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1. REALCAT: A New Platform to Bring Catalysis to the Lightspeed

Author

Paul Sébastien, Heyte Svetlana, Katryniok Benjamin, Garcia-Sancho Cristina, Maireles-Torres Pedro, and Dumeignil Franck

Subjects
Chemical technology, TP1-1185, Energy industries. Energy policy. Fuel trade, HD9502-9502.5
Abstract

Catalysis, irrespective of its form can be considered as one of the most important pillars of today’s chemical industry. The development of new catalysts with improved performances is therefore a highly strategic issue. However, the a priori theoretical design of the best catalyst for a desired reaction is not yet possible and a time- and money-consuming experimental phase is still needed to develop a new catalyst for a given reaction. The REALCAT platform described in this paper consists in a complete, unique, integrated and top-level high-throughput technologies workflow that allows a significant acceleration of this kind of research. This is illustrated by some preliminary results of optimization of the operating conditions of glycerol dehydration to acrolein over an heteropolyacid-based supported catalyst. It is shown that using REALCAT high-throughput tools a more than 10-fold acceleration of the operating conditions optimization process is obtained.

Published
2015
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4. Direct Synthesis of Dimethyl Carbonate from Methanol and CO 2 over ZrO 2 Catalysts Combined with a Dehydrating Agent and a Cocatalyst.

Author

Shi, Dichao, Heyte, Svetlana, Capron, Mickaël, and Paul, Sébastien

Abstract

Zirconia nanocrystals as catalysts for the direct synthesis of dimethyl carbonate (DMC) from methanol and carbon dioxide have received significant interest recently. In this paper, three zirconia-based catalysts presenting different monoclinic and tetragonal phase contents are prepared and characterized by X-ray diffraction (XRD), N2 adsorption–desorption, transmission electron microscopy (TEM), and temperature-programmed desorption of NH3 and CO2 (NH3-TPD and CO2-TPD). The catalytic performances of these solids are evaluated in terms of DMC production. This production is low when using the bare zirconias, but it is significantly increased in the presence of 1,1,1-trimethoxymethane (TMM) playing the role of a dehydrating agent, which shifts the thermodynamic equilibrium. Moreover, the production of DMC is further improved by adding a second solid catalyst (cocatalyst), the molecular sieve 13X, to accelerate the hydration of TMM. Hence, the molecular sieve 13X plays a dual role by trapping water molecules formed by the reaction of DMC synthesis and providing strong acidic sites catalyzing TMM hydrolysis. To the best of our knowledge, the combination of two solid catalysts in the reaction medium to accelerate the water elimination to obtain higher DMC production from CO2 and methanol has never been reported. [ABSTRACT FROM AUTHOR]

Published
2024
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7. Supported Gold Catalysts for Base-Free Furfural Oxidation: The State of the Art and Machine-Learning-Enabled Optimization

Author

Thuriot-Roukos, Joëlle, primary, Ferraz, Camila Palombo, additional, K. Al Rawas, Hisham, additional, Heyte, Svetlana, additional, Paul, Sébastien, additional, Itabaiana Jr, Ivaldo, additional, Pietrowski, Mariusz, additional, Zieliński, Michal, additional, Ghazzal, Mohammed N., additional, Dumeignil, Franck, additional, and Wojcieszak, Robert, additional

Published
2023
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10. Combined theoretical and experimental kinetic approach for methane conversion on model supported Pd/La0.7MnO3 NGV catalyst: Sensitivity to inlet gas composition and consequence on the Pd-support interface

Author

Zheng, Yuanshuang, primary, Decoster, Amaury, additional, Osti, Andrea, additional, Glisenti, Antonella, additional, Dacquin, Jean-Philippe, additional, Dhainaut, Fabien, additional, Heyte, Svetlana, additional, and Granger, Pascal, additional

Published
2022
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11. Versatility of Supported Gold Nanoparticles on Hydrotalcites used for Oxidation and Reduction Reactions

Author

Drault, Fabien, Snoussi, Youssef, Ferraz, Camila, Thuriot-Roukos, Joelle, Heyte, Svetlana, Junior, Ivaldo, Marinova, Maya, Paul, Sébastien, Wojcieszak, Robert, Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS), Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Universidade Federal do Rio de Janeiro (UFRJ), Institut Michel Eugène Chevreul - FR 2638 (IMEC), and Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)

Subjects
catalysis, oxidation, CO 2, Gold nanoparticles, reduction, furfural, [CHIM.CATA]Chemical Sciences/Catalysis
Abstract

Regardless of their size, supported gold nanoparticles are largely used for liquid-phase oxidation reactions. Small gold nanoparticles exhibit good performance during the reduction of organic compounds. The direct reduction of carboxylic acid to aldehyde is a famous and familiar reaction in the field of organic chemistry and is considered as one of the fundamental chemical transformations. Herein, we present Au/hydrotalcite, Au/MgO, and Au/Al2O3 systems as heterogeneous versatile catalysts to realize the oxidation of furfural (FF) to furoic acid (FA) and realize the reduction of FA to FF. Experiments showed that in standard aqueous conditions under air, FF can be easily oxidized to FA. When DMSO was used as a solvent to conduct the experiments under an atmosphere of CO2, FA was reduced to FF. The Au/HT series of catalysts was found to be active in both transformations, pointing out the versatility of the gold-based catalysts. The activity significantly depends on the acid-base properties of the catalyst.

Published
2022

13. Performance of Cu/ZnO Nanosheets on Electrospun Al 2 O 3 Nanofibers in CO 2 Catalytic Hydrogenation to Methanol and Dimethyl Ether.

Author

Maor, Itzhak I., Heyte, Svetlana, Elishav, Oren, Mann-Lahav, Meirav, Thuriot-Roukos, Joelle, Paul, Sébastien, and Grader, Gideon S.

Subjects
*METHYL ether, *ALUMINUM oxide, *COPPER, *CATALYTIC hydrogenation, *CARBON dioxide, *NANOFIBERS
Abstract

The synthesis of methanol and dimethyl ether (DME) from carbon dioxide (CO2) and green hydrogen (H2) offers a sustainable pathway to convert CO2 emissions into value-added products. This heterogeneous catalytic reaction often uses copper (Cu) catalysts due to their low cost compared with their noble metal analogs. Nevertheless, improving the activity and selectivity of these Cu catalysts for these products is highly desirable. In the present study, a new architecture of Cu- and Cu/Zn-based catalysts supported on electrospun alumina nanofibers were synthesized. The catalysts were tested under various reaction conditions using high-throughput equipment to highlight the role of the hierarchical fibrous structure on the reaction activity and selectivity. The Cu or Cu/ZnO formed a unique structure of nanosheets, covering the alumina fiber surface. This exceptional morphology provides a large surface area, up to ~300 m2/g, accessible for reaction. Maximal production of methanol (~1106 gmethanolKgCu−1∙h−1) and DME (760 gDMEKgCu−1∙h−1) were obtained for catalysts containing 7% wt. Cu/Zn with a weight ratio of 2.3 Zn to Cu (at 300 °C, 50 bar). The promising results in CO2 hydrogenation to methanol and DME obtained here point out the significant advantage of nanofiber-based catalysts in heterogeneous catalysis. [ABSTRACT FROM AUTHOR]

Published
2023
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16. Carbon-based catalysts for Fischer–Tropsch synthesis

Author

Ordomsky, Vitaly, Wang, Qiyan, Zhou, Wen-Juan, Heyte, Svetlana, Thuriot-Roukos, Joëlle, Marinova, Maya, Addad, Ahmed, Rouzière, Stéphan, Simon, Pardis, Capron, Mickael, Zhang, Linjie, Grimaud, Alexis, Schwiedernoch, Renate, Hernández, Willinton Yesid, Naghavi, Negar, Pedrolo, Débora, Schwaab, Marcio, Marcilio, Nilson, Khodakov, Andrei, Santos, Sara, Urbina-Blanco, César, Zhou, Wenjuan, Yang, Yong, Joelle, Thuriot-Roukos, Ersen, Ovidiu, Baaziz, Walid, Safonova, Olga, Saeys, Mark, Gu, Bang, Peron, Deizi, Barrios, Alan, Virginie, Mirella, La Fontaine, Camille, Briois, Valérie, Vorokhta, Mykhailo, Šmíd, Břetislav, Moldovan, Simona, Koneti, Siddardha, Gambu, Thobani, Hernández, Willinton, Impéror-Clerc, Marianne, Vovk, Evgeny, Wu, Dan, Nuns, Nicolas, Palčić, Ana, Jaén, Sara Navarro, Cai, Mengdie, Liu, Chong, Pidko, Evgeny, Valtchev, Valentin, Yan, Zhen, Zhang, Songwei, Li, Jerry Pui Ho, Zhao, Jingpeng, Yuan, Biao, He, Tao, Yu, Yi, Li, Tao, Hu, Di, Chen, Yanping, Wei, Jiatong, Duyar, Melis, Liu, Jian, Dalian Institute of Chemical Physics - Chinese Academy of Sciences, University of Surrey (UNIS), Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS), Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), ANR-16-CE06-0013,NANO4FuT,Synthèse des carburants alternatifs et des molécules plateforme sur nanoréacteurs(2016), CNRS, Centrale Lille, ENSCL, Univ. Artois, Université de Lille, Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181, Ordomsky, Vitaly, Centrale Lille Institut (CLIL)-Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille, Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, 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 Michel Eugène Chevreul - FR 2638 (IMEC), Université d'Artois (UA)-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Centrale Lille Institut (CLIL), Unité Matériaux et Transformations - UMR 8207 (UMET), Institut de Chimie du CNRS (INC)-Institut National de la Recherche Agronomique (INRA)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL), Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Chimie du solide et de l'énergie (CSE), Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Solvay (France), Instituto Federal do Rio Grande do Sul (IFRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), 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)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), 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), Paul Scherrer Institute (PSI), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Charles University [Prague] (CU), Groupe de physique des matériaux (GPM), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Ruđer Bošković Institute (IRB), Delft University of Technology (TU Delft), Laboratoire catalyse et spectrochimie (LCS), Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Université de Caen Normandie (UNICAEN), ShanghaiTech University [Shanghai], Beihang University (BUAA), School of Physics Science and Engineering, Tongji University, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-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)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-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)-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 d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille, Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Centre National de la Recherche Scientifique (CNRS)-Collège de France (CdF (institution))-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)

Subjects
Materials science, chemistry.chemical_element, 02 engineering and technology, Carbon nanotube, 010402 general chemistry, 01 natural sciences, 7. Clean energy, law.invention, Catalysis, law, [CHIM] Chemical Sciences, medicine, [CHIM]Chemical Sciences, Coal, Gasoline, Carbon nanofiber, business.industry, Fischer–Tropsch process, General Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, chemistry, 0210 nano-technology, business, Carbon, Activated carbon, medicine.drug
Abstract

International audience; Fischer-Tropsch synthesis (FTS) is an essential approach to convert coal, biomass, and shale gas into fuels and chemicals, such as lower olefins, gasoline, diesel, and so on. In recent years, there has been increasing motivation to deploy FTS at commercial scales which has been boosting the discovery of high performance catalysts. In particular, the importance of support in modulating the activity of metals has been recognized and carbonaceous materials have attracted attention as supports for FTS. In this review, we summarised the substantial progress in the preparation of carbon-based catalysts for FTS by applying activated carbon (AC), carbon nanotubes (CNTs), carbon nanofibers (CNFs), carbon spheres (CSs), and metal-organic frameworks (MOFs) derived carbonaceous materials as supports. A general assessment of carbon-based catalysts for FTS, concerning the support and metal properties, activity and products selectivity, and their interactions is systematically discussed. Finally, current challenges and future trends in the development of carbon-based catalysts for commercial utilization in FTS are proposed.

Published
2021

20. Catalytic processes for the direct synthesis of dimethyl carbonate from CO2 and methanol: a review.

Author

Shi, Dichao, Heyte, Svetlana, Capron, Mickaël, and Paul, Sébastien

Subjects
*DRYING agents, *METAL-organic frameworks, *METAL catalysts, *MOLECULAR sieves, *ETHANES, *METHANOL as fuel
Abstract

The direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol has recently attracted much attention because such a process would allow the application of green chemistry principles. However, its major drawbacks lie in the high stability of CO2 and in the thermodynamic equilibrium of the reaction. The present review aims to discuss strategies that have been explored by researchers recently to improve the yield of DMC. Elaborate catalysts for the activation of CO2 and methanol, such as organometallic catalysts, ionic liquids, alkali metal catalysts, heteropolyacid catalysts, metal-supported catalysts, metal organic frameworks (MOFs) and metal oxide catalysts, are summarized and discussed in this review paper. Moreover, the significance of using a dehydrating agent for in situ water trapping during the reaction (and concomitant thermodynamic equilibrium shift), such as molecular sieves, ionic liquids, acetals, esters and nitriles, is also considered and the detailed roles of dehydrating agents in the formation of DMC are analyzed in this review. [ABSTRACT FROM AUTHOR]

Published
2022
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21. Influence of the structure of trigonal Mo-V-M3rd oxides (M3rd = -, Fe, Cu, W) on catalytic performances in selective oxidations of ethane, acrolein, and allyl alcohol

Author

Ishikawa, Satoshi, primary, Murayama, Toru, additional, Katryniok, Benjamin, additional, Dumeignil, Franck, additional, Araque, Marcia, additional, Heyte, Svetlana, additional, Paul, Sébastien, additional, Yamada, Yudai, additional, Iwazaki, Mizuki, additional, Noda, Nagisa, additional, and Ueda, Wataru, additional

Published
2019
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22. Ruthenium‐Catalyzed Coupling Reactions of CO2 with C2H4 and Hydrosilanes towards Silyl Esters.

Author

Kunihiro, Kana, Heyte, Svetlana, Paul, Sébastien, Roisnel, Thierry, Carpentier, Jean‐François, and Kirillov, Evgueni

Subjects
*CARBOXYLATION, *ESTERS, *TURNOVER frequency (Catalysis), *CARBON dioxide fixation, *BATCH reactors, *PHOSPHINES
Abstract

A series of in situ‐prepared catalytic systems incorporating RuII precursors and bidentate phosphine ligands has been probed in the reductive carboxylation of ethylene in the presence of triethylsilane as reductant. The catalytic production of propionate and acrylate silyl esters was evidenced by high‐throughput screening (HTS) and implemented in batch reactor techniques. The most promising catalyst systems identified were made of Ru(H)(Cl)(CO)(PPh3)3 and 1,4‐bis(dicyclohexylphosphino)butane (DCPB) or 1,1'‐ferrocene‐diyl‐bis(cyclohexylphosphine) (DCPF). A marked influence of water on the acrylate/propionate selectivity was noted. Turnover numbers [mol mol(Ru)−1] up to 16 for acrylate and up to 68 for propionate were reached under relatively mild conditions (20 bar, 100 °C, 0.5 mol % Ru, 40 mol % H2O vs. HSiEt3). Possible mechanisms are discussed. [ABSTRACT FROM AUTHOR]

Published
2021
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24. Role of Crystalline Structure in Allyl Alcohol Selective Oxidation over Mo3VO                            x                          Complex Metal Oxide Catalysts

Author

Murayama, Toru, Katryniok, Benjamin, Heyte, Svetlana, Araque, Marcia, Ishikawa, Satoshi, Dumeignil, Franck, Paul, Sébastien, Ueda, Wataru, Hokkaido University [Sapporo, Japan], Tokyo Metropolitan University [Tokyo] (TMU), Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS), Centrale Lille Institut (CLIL)-Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille, Kanagawa University, Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), and Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.CATA]Chemical Sciences/Catalysis, ComputingMilieux_MISCELLANEOUS
Abstract

International audience

Published
2016

28. REALCAT: A new platform to bring catalysis to the lightspeed

Author

Centrale Lille, Université Lille 2 Droit et Santé, European Commission, Agence Nationale de la Recherche (France), Paul, Sèbastien, Heyte, Svetlana, Katryniok, Benjamin, García Sancho, Cristina, Maireles-Torres, Pedro, Dumeignil, F., Centrale Lille, Université Lille 2 Droit et Santé, European Commission, Agence Nationale de la Recherche (France), Paul, Sèbastien, Heyte, Svetlana, Katryniok, Benjamin, García Sancho, Cristina, Maireles-Torres, Pedro, and Dumeignil, F.

Abstract

[EN]: Catalysis, irrespective of its form can be considered as one of the most important pillars of today’s chemical industry. The development of new catalysts with improved performances is therefore a highly strategic issue. However, the a priori theoretical design of the best catalyst for a desired reaction is not yet possible and a time- and money-consuming experimental phase is still needed to develop a new catalyst for a given reaction. The REALCAT platform described in this paper consists in a complete, unique, integrated and top-level high-throughput technologies workflow that allows a significant acceleration of this kind of research. This is illustrated by some preliminary results of optimizationof the operating conditions of glycerol dehydration to acrolein over an heteropolyacid-based supported catalyst. It is shown that using REALCAT high-throughput tools a more than 10-fold acceleration of the operating conditions optimization process is obtained., [FR]: La catalyse, quelle que soit sa forme, peut être considérée comme un des plus importants piliers de l’industrie chimique. Le développement de nouveaux catalyseurs aux propriétés catalytiques améliorées est ainsi d’une importance stratégique capitale. À ce jour la catalyse n’est pas une science prédictive et la conception théorique d’un catalyseur pour une réaction donnée n’est pas encore possible et une approche expérimentale consommatrice en temps et en ressource est nécessaire. La plateforme REALCAT décrite dans cet article consiste en un ensemble complet, intégré et unique au monde d’équipements de criblage permettant une accélération significative de la recherche dans le domaine de la catalyse. Un premier exemple d’optimisation des conditions opératoires de la déshydratation du glycérol en acroléine sur catalyseur hétéropolyanionique est donné à titre d’illustration. Il montre que les outils de la plateforme REALCAT permettent de réduire par au moins un facteur 10 le temps d’optimisation des conditions opératoires de la réaction étudiée

Published
2015

30. Role of Crystalline Structure in Allyl Alcohol Selective Oxidation over Mo3VO x Complex Metal Oxide Catalysts.

Author

Murayama, Toru, Katryniok, Benjamin, Heyte, Svetlana, Araque, Marcia, Ishikawa, Satoshi, Dumeignil, Franck, Paul, Sébastien, and Ueda, Wataru

Subjects
CRYSTAL structure, ALLYL alcohol, SELECTIVE catalytic oxidation, METAL catalysts, METALLIC oxides, ACRYLIC acid, ALDEHYDES
Abstract

The role of the crystalline phase of Mo3VO x in the catalytic oxidation of allyl alcohol over four kinds of crystalline (orthorhombic, trigonal, tetragonal, amorphous) Mo3VO x catalysts was investigated to determine the active sites for the reactions. Tetragonal Mo3VO x was found less active for the formation of acrylic acid from allyl alcohol, although acrolein was obtained selectively at higher temperature. For orthorhombic and trigonal Mo3VO x catalyst, allyl alcohol converted to acrolein and propanal competitively at the mouth of the heptagonal channel over the a- b plane of the rod-type crystalline particles, and these aldehydes were oxidized consecutively to acrylic acid. Acrylic acid was formed effectively at increased reaction temperature over orthorhombic, trigonal and amorphous Mo3VO x catalysts, and the maximum yields of acrylic acid were 73 % for the orthorhombic Mo3VO x catalyst and 72 % for the trigonal Mo3VO x catalyst at 350 °C. [ABSTRACT FROM AUTHOR]

Published
2016
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31. The Role of Steric Effects and Acidity in the Direct Synthesis of iso-Paraffins from Syngas on Cobalt Zeolite Catalysts.

Author

Subramanian, Vijayanand, ZholobENko, Vladimir L., ChENg, Kang, Lancelot, Christine, Heyte, Svetlana, Thuriot, Joelle, Paul, SébastiEN, Ordomsky, Vitaly V., and Khodakov, Andrei Y.

Subjects
PARAFFIN wax, SYNTHESIS gas, COBALT compounds, ZEOLITE catalysts, MOLECULAR structure
Abstract

This study focuses on the effects of the localization of Co species, zeolite structure, and acidity on the performance of Co bifunctional catalysts promoted with Pt for the direct synthesis of iso-paraffins from syngas. ZSM-5, MOR, and BEA were chosen as zeolites with different structures and pore diameters. The catalysts were prepared either by incipient wetness impregnation or by the mechanical mixing of the zeolite with a conventional silica-supported Co catalyst. The increase in the pore size and open character of the zeolite structure from ZSM-5 to BEA resulted in a higher fraction of Co located inside the pores of the catalysts prepared by impregnation. The catalytic performance was affected strongly by the zeolite acidity, pore structure, and Co distribution between the pores and the external surface. The selectivity to short-chain iso-paraffins is affected principally by the zeolite acidity, whereas the selectivity to long-chain branched hydrocarbons mostly depends on steric effects. [ABSTRACT FROM AUTHOR]

Published
2016
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32. Ruthenium-Catalyzed Coupling Reactions of CO 2 with C 2 H 4 and Hydrosilanes towards Silyl Esters.

Author

Kunihiro K, Heyte S, Paul S, Roisnel T, Carpentier JF, and Kirillov E

Abstract

A series of in situ-prepared catalytic systems incorporating Ru II precursors and bidentate phosphine ligands has been probed in the reductive carboxylation of ethylene in the presence of triethylsilane as reductant. The catalytic production of propionate and acrylate silyl esters was evidenced by high-throughput screening (HTS) and implemented in batch reactor techniques. The most promising catalyst systems identified were made of Ru(H)(Cl)(CO)(PPh 3 ) 3 and 1,4-bis(dicyclohexylphosphino)butane (DCPB) or 1,1'-ferrocene-diyl-bis(cyclohexylphosphine) (DCPF). A marked influence of water on the acrylate/propionate selectivity was noted. Turnover numbers [mol mol(Ru) -1 ] up to 16 for acrylate and up to 68 for propionate were reached under relatively mild conditions (20 bar, 100 °C, 0.5 mol % Ru, 40 mol % H 2 O vs. HSiEt 3 ). Possible mechanisms are discussed., (© 2021 Wiley-VCH GmbH.)

Published
2021
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