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7 results on '"Alain Favre-Réguillon"'

1. Deactivation of Pd/C catalysts by irreversible loss of hydrogen spillover ability of the carbon support

Author

Laurent Vanoye, Boris Guicheret, Camila Rivera-Cárcamo, Jérémy Audevard, Javier Navarro-Ruiz, Iker del Rosal, Iann C. Gerber, Cristian H. Campos, Bruno Fernandes Machado, Jérôme Volkman, Régis Philippe, Philippe Serp, Alain Favre-Réguillon, Catalyse, Polymérisation, Procédés et Matériaux (CP2M), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École Supérieure de Chimie Physique Électronique de Lyon (CPE)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de chimie de coordination (LCC), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de physique et chimie des nano-objets (LPCNO), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Fédération de recherche « Matière et interactions » (FeRMI), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Universidad de Concepción - University of Concepcion [Chile], Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials (LSRE-LCM), Faculdade de Engenharia (LSRE-LCM), Universidade do Porto = University of Porto, Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), and ANR-19-CE07-0030,COMET,Catalyse Coopérative Entre Atomes Et Nanoparticules Métalliques(2019)

Subjects
[CHIM]Chemical Sciences, [CHIM.CATA]Chemical Sciences/Catalysis, Physical and Theoretical Chemistry, Catalysis
Abstract

International audience; General interest in solvent-free catalytic processes is driven by the development of environmentally and economically acceptable procedures. Such processes require the use of highly active and stable catalysts. This study reports on the synthesis, characterization, and kinetic evaluation of two highly active Pd catalysts supported on different carbons support, i.e., multi-walled carbon nanotubes (CNT) and few-layer graphene (FLG). These catalysts, with similar Pd loading (∼2 wt%) and containing both Pd single atoms (PdSA) and nanoparticles (PdNP), were systematically tested for solvent-free total hydrogenation of squalene (SQE) to obtain high-purity squalane (SQA). Thanks to the unique cooperative catalysis between PdSA and PdNP involving H-spillover, the activities of both catalysts were high compared to catalysts described in the literature. Solvent-free total hydrogenation of SQE could be performed under mild conditions (120 °C, 20 bar H2, 4 h) using ultralow Pd loading (60 ppm). However, since this reduction reaction is highly exothermic (ΔHR= − 765 kJ.mol−1), heat management during the reactor operation with these highly active catalysts is crucial to avoid deactivation and thermal runaway. Under these conditions, Pd/FLG was highly active but deactivated, unlike Pd/CNT, which still has high activity, but does not deactivate. Characterizations (ICP, XPS, Raman, TPD-MS, HAADF-STEM) of the Pd/FLG catalyst before and after reaction, supported by calculations based on density functional theory, allowed us to propose a new mechanism of catalyst deactivation involving the chemical reduction of specific surface oxygen groups of the carbon support induced by H-spillover.

Published
2023

2. Selective aerobic oxidation of aliphatic aldehydes: the critical role of percarboxylate anion on the selectivity

Author

Laurent Vanoye and Alain Favre-Réguillon

Subjects
Fluid Flow and Transfer Processes, Chemistry (miscellaneous), Process Chemistry and Technology, Chemical Engineering (miscellaneous), Catalysis
Abstract

During the aerobic oxidation of aldehydes, peracids accumulate in the reaction mixture and may be decomposed in a non-selective way during workup. Using carboxylate salts, the peracids are selectively transformed into the carboxylic acids in situ.

Published
2023

4. Adjustment of the Single Atom/Nanoparticle Ratio in Pd/CNT Catalysts for Phenylacetylene Selective Hydrogenation

Author

Jérémy Audevard, Javier Navarro‐Ruiz, Vincent Bernardin, Yann Tison, Anna Corrias, Iker Del Rosal, Alain Favre‐Réguillon, Régis Philippe, Iann C. Gerber, Philippe Serp, Laboratoire de chimie de coordination (LCC), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de physique et chimie des nano-objets (LPCNO), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Fédération de recherche « Matière et interactions » (FeRMI), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Catalyse, Polymérisation, Procédés et Matériaux (CP2M), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École Supérieure de Chimie Physique Électronique de Lyon (CPE)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM), Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), University of Kent [Canterbury], Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), and ANR-19-CE07-0030,COMET,Catalyse Coopérative Entre Atomes Et Nanoparticules Métalliques(2019)

Subjects
Inorganic Chemistry, Organic Chemistry, Nanoparticles, [CHIM]Chemical Sciences, Hydrogenation, [CHIM.CATA]Chemical Sciences/Catalysis, Physical and Theoretical Chemistry, Catalysis, Palladium, Carbon, Hydrogen
Abstract

International audience; Pd/C catalysts are widely used for hydrogenation reactions in the chemical industry. One of the reasons for their high activity is the ability of Pd nanoparticles (PdNP) to dissociate H2 and promote H-spillover. Nevertheless, for selective hydrogenation unpromoted Pd/C catalysts show disappointing results. The use of supported Pd single atom (PdSA) catalysts permits to achieve high selectivity. However, PdSA show low activity because they have difficulty in activating H2. A cooperative catalysis between PdNP and PdSA operates for the hydrogenation of alkenes thanks to the H-spillover, which makes it possible to obtain active isolated PdSA−H species. Here, we present experimental and computational results obtained for phenylacetylene hydrogenation on Pd/CNT catalysts showing different PdSA/PdNP ratios. Tuning this ratio allows doubling the activity while reaching high selectivity to styrene at high conversion. DFT calculations suggest that the first coordination sphere of PdSA has a pronounced effect on their reactivity.

Published
2023

5. 'Cocktail'-Type Catalysis for Cinnamaldehyde Hydrogenation

Author

Philippe Serp, Jérémy Audevard, Javier Navarro-Ruiz, Vincent Bernardin, Régis Philippe, Anna Corrias, Yann Tison, Alain Favre-Réguillon, Iker Del Rosal, and Iann C. Gerber

Subjects
History, Polymers and Plastics, Business and International Management, Industrial and Manufacturing Engineering
Published
2023

6. Solvent‐Free Hydrogenation of Squalene Using Parts per Million Levels of Palladium Supported on Carbon Nanotubes: Shift from Batch Reactor to Continuous‐Flow System

Author

Boris Guicheret, Laurent Vanoye, Camila Rivera‐Cárcamo, Claude de Bellefon, Philippe Serp, Régis Philippe, and Alain Favre‐Réguillon

Subjects
Squalene, General Energy, Nanotubes, Carbon, General Chemical Engineering, Solvents, Environmental Chemistry, General Materials Science, Hydrogenation, Catalysis, Palladium
Abstract

The transition from batch catalytic processes to continuous flow processes requires highly active and stable catalysts that still need to be developed. The preparation and characterization of catalysts where palladium single atoms and nanoparticles are simultaneously present on carbon nanotubes were recently reported by us. These catalysts are considerably more active than commercial or previously described catalysts for the liquid phase hydrogenation of terpenes. Herein is shown that under solvent-free conditions, squalene (SQE) could be converted into squalane (SQA,98 %) using only 300 ppm of Pd in less than 1.4 h at 20 bar H

Published
2022

7. Process intensification of the catalytic hydrogenation of squalene using a Pd/CNT catalyst combining nanoparticles and single atoms in a continuous flow reactor

Author

Laurent Vanoye, Boris Guicheret, Camila Rivera-Cárcamo, Ruben Castro Contreras, Claude de Bellefon, Valérie Meille, Philippe Serp, Régis Philippe, Alain Favre-Réguillon, Catalyse, Polymérisation, Procédés et Matériaux (CP2M), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École Supérieure de Chimie Physique Électronique de Lyon (CPE)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de chimie de coordination (LCC), Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Conservatoire National des Arts et Métiers [CNAM] (CNAM), HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM), 'DEEPER' project / Region Auvergne-Rhône-Alpes (contract number 15 021131 01 – CNR006) - 20th FUI call, and ANR-19-CE07-0030,COMET,Catalyse Coopérative Entre Atomes Et Nanoparticules Métalliques(2019)

Subjects
Squalene, Seamless scale-up, [CHIM.GENI]Chemical Sciences/Chemical engineering, [CHIM.ORGA]Chemical Sciences/Organic chemistry, General Chemical Engineering, Structured reactors, Environmental Chemistry, Catalytic hydrogenation, [CHIM.CATA]Chemical Sciences/Catalysis, General Chemistry, Palladium, Carbon nanotube support, Industrial and Manufacturing Engineering
Abstract

International audience; A process intensification study for the full hydrogenation of bio-derived platform molecule squalene (SQE) into squalane (SQA), using commercial heterogeneous Pd catalysts and Pd supported on carbon nanotubes (CNT) is reported. Pd/CNT shows a substantial improvement of the catalytic activity for the total hydrogenation of SQE into SQA thanks to cooperativities between Pd nanoparticles and single atoms simultaneously present on the CNT. However, the stirred reactor's productivity, scalability, and operability are limited by the exothermicity of the reaction (ΔrH = − 765 kJ.mol−1). The implementation of the Pd/CNT catalyst in flow was then studied after coating this catalyst on metallic open cell foams. Using the foam-based milli-reactor's characteristics, including high mass and heat transfer rates and safety, fully reduced SQA (>99 %) was obtained at 180 °C and 30 bar of H2 for a contact time of 1.45 min with a space–time yield of 68 molSQA.molPd−1.min−1. Finally, a scale-up strategy (7 fold) was successfully attempted in a commercially available pilot-scale reactor that meets further seamless scale-up requirements. A production capacity of 2 kg per day using a commercial intensified reactor with a reacting volume of 43.2 mL was obtained under mild conditions (120 °C and 30 bar of H2).

Published
2022

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