide (DDAM) followed by removal of trimethylsilyl protecting groups. The solution properties of HMPAMs were studied in dilute aqueous solution by fluorescence spectroscopy, NMR and viscometry. The properties in aqueous solution of HMPAMs clearly displayed the formation of hydrophobic interactions between alkyl stickers. While dodecyl containing HMPAMs mainly showed a progressive collapse of the copolymer coil with the increasing fraction of hydrophobic moieties (weak intra-chain associations), pentadecylcyclohexyl groups containing HMPAMs exhibited a much lower solubility in water due to strong intra- and inter-chain associations. Experimental data were analyzed using the mean field theory developed by Semenov and Rubinstein (SR) for associating polymers. Using a set of realistic parameters, taking into account the solubility of the backbone, the fraction of stickers and the strength of hydrophobic attractions, we show that the SR model offers a quantitative description of the thermodynamic properties of HMPAMs in terms of individual and collective behavior of polymers chains; i.e. swelling and phase separation, respectively. (C) 2013 Elsevier Ltd. All rights reserved.
  • Dominique Hourdet
    Macromolecular Chemistry and Physics 214 2882 - 2890 2013年 [査読有り][通常論文]
  • Dominique Hourdet
    Macromolecules 46 4567 4574  2013年 [査読有り][通常論文]
  • Dominique Hourdet
    Macromolecules 46 4095 - 4104 2013年 [査読有り][通常論文]


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