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109. Importance of the decoration in shaped cobalt nanoparticles in the acceptor-less secondary alcohol dehydrogenation

Author

Kaźmierczak, Kamila, primary, Ramamoorthy, Raj Kumar, additional, Moisset, Arthur, additional, Viau, Guillaume, additional, Viola, Arnaud, additional, Giraud, Marion, additional, Peron, Jennifer, additional, Sicard, Lorette, additional, Piquemal, Jean-Yves, additional, Besson, Michèle, additional, Perret, Noémie, additional, and Michel, Carine, additional

Published
2020
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112. Importance of water in selective alcohol oxidation catalyzed by gold and platinum

Author

Gu, Qingyi, Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Bourse CSC, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Michel, Carine

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

National audience

Published
2018

113. Au-Cu bimetallic catalysts for the selective oxidation of fatty alcohol ethoxylates to alkyl ether carboxylic acids

Author

Gu, Qingyi, Michel, Carine, Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Bourse CSC, Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2018

114. Understanding the stability of γ-Alumina in aqueous medium for biomass conversion

Author

Michel, Carine, Réocreux, Romain, Sautet, Philippe, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Michel, Carine, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, [CHIM.MATE]Chemical Sciences/Material chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2017

116. Adsorption of lubricant additives by molecular modeling

Author

Blanck, Sarah, Loehlé, Sophie, Steinmann, Stephan N., Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Steinmann, Stephan N.

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract

International audience

Published
2019

117. Solvation of noble metals surfaces in water by a local-suface/water forcefield

Author

Clabaut, Paul, Michel, Carine, Steinmann, Stephan N., Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Steinmann, Stephan N., École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2019

118. Wettability@Al2O3: Adsorption of lubricant additives by molecular modeling

Author

Blanck, Sarah, Loehlé, Sophie, Steinmann, Stephan N., Michel, Carine, Steinmann, Stephan N., TOTAL, Centre de recherche de Solaize (CReS), Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract

International audience

Published
2019

119. Developing an efficient approach for the computation of solvation free energy at the metal/liquid interface

Author

Clabaut, Paul, Michel, Carine, Steinmann, Stephan N., Steinmann, Stephan N., Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract

International audience

Published
2019

121. Decomposition mechanism of lignin models on Pt(111) combining single crystal experiments and first principle calculations

Author

Michel, Carine, Réocreux, Romain, Sautet, Philippe, Ould Hamou, Cherif Aghiles, Giorgi, Javier B., Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), University of Ottawa [Ottawa], LIA Funcat, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Michel, Carine

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2017

122. Molecular oxygen activation catalyzed by gold: unraveling the role of base

Author

Gu, Qingyi, Michel, Carine, Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Bourse CSC, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2017

123. Modeling reactivity at the solid/liquid interface: are we there yet?

Author

Michel, Carine, Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and DCP

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience; To describe reactions occurring at the solid/water interface is currently one of the major challenges in modeling in Heterogeneous Catalysis in particular in the context of Green Chemistry and biomass valorization where water is a natural solvent. Modeling such an interface requires a proper depiction of the water solvent together with an adequate description of the surface state. Several approaches are available nowadays in the literature, from continuum models to a full explicit description of the liquid water.[1]We have recently shown that continuum models are key to a proper description of reactions occurring at the electrochemical interface on the formic acid oxidation into CO2.[2] They also open the door to a proper inclusion of the effect of co-adsorbed anions in thermal heterogeneous catalysis.[3] In both cases, charges are involved and the electrostatic contribution in the major one. When H-bonding between the liquid water and the reactant or intermediate is crucial, continuum models are not sufficient and an explicit inclusion of water molecule is a necessity. As a first step, micro-solvation can be an effective approach that allowed us to interpret solvent effect in the conversion of levulinic acid into γ-valerolactone.[4] Moving to a full description of reactivity the water/metal interface is still beyond a full complete DFT approach provided the minimal size of the periodic cell that is necessary and the minimal sampling required. Nevertheless, being less demanding, inspecting transformations occurring at oxide/water interface is now reachable, as illustrated by our recent work on the stability of γ-alumina in water.[5]REFERENCES[1].M. Saleheen, A. Heyden, ACS Catal. 2018, 8,. 2188-2194 [2].S. N. Steinmann, C. Michel, R. Schwiedernoch, J.-S. Filhol, P. Sautet, Chemphyschem, 2015, 16, 2307-2311[3].P. Wang, S. N. Steinmann, G. Fu, C. Michel, and P. Sautet, ACS Catalysis, 2017, 7, 1955–1959[4].C. Michel, J. Zaffran, A. M. Ruppert, J. Matras-Michalska, M. Jedrzejczyk, J. Grams, P. Sautet, Chem. Comm. 2014, 50, 12450–12453 [5].R. Réocreux, “Biomass derivatives in heterogeneous catalysis: adsorption, reactivity and support from first principles”, PhD thesis, (2017)

Published
2017

124. Modelling heterogeneous photocatalysts for water splitting: What can we ask from quantum chemistry?

Author

Le Bahers, Tangui, Antton, Curutchet, Garcia-Esparza, Angel T., Melissen, Sigismund Teunis Alexander George, Steinmann, Stephan N., Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), and Le Bahers, Tangui

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2018

125. White Book on Physical and Rehabilitation Medicine in Europe. Introductions, Executive Summary, and Methodology

Author

Negrini, Stefano, Moslavac, Saša, Cantista, Pedro, Ceravolo, Maria Gabriella, Christodoulou, Nicolas, Delarque, Alain, Gutenbrunner, Christoph, Kiekens, Carlotte, Varela-Donoso, Enrique, Ward, Anthony B., Zampolini, Mauro, Antunes, Filipe, Boldrini, Paolo, Boyer, Francois Constant, Burn, John P. S., Devecerski, Gordana, Didier, Jean- Pierre, Foti, Calogero, Franchignoni, Franco, Grimby, Gunnar, Ilieva, Elena M., Janssen, Wim G. M., Juocevicius, Alvydas, Kucukdeveci, Ayse A., Lains, Jorge, Laxe, Sara, McElligott, Jacinta, McNamara, Angela, Michail, Xanthi, Oral, Aydan, Ozcakar, Levent, Quittan, Michael, Rapidi, Christina-Anastasia, Rode, Gilles, Singh, Rajiv K., Sjolund, Bengt H., Stam, Henk J., Stucki, Gerold, Takac, Peter, Tederko, Piotr, Aguiar- Branco, Catarina, Bardot, Philippe, Barotsis, Nikolaos, Bertolini, Carlo, Bickenbach, Jerome, Borg, Kristian, Chaler, Joaquim, Chamberlain, Anne, Delargy, Mark, Giustini, Alessandro, Glaesener, Jean-Jacques, Grabljevec, Klemen, Hornacek, Karol, Jandric, Slavica Dj., Kujawa, Jolanta, Marincek, Crt, Michel, Carine, Nulle, Anda, Nunes, Renato, Pascoa, Pinheiro Joao, Paysant, Jean, Perennou, Dominic, Popa, Daiana, Rapin, Amandine, Rossetti, Yves, Rosulescu, Eugenia, Smolenski, Ulrich Christian, Stibrant, Sunnerhagen Katharina, Tesio, Luigi, Valero- Alcaide, Raquel, Vetra, Aivars, Votava, Jiri, Wade, Derick T., Wever, Daniel, Winkelmann, Andreas, and Rehabilitation Medicine

Subjects
030506 rehabilitation, medicine.medical_specialty, medicine.medical_treatment, Specialty, Physical Therapy, Sports Therapy and Rehabilitation, World health, Convention, 03 medical and health sciences, 0302 clinical medicine, Physical medicine and rehabilitation, Humans, Medicine, media_common.cataloged_instance, Disabled Persons, Books* Disabled Persons/rehabilitation* Europe Humans Physical and Rehabilitation Medicine, Functioning, European union, Competence (human resources), media_common, Disability, Executive summary, Rehabilitation, business.industry, Books, Physical and Rehabilitation Medicine, Europe, Action plan, 0305 other medical science, business, 030217 neurology & neurosurgery
Abstract

The White Book (WB) of Physical and Rehabilitation Medicine (PRM) in Europe is produced by the 4 European PRM Bodies (European Academy of Rehabilitation Medicine - EARM, European Society of PRM - ESPRM, European Union of Medical Specialists - PRM Section, European College of PRM-ECPRM served by the European Union of Medical Specialists-PRM Board) and constitutes the reference book for PRM physicians in Europe. It has now reached its third edition; the first was published in 1989 and the second in 2006/2007. The WB has multiple purposes, including providing a unifying framework for European countries, to inform decision-makers on European and national level, to offer educational material for PRM trainees and physicians and information about PRM to the medical community, other rehabilitation professionals and the public. The WB states the importance of PRM, a primary medical specialty that is present all over Europe, with a specific corpus disciplinae, a common background and history throughout Europe. PRM is internationally recognized and a partner of major international bodies, including the World Health Organization (WHO). PRM activities are strongly based on the documents of the United Nations (UN) and WHO, such as the Convention of the Rights of Persons with Disabilities (2006), the World Report on Disability (2011), the WHO Global Disability Action Plan 2014-2021 (2014) and the WHO initiative "Rehabilitation 2030: a call for action" (2017). The WB is organized in 4 sections, 11 chapters and some appendices. The WB starts with basic definitions and concepts of PRM and continues with why rehabilitation is needed by individuals and society. Rehabilitation focuses not only on health conditions but also on functioning. Accordingly. PRM is the medical specialty that strives to improve functioning of people with a health condition or experiencing disability. The fundamentals of PRM, the history of the PRM specialty, and the structure and activities of PRM organizations in Europe are presented, followed by a thorough presentation of the practice of PRM, i.e. knowledge and skills of PRM physicians, the clinical field of competence of PRM, the place of the PRM specialty in the healthcare system and society, education and continuous professional development of PRM physicians, specificities and challenges of science and research in PRM. The WB concludes with the way forward for the specialty: challenges and perspectives for the future of PRM.

Published
2018

126. Developping an efficient approach for the computation of solvation free energy at the metal/liquid interface

Author

Clabaut, Paul, Schweitzer, Benjamin, Michel, Carine, Steinmann, Stephan N., Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), ANR-14-CE06-0030,MuSiC,Simulations multi-échelles de catalyseurs bifontionnels(2014), Steinmann, Stephan N., Appel à projets générique - Simulations multi-échelles de catalyseurs bifontionnels - - MuSiC2014 - ANR-14-CE06-0030 - Appel à projets générique - VALID, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2018

127. A Force Field for Water Over Pt(111): Development, Assessment And Comparison

Author

Steinmann, Stephan N., Michel, Carine, Fleurat-Lessard, Paul, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Institut de Chimie Moléculaire de l'Université de Bourgogne [Dijon] (ICMUB), Centre National de la Recherche Scientifique (CNRS)-Université de Bourgogne (UB)-Institut de Chimie du CNRS (INC), ANR-14-CE06-0030,MuSiC,Simulations multi-échelles de catalyseurs bifontionnels(2014), Steinmann, Stephan N., Appel à projets générique - Simulations multi-échelles de catalyseurs bifontionnels - - MuSiC2014 - ANR-14-CE06-0030 - Appel à projets générique - VALID, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Université de Bourgogne (UB)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2018

128. Front cover - Supported gold–nickel nano-alloy as a highly efficient catalyst in levulinic acid hydrogenation with formic acid as an internal hydrogen source

Author

Keller, Nicolas, Michel, Carine, Ruppert, Agnieszka M., Sautet, Philippe, Brzezińska, Magdalena, Sneka-Płatek, Olga, Kazmierczak, K., Jędrzejczyk, Marcin, Laboratoire des Matériaux, Surfaces et Procédés pour la Catalyse (LMSPC), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Łódź University of Technology, University of California [Los Angeles] (UCLA), University of California, IRCELYON-C'Durable (CDURABLE), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and University of California (UC)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM]Chemical Sciences, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2018

132. Group additivity for adsorbed polyols at a Pt (111) surface under aqueous conditions: DFT precision on a spreadsheet

Author

Schweitzer, Benjamin, Steinmann, Stephan N., Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), ANR-14-CE06-0030,MuSiC,Simulations multi-échelles de catalyseurs bifontionnels(2014), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Steinmann, Stephan N., and Appel à projets générique - Simulations multi-échelles de catalyseurs bifontionnels - - MuSiC2014 - ANR-14-CE06-0030 - Appel à projets générique - VALID

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2017

133. Control of the anisotropic shape of cobalt nanorods in the liquid phase - From experiment to theory… and back

Author

Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Michel, Carine, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.INOR] Chemical Sciences/Inorganic chemistry, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2016

134. When modelling bridges electro-catalysis and heterogeneous catalysis: The case of the formic acid decomposition

Author

Michel, Carine, Steinmann, Stephan N., Sautet, Philippe, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Michel, Carine, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract

International audience; The (electro)-catalytic decomposition of formic acid in solution is a key reaction for transfer hydrogenation, hydrogen storage and direct formic acid fuel cell.1) On the one hand, our first principles simulations of the electrooxidation of formic acid over nickel identify the reorientation of the formate intermediate and the desorption of CO2 as the rate-limiting steps.2) Although they are not associated with an electron transfer, these barriers are strongly modified when the electrochemical potential is explicitly accounted for using a surface charging method and when modelling the influence of the solvent with a continuum. Hence, such a level of modelling is key to understand the kinetic limitations that penalize the reaction.On the other hand, in heterogenous catalytic conditions, palladium supported catalysts are most promising, but the efficiency and selectivity are strongly impacted by the pH, or in other words by the presence of sodium formate in solution.3) We will show that the presence of this anionic promoter is key to render palladium really active. The promoter effect is traced back to the modulation of the electric field at the catalyst surface, with a strongly contrasted action on the various species along the competing pathways. Here again, the activation barrier for the reorientation of the formate intermediate is strongly modified. The promoter effect is well captured by modelling the anion by an electron injected into the surface, and an idealized counter-ion distribution representative of the electrolyte, in a methodology that is reminiscent of the modelling of electrocatalytic processes. However, we will show that the chemical promotion through an adsorbate investigated herein is complementary to electrocatalytic conditions where the potential is maintained constant.References1.Q.-L. Zhu, Q. Xu, Energ. Envir. Sci. 2015, 8, 478-5122.S.N. Steinmann, C.Michel, R.Schwiedernoch, J.-S.Filhol, P.Sautet, , ChemPhysChem, 2015, 16, 2307-23113.K. Jiang, K. Xu, S. Zou, W.-B. Cai, J. Am. Chem. Soc. 2014, 136, 4861.

Published
2016

135. H-transfer processes: Why the chemical environment DOES matter

Author

Dumon, Alexandre S., Michel, Carine, Sautet, Philippe, Pera-Titus, Marc, Ruppert, Agnieszka M., Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, Łódź University of Technology, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Michel, Carine

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2016

136. Searching for Promising Catalysts in Alcohols Aminations by Using Scaling, BEP Relations and Micro-kinetics modeling

Author

Michel, Carine, Tao, Wang, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), ANR-13-CDII-0004,SHAPes,Nouveaux procédés d'amination sélective pour la synthèse de monomères biosourcés(2013), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Michel, Carine, and Chimie Durable – Industries, Innovation - Nouveaux procédés d'amination sélective pour la synthèse de monomères biosourcés - - SHAPes2013 - ANR-13-CDII-0004 - CD2I - VALID

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2016

137. Surface Nitridation Mechanism of Ni Catalyst in Alcohols Aminations

Author

Tao, Wang, Michel, Carine, Pera-Titus, Marc, Sautet, Philippe, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, ANR-13-CDII-0004,SHAPes,Nouveaux procédés d'amination sélective pour la synthèse de monomères biosourcés(2013), Michel, Carine, Chimie Durable – Industries, Innovation - Nouveaux procédés d'amination sélective pour la synthèse de monomères biosourcés - - SHAPes2013 - ANR-13-CDII-0004 - CD2I - VALID, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Eco-Efficient Products & Processes Laboratory (E2P2L), and RHODIA-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2016

138. A join experimental and theoretical study on levulinic acid conversion into gamma-valerolactone

Author

Michel, Carine, Ruppert, Agnieszka M., Grams, Jacek, Sautet, Philippe, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Łódź University of Technology, Michel, Carine, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract

International audience; γ-valerolactone (GVL) is an attractive platform molecule that can be derived from biomass and can be converted to a variety of chemicals, including biofuel additives. It can be nicely derived from cellulose in few steps. The last step is the conversion of levulinic acid (LA) into γ-valerolactone (GVL), where ideally the hydrogen-source is the formic acid that is co-generated with LA. In mild conditions, this reaction is believed to start with the hydrogenation of the ketone function, followed by a cyclizing esterification. While Ru is a poor hydrogenation catalyst compared to Pt or Pd in gas phase, it is efficient in aqueous phase conditions to hydrogenate ketones such as the conversion of LA into GVL. Comparing experiments in THF and water, we showed that the activity of Ru/TiO2 catalyst is highly sensitive to its environment while Pt/TiO2 is not. Better insight is provided by periodic DFT calculations at the GGA level. The presence of a H-bonded water molecule can affect the adsorption of the reactant, intermediate or product. For instance, the obtained alcohol is not directly chemisorbed on the surface: it is strongly h-bonded to the chemisorbed water molecule. This water molecule dramatically reduces the energetic span of the reaction pathway on Ru, hence enhancing the catalytic activity. Conversely, the presence of such a H-bonded water molecule doesn’t not affect the energetic span of the reaction pathway on Pt. Finally, we predict also that this activation can be generalized to other oxophilic metals such as Co or Ni.[1] This study demonstrates that the knowledge accumulated over the years for gas phase reactions at metallic surfaces is not systematically transferable to aqueous phase conditions since water can also play an essential role in the catalytic activity. It also explains why ruthenium is so widely used to transform cellulosic feedstock while it is generally discarded for oil-based feedstock.[2] We further investigated the LA hydrogenation with FA as a hydrogen source using various Ru/C as efficient catalysts. We showed that the intermediate surface formate inhibits at least partially the LA hydrogenation. In addition, the FA decomposition is highly sensitive to the kind of the preparation method of the Ru/C catalyst: (i) the process looks structure sensitive favoured on larger particles and (ii) residual chlorine decreases significantly the FA decomposition rate.[3] REFERENCES[1] Michel, C.; Zaffran, J.; Ruppert, A. M.; Matras-Michalska, J.; Jedrzejczyk, M.; Grams, J. ; Sautet, P. Chem. Comm., 2014, 50, 12450-12453[2] Michel, C. ; Gallezot, P. ACS Catalysis, 2015, 5, 4130-4132[3] Ruppert, A. M.; Jedrzejczyk, M.; Sneka-Platek, O.; Keller, N.; Dumon, A. S.; Michel, C.; Sautet, P. & Grams, J. Green Chem. 2016, ASAP, 10.1039/C5GC02200B

Published
2016

139. Anisole on Pt(111): DFT & UHV for a better picture of lignin decomposition

Author

Réocreux, Romain, Ould Hamou, Cherif Aghiles, Giorgi, Javier B., Michel, Carine, Sautet, Philippe, Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), University of Ottawa [Ottawa], LIA Funcat, Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), and Michel, Carine

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2016

140. Alcohol amination catalyzed by metal supported catalysts: The role of co-adsorbed species revealed by DFT studies

Author

Michel, Carine, Dumon, Alexandre S., Wischert, Raphael, Pera-Titus, Marc, Sautet, Philippe, Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), ANR-13-CDII-0004,SHAPes,Nouveaux procédés d'amination sélective pour la synthèse de monomères biosourcés(2013), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, Michel, Carine, and Chimie Durable – Industries, Innovation - Nouveaux procédés d'amination sélective pour la synthèse de monomères biosourcés - - SHAPes2013 - ANR-13-CDII-0004 - CD2I - VALID

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract

International audience; Amines are essential intermediates in chemical industries. To obtain them from alcohols is an alternative to the current processes that opens the road to the utilization of biomass-sourced alcohols. When catalyzed by metal supported catalysts, this reaction follows the H-borrowing mechanism. It starts with the alcohol dehydrogenation, followed by the addition of the amine on the intermediated aldehyde. Then, the resulting imine is hydrogenated into amine. This hydrogen transfer from the alcohol to the imine is an elegant route that limits the utilization of an external source of H2. In this context, we focus on the challenging amination of aliphatic alcohol by ammonia where the selectivity issue is prominent. In the quest of the best catalyst, we propose here to perform a detailed DFT study of the reaction mechanism on two metals, namely Pd and Ni. We based our study on the hydrogen-borrowing mechanism, using methanol as a simple model of alcohol. We computed the various possible reaction paths for the methanol dehydrogenation and then the imine hydrogenation using periodic DFT calculations with the PBE functional. Since the C-N coupling does not require any metal supported catalyst to proceed efficiently, we didn’t consider the elementary steps of this reaction. Comparing the energetic span obtained on Pd(111) and Ni(111), we predicted that Pd was slightly more active than Ni (1.26eV vs. 1.31eV). However, according to recent experimental studies[Shimizu et al. ACS Catal. 2013, 3, 112−117], Ni supported catalysts are clearly more active than Pd to perform the amination of aliphatic alcohol with ammonia. Since this reaction occurs in liquid phase but under a pressure of ammonia, we evaluate the coverage of ammonia at around 1/9ML at the working pressure and temperature (4 bar, 160°C). Then, we re-investigated the reaction paths including the effect of the co-adsorbed ammonia. On Pd(111), it pushes up slightly the first CH bond breaking in methanol and destabilizes also the strongly adsorbed amine leading to a reduced energetic span of 1.05eV. On Ni(111), the results are even more contrasted: ammonia stabilizes the initial OH scission transition state and strongly destablizes the amine. Then, the energetic span of the overall reaction is reduced to 0.78eV. Ni is then predicted being much more active than Pd. This is a clear example of the importance of co-adsorbed species on the activity of metallic catalysts in hydrogenation/dehydrogenation reactions.

Published
2016

141. An Efficient Theoretical Tool for Screening Promising Heterogeneous Catalysts in Alcohols Selective Aminations

Author

Tao, Wang, Dumon, Alexandre S., Michel, Carine, Pera-Titus, Marc, Sautet, Philippe, Michel, Carine, Chimie Durable – Industries, Innovation - Nouveaux procédés d'amination sélective pour la synthèse de monomères biosourcés - - SHAPes2013 - ANR-13-CDII-0004 - CD2I - VALID, Laboratoire de Chimie - UMR5182 (LC), École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), ANR-13-CDII-0004,SHAPes,Nouveaux procédés d'amination sélective pour la synthèse de monomères biosourcés(2013), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Eco-Efficient Products &Processes Laboratory (E2PL2), and Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2016

142. Anisole decomposition in UHV conditions. When DFT and experiments play ping-pong on a Pt(111) surface

Author

Réocreux, Romain, Ould Hamou, Cherif Aghiles, Giorgi, Javier B., Michel, Carine, Sautet, Philippe, Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), University of Ottawa [Ottawa], LIA Funcat, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2016

143. Computational Studies Across Catalysis

Author

Michel, Carine, Michel, Carine, Laboratoire de Chimie - UMR5182 (LC), Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École normale supérieure - Lyon (ENS Lyon)-Institut de Chimie du CNRS (INC), Ecole Normale Supérieure de Lyon, Christophe Coutanceau, École normale supérieure de Lyon (ENS de Lyon)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, catalysis, biomass, Biomasse, [CHIM.CATA] Chemical Sciences/Catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, Solvatation, Catalyse, DFT
Published
2016

145. C-H Activation and Proton Transfer Initiate Alkene Metathesis Activity of the Tungsten(IV)-Oxo Complex.

Author

Chan, Ka Wing, Chan, Ka Wing, Lam, Erwin, D'Anna, Vincenza, Allouche, Florian, Michel, Carine, Safonova, Olga V, Sautet, Philippe, Copéret, Christophe, Chan, Ka Wing, Chan, Ka Wing, Lam, Erwin, D'Anna, Vincenza, Allouche, Florian, Michel, Carine, Safonova, Olga V, Sautet, Philippe, and Copéret, Christophe

Abstract

In alkene metathesis, while group 6 (Mo or W) high-oxidation state alkylidenes are accepted to be key reaction intermediates for both homogeneous and heterogeneous catalysts, it has been proposed that low valent species in their +4 oxidation state can serve as precatalysts. However, the activation mechanism for these latter species-generating alkylidenes-is still an open question. Here, we report the syntheses of tungsten(IV)-oxo bisalkoxide molecular complexes stabilized by pyridine ligands, WO(OR)2py3 (R = CMe(CF3)2 (2a), R = Si(O tBu)3 (2b), and R = C(CF3)3 (2c); py = pyridine), and show that upon activation with B(C6F5)3 they display alkene metathesis activities comparable to W(VI)-oxo alkylidenes. The initiation mechanism is examined by kinetic, isotope labeling and computational studies. Experimental evidence reveals that the presence of an allylic CH group in the alkene reactant is crucial for initiating alkene metathesis. Deuterium labeling of the allylic C-H group shows a primary kinetic isotope effect on the rate of initiation. DFT calculations support the formation of an allyl hydride intermediate via activation of the allylic C-H bond and show that formation of the metallacyclobutane from the allyl "hydride" involves a proton transfer facilitated by the coordination of a Lewis acid (B(C6F5)3) and assisted by a Lewis base (pyridine). This proton transfer step is rate determining and yields the metathesis active species.

Published
2018

146. DFT investigations for the catalytic reaction mechanism of methane combustion occurring on Pd(ii)/Al-MCM-41.

Author

Gannouni, Anis, Gannouni, Anis, Michel, Carine, Delbecq, Françoise, Zina, Mongia Saïd, Sautet, Philippe, Gannouni, Anis, Gannouni, Anis, Michel, Carine, Delbecq, Françoise, Zina, Mongia Saïd, and Sautet, Philippe

Abstract

In this work, a theoretical analysis was carried out on the mechanism of methane combustion occurring on single site palladium oxide species [Pd]2+ supported on Al-MCM-41 silica. Single site Pd-oxo and PdO2-superoxo structures were used to represent the active centers. Activation energies for all the elementary steps involved in the oxidation of methane into formaldehyde are presented. The competition of methane/methanol substrates on active sites was examined. It was found that the formation of methanol via the reaction of methane with the superoxo species, formed via the adsorption of O2 on reduced Pd(ii) centers, facilitates the production of the very active Pd-oxo catalytic sites.

Published
2018

147. Force Field for Water over Pt(111): Development, Assessment, and Comparison.

Author

Steinmann, Stephan N, Steinmann, Stephan N, Ferreira De Morais, Rodrigo, Götz, Andreas W, Fleurat-Lessard, Paul, Iannuzzi, Marcella, Sautet, Philippe, Michel, Carine, Steinmann, Stephan N, Steinmann, Stephan N, Ferreira De Morais, Rodrigo, Götz, Andreas W, Fleurat-Lessard, Paul, Iannuzzi, Marcella, Sautet, Philippe, and Michel, Carine

Abstract

Metal/water interfaces are key in many natural and industrial processes, such as corrosion, atmospheric, or environmental chemistry. Even today, the only practical approach to simulate large interfaces between a metal and water is to perform force-field simulations. In this work, we propose a novel force field, GAL17, to describe the interaction of water and a Pt(111) surface. GAL17 builds on three terms: (i) a standard Lennard-Jones potential for the bonding interaction between the surface and water, (ii) a Gaussian term to improve the surface corrugation, and (iii) two terms describing the angular dependence of the interaction energy. The 12 parameters of this force field are fitted against a set of 210 adsorption geometries of water on Pt(111). The performance of GAL17 is compared to several other approaches that have not been validated against extensive first-principles computations yet. Their respective accuracy is evaluated on an extended set of 802 adsorption geometries of H2O on Pt(111), 52 geometries derived from icelike layers, and an MD simulation of an interface between a c(4 × 6) Pt(111) surface and a water layer of 14 Å thickness. The newly developed GAL17 force field provides a significant improvement over previously existing force fields for Pt(111)/H2O interactions. Its well-balanced performance suggests that it is an ideal candidate to generate relevant geometries for the metal/water interface, paving the way to a representative sampling of the equilibrium distribution at the interface and to predict solvation free energies at the solid/liquid interface.

Published
2018

148. Direct n-octanol amination by ammonia on supported Ni and Pd catalysts: activity is enhanced by 'spectator' ammonia adsorbates

Author

Dumon, Alexandre S, Dumon, Alexandre S, Wang, Tao, Ibanez, Javier, Tomer, Ajay, Yan, Zhen, Wischert, Raphael, Sautet, Philippe, Pera-Titus, Marc, Michel, Carine, Dumon, Alexandre S, Dumon, Alexandre S, Wang, Tao, Ibanez, Javier, Tomer, Ajay, Yan, Zhen, Wischert, Raphael, Sautet, Philippe, Pera-Titus, Marc, and Michel, Carine

Abstract

DFT calculations highlight the role of co-adsorbed ammonia in catalytic activity in the amination of alcohols by ammonia.

Published
2018

150. Supported gold-nickel nano-alloy as a highly efficient catalyst in levulinic acid hydrogenation with formic acid as an internal hydrogen source

Author

Ruppert, Agnieszka M, Ruppert, Agnieszka M, Jedrzejczyk, Marcin, Potrzebowska, Natalia, Kazmierczak, Kamila, Brzezinska, Magdalena, Sneka-Platek, Olga, Sautet, Philippe, Keller, Nicolas, Michel, Carine, Grams, Jacek, Ruppert, Agnieszka M, Ruppert, Agnieszka M, Jedrzejczyk, Marcin, Potrzebowska, Natalia, Kazmierczak, Kamila, Brzezinska, Magdalena, Sneka-Platek, Olga, Sautet, Philippe, Keller, Nicolas, Michel, Carine, and Grams, Jacek

Abstract

The surface Au–Ni nano-alloy was very efficiently used for the first time for the hydrogenation of levulinic acid with formic acid as an internal hydrogen source.

Published
2018

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