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6. Probing the Core and Surface Composition of Base-Metal Nanoalloys to Rationalize their Selectivity: The Case of Ni-Fe/SiO 2 Catalysts for the Liquid-Phase Hydrogenation of Furfural

Author

Shi, Dichao, Sadier, Achraf, Girardon, Jean-Sébastien, Mamede, Anne-Sophie, Ciotonea, Carmen, Marinova, Maya, Stievano, Lorenzo, Sougrati, Moulay, La Fontaine, Camille, Paul, Sébastien, Wojcieszak, Robert, Marceau, Eric, 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), Unité Matériaux et Transformations - UMR 8207 (UMET), 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), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Montpellier (UM), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), and ANR-17-CE07-0022,NobleFreeCat,Nanoparticules bimétalliques sans métal noble pour l'hydrogénation des sucres(2017)

Subjects
selectivity, core-shell structure, bimetallic catalysts, LEIS, furfural, [CHIM.CATA]Chemical Sciences/Catalysis, furfuryl alcohol
Abstract

International audience; Bimetallic catalysis for conversion of bio-sourced molecules has often relied on noble metals that should be replaced in the near future by the association of cheaper and more abundant base metals, also known by a poor Z-contrast, which makes in-depth characterization of these systems challenging. However, determining the distribution of base metals in bimetallic nanoparticles is of paramount importance if one wants to rationalize their selectivity. Besides demonstrating that, despite their oxidable character, Ni-Fe catalysts are stable systems for liquid-phase hydroconversion of furfural, this study demonstrates that heterogeneities in the structure of reduced Ni-Fe nanoparticles are key to understanding their catalytic properties, provides a characterization methodology to discriminate between their surface and core compositions, and determines an adequate balance between the two metals that allows tuning the relative rates of the various reaction pathways and, thus, the selectivity.

Published
2022

7. Mn- or Cu- substituted LaFeO3-based three-way catalysts: Highlighting different catalytically operating modes of La0.67Fe0.8M0.2O3 (M=Cu, Mn)

Author

Nandi, Shreya, primary, Wu, Jiang Xiang, additional, Simon, Pardis, additional, Nuns, Nicolas, additional, Trentesaux, Martine, additional, Tougerti, Asma, additional, Fonda, Emiliano, additional, Girardon, Jean-Sébastien, additional, Paul, Jean-François, additional, Mamede, Anne-Sophie, additional, and Berrier, Elise, additional

Published
2021
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8. Mn- or Cu- substituted LaFeO 3 -based three-way catalysts: Highlighting different catalytically operating modes of La 0.67 Fe 0.8 M 0.2 O 3 (M=Cu, Mn)

Author

Nandi, Shreya, Wu, Jiang Xiang, Simon, Pardis, Nuns, Nicolas, Trentesaux, Martine, Tougerti, Asma, Fonda, Emiliano, Girardon, Jean-Sébastien, Paul, Jean-François, Mamede, Anne-Sophie, Berrier, Elise, 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, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), and Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)

Subjects
Raman spectroscopy, XPS, Three-way catalysis, Operando, [CHIM.CATA]Chemical Sciences/Catalysis, Perovskite
Abstract

International audience; The present work aims at presenting our investigations on the redox behaviour of Cu-or Mndoped LaFeO 3-based perovskite powders under three-way catalysis (TWC) relevant conditions. Two distinct La-deficient catalysts of generic formula La 0.67 Fe 0.8 Mn 0.2 O 3 and La 0.67 Fe 0.8 Cu 0.2 O 3 denoted as Mn-dLFO and Cu-dLFO, respectively, were prepared based on the conventional citrate complexation route and systematically investigated using complementary characterisation techniques. This study has made it possible to highlight fundamentally different structures. In Cu-dLFO, most Cu 2+ cations are expelled from the LaFeO 3 perovskite lattice in the form of a segregated CuO phase. On the other hand, in the case of Mn-dLFO, majority of Mn 3+ cations are stabilised within the perovskite solid solution, while substantial iron exsolution in the form of an additional α-Fe 2 O 3 phase was evidenced. The evolution of both catalysts during CO-TPR using operando Raman revealed the formation of polycyclic aromatic hydrocarbons (PAHs) besides the relative structural stability of the LaFeO 3 lattice. The reduction of Mn 3+ to Mn 2+ , indirectly suggested by Raman analysis, is further supported by a quasi-in situ XPS study. The latter also evidenced the reduction of CuO to metal copper to a large extent in Cu-dLFO. In addition, a share of the α-Fe 2 O 3 phase present in Mn-dLFO is reduced to metal Fe 0 during CO oxidation, and is fully re-oxidised upon NO reduction. Our investigation thus evidences that both copper and manganese sites in Cu-dLFO and Mn-dLFO, respectively, are redox-active centres upon CO oxidation / NO reduction with, however, varying operating modes underpinned by their fundamentally different structures.

Published
2021

10. From a Sequential Chemo-Enzymatic Approach to a Continuous Process for HMF Production from Glucose

Author

Gimbernat, Alexandra, Guehl, Marie, Ferreira, Nicolas Lopes, Heuson, Egon, Dhulster, Pascal, Capron, Mickael, Dumeignil, Franck, Delcroix, Damien, Girardon, Jean Sébastien, Froidevaux, Rénato, Institut Charles Viollette (ICV) - EA 7394 (ICV), Université du Littoral Côte d'Opale (ULCO)-Université de Lille-Institut National de la Recherche Agronomique (INRA)-Université d'Artois (UA)-Institut Supérieur d'Agriculture, 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, IFP Energies nouvelles (IFPEN), This research was funded by IFP Energies nouvelles for funding these studies. Chevreul Institute (FR 2638), Ministère de l’Enseignement Supérieur et de la Recherche, Région Hauts-de-France (CPER ALIBIOTECH), REALCAT platform (‘Future Investments’ program (PIA), with the contractual reference ‘ANR-11-EQPX-0037′) and FEDER are acknowledged for supporting and funding partially this work., ANR-11-EQPX-0037,REALCAT,Plateforme intégREe AppLiquée au criblage haut débit de CATalyseurs pour les bioraffineries(2011), Université d'Artois (UA)-Institut National de la Recherche Agronomique (INRA)-Université du Littoral Côte d'Opale (ULCO)-Institut Supérieur d'Agriculture-Université de Lille, Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), ENSCL, Université de Lille, CNRS, INRA, ISA, Centrale Lille, Univ. Artois, Univ. Littoral Côte d’Opale, Institut Charles Viollette (ICV) - EA 7394 [ICV], Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS], IFP Energies nouvelles [IFPEN], Unité de Catalyse et de Chimie du Solide - UMR 8181 (UCCS), Université d'Artois (UA)-Ecole Centrale de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), and ANR-11-EQPX-0037/11-EQPX-0037,REALCAT,Plateforme intégREe AppLiquée au criblage haut débit de CATalyseurs pour les bioraffineries(2011)

Subjects
chemo-enzymatic catalysis, biomass, 5-hydroxymethylfurfural (HMF), lcsh:Chemical technology, lcsh:Chemistry, lcsh:QD1-999, [CHIM]Chemical Sciences, lcsh:TP1-1185, (bio) catalysis, glucose, chemo‐enzymatic catalysis, HMF, (bio)catalysis
Abstract

International audience; Notably available from the cellulose contained in lignocellulosic biomass, glucose is a highly attractive substrate for eco-efficient processes towards high-value chemicals. A recent strategy for biomass valorization consists on combining biocatalysis and chemocatalysis to realise the so-called chemo-enzymatic or hybrid catalysis. Optimisation of the glucose conversion to 5-hydroxymethylfurfural (HMF) is the object of many research efforts. HMF can be produced by chemo-catalyzed fructose dehydration, while fructose can be selectively obtained from enzymatic glucose isomerization. Despite recent advances in HMF production, a fully integrated efficient process remains to be demonstrated. Our innovative approach consists on a continuous process involving enzymatic glucose isomerization, selective arylboronic-acid mediated fructose complexation/transportation, and chemical fructose dehydration to HMF. We designed a novel reactor based on two aqueous phases dynamically connected via an organic liquid membrane, which enabled substantial enhancement of glucose conversion (70%) while avoiding intermediate separation steps. Furthermore, in the as-combined steps, the use of an immobilized glucose isomerase and an acidic resin facilitates catalyst recycling

Published
2018

11. Bimetallic Fe-Ni/SiO2 catalysts for furfural hydrogenation: Identification of the interplay between Fe and Ni during deposition-precipitation and thermal treatments

Author

Shi, Dichao, primary, Yang, Qifeng, additional, Peterson, Christi, additional, Lamic-Humblot, Anne-Félicie, additional, Girardon, Jean-Sébastien, additional, Griboval-Constant, Anne, additional, Stievano, Lorenzo, additional, Sougrati, Moulay T., additional, Briois, Valérie, additional, Bagot, Paul A.J., additional, Wojcieszak, Robert, additional, Paul, Sébastien, additional, and Marceau, Eric, additional

Published
2019
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13. GECat 2015

Author

Louis, Benoît, Fongarland, Pascal, Marie, Olivier, Petitjean, Hugo, Chizallet, Céline, Borremans, Didier, Marques, Rui, Fontaine, Céline, Onfroy, Thomas, Girardon, Jean-Sébastien, Institut de Chimie de Strasbourg, Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), 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), Normandie Université (NU), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), IFP Energies nouvelles (IFPEN), Total Research & Technology Center Feluy, TOTAL S.A., RHODIA Research & Technologies, RHODIA, Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Poitiers-Institut de Chimie du CNRS (INC), Laboratoire de Réactivité de Surface (LRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Université de Poitiers-Institut national des sciences de l'Univers (INSU - CNRS)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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
2017

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