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2 results on '"Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials (LSRE-LCM) Departamento de Tecnologia Quimica e Biologica Escola Superior de Tecnologia e Gestao (LSRE-LCM)"'

1. Control of the single atom/nanoparticle ratio in Pd/C catalysts to optimize the cooperative hydrogenation of alkenes

Author

Camila Rivera‐Cárcamo, Alain Favre-Réguillon, C. de Bellefon, Iann C. Gerber, Boris Guicheret, Régis Philippe, J. Audevard, I. del Rosal, Bruno F. Machado, R. Castro Contreras, Laurent Vanoye, Philippe Serp, Laboratoire de chimie de coordination (LCC), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de physique et chimie des nano-objets (LPCNO), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC), Laboratoire de Génie des Procédés Catalytiques (LGPC), École Supérieure Chimie Physique Électronique de Lyon-Centre National de la Recherche Scientifique (CNRS)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon, Conservatoire National des Arts et Métiers [CNAM] (CNAM), Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials (LSRE-LCM) Departamento de Tecnologia Quimica e Biologica Escola Superior de Tecnologia e Gestao (LSRE-LCM), Instituto Politecnico de Braganca, Fundação para a Ciência e a Tecnologia, CONICYT, Région Auvergne-Rhône-Alpes (contract number 15 021131 01 – CNR006), ANR-19-CE07-0030,COMET,Catalyse Coopérative Entre Atomes Et Nanoparticules Métalliques(2019), 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), 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), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-École Supérieure de Chimie Physique Électronique de Lyon (CPE)-Centre National de la Recherche Scientifique (CNRS), and HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)

Subjects
chemistry.chemical_classification, [CHIM.ORGA]Chemical Sciences/Organic chemistry, Chemistry, Alkene, Inorganic chemistry, Nanoparticle, chemistry.chemical_element, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, Orders of magnitude (numbers), 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Oxygen, Catalysis, 0104 chemical sciences, Hydrogen spillover, 0210 nano-technology, Dispersion (chemistry), Isomerization
Abstract

International audience; We recently reported (R. Castro Contreras, B. Guicheret, B. F. Machado, C. Rivera-Cárcamo, M. A. Curiel Alvarez, B. Valdez Salas, M. Ruttert, T. Placke, A. Favre Réguillon, L. Vanoye, C. de Bellefon, R. Philippe and P. Serp, J. Catal., 2019, 372, 226–244) that a structure/activity correlation exists in Pd/C catalysts for myrcene hydrogenation, which integrates the Pd dispersion, and the surface concentration of oxygen groups and defects of the support. Here, through a combined experimental–theoretical study, we provide an explanation of the influence of these three structural characteristics of Pd/C catalysts for alkene hydrogenation. Highly dispersed Pd nanoparticles (PdNP) are necessary to activate dihydrogen. A high concentration of surface defects on the support is necessary to stabilize Pd single atoms (PdSA), which coexist with PdNP on Pd/C catalysts. A high concentration of oxygenated surface groups is also necessary on the support to allow hydrogen spillover. We demonstrate that such a combination allows cooperative catalysis to operate between PdNP and PdSA that involves the formation of PdSA–H species, which are much more active than PdNP–H for alkene hydrogenation but also isomerization. Importantly, we also report an efficient method to control the ratio between PdSA and PdNP in Pd/C catalysts of similar loadings and show that the control of this ratio allows the development of a new generation of stable and highly active catalysts integrating the ultra-rational use of precious metals in short supply. Indeed, for myrcene hydrogenation, activity variations of several orders of magnitude were measured as a function of the value of this ratio.

Published
2021

2. Role of Nitrogen Doping on the Performance of Carbon Nanotube Catalysts: A Catalytic Wet Peroxide Oxidation Application

Author

Sergio Morales-Torres, José L. Figueiredo, Philippe Serp, Maria Martin-Martinez, Helder Gomes, Adrián M.T. Silva, Bruno F. Machado, Joaquim L. Faria, Rui S. Ribeiro, Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials (LSRE-LCM) Departamento de Tecnologia Quimica e Biologica Escola Superior de Tecnologia e Gestao (LSRE-LCM), Instituto Politecnico de Braganca, Laboratoire de chimie de coordination (LCC), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées, Laboratory of Separation and Reaction Engineering (LSRE), Universidade do Porto, and Faculdade de Engenharia

Subjects
Nitrogen, Inorganic chemistry, Nitrogen doping, chemistry.chemical_element, 02 engineering and technology, Carbon nanotube, 010402 general chemistry, Heterogeneous catalysis, 7. Clean energy, 01 natural sciences, Peroxide, Catalysis, law.invention, Inorganic Chemistry, chemistry.chemical_compound, law, Oxidation, Doping, [CHIM.COOR]Chemical Sciences/Coordination chemistry, Physical and Theoretical Chemistry, Nanotubes, Organic Chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, chemistry, 13. Climate action, Environmental chemistry, 0210 nano-technology
Abstract

International audience; Four magnetic carbon nanotube (CNT) samples (undoped, completely N-doped, and two selectively N-doped) were synthesized by chemical vapor deposition. The materials were tested in the catalytic wet peroxide oxidation (CWPO) of highly concentrated 4-nitrophenol solutions (4-NP, 5 g L−1). Relatively mild operating conditions were considered (atmospheric pressure, T=50 °C, pH 3), using a catalyst load of 2.5 g L−1 and the stoichiometric amount of H2O2 needed for the complete mineralization of 4-NP. N-doping was identified to influence considerably the CWPO performance of the materials. In particular, undoped CNTs, with a moderate hydrophobicity, favor the controllable and efficient decomposition of H2O2 into highly reactive hydroxyl radicals (HO.), thus showing high catalytic activity for 4-NP degradation. On the other hand, the completely N-doped catalyst, fully hydrophilic, favors a quick decomposition of H2O2 into nonreactive O2 and H2O species. The selectively N-doped amphiphilic catalysts, that is, hybrid structures containing undoped sections followed by N-doped ones, provided intermediate results, namely, a higher N content favored H2O2 decomposition towards nonreactive H2O and O2 species, whereas a lower N content resulted in the formation of HO., increasing 4-NP mineralization. Catalyst stability and reusability were also investigated by consecutive CWPO runs.

Published
2016

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