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1. Surface molecular imprinting over supported metal catalysts for size-dependent selective hydrogenation reactions

Author

Vitaly V. Ordomsky, Olga V. Safonova, Willinton Y. Hernández, Dan Wu, Ahmed Addad, Andrei Y. Khodakov, Evgeny I. Vovk, Walid Baaziz, Bang Gu, Maya Marinova, Ovidiu Ersen, Nicolas Nuns, Wen-Juan Zhou, 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), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), 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), Institut Michel Eugène Chevreul - FR 2638 (IMEC), 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), Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-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)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, 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)-Centre National de la Recherche Scientifique (CNRS), Paul Scherrer Institute (PSI), 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), 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)-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 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), Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, 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 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), and 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)

Subjects
Steric effects, chemistry.chemical_classification, Chemistry, Process Chemistry and Technology, Bioengineering, 02 engineering and technology, Polymer, 010402 general chemistry, 021001 nanoscience & nanotechnology, Heterogeneous catalysis, 01 natural sciences, Biochemistry, Combinatorial chemistry, Catalysis, 0104 chemical sciences, Adsorption, Molecule, [CHIM]Chemical Sciences, 0210 nano-technology, Selectivity, Molecular imprinting, ComputingMilieux_MISCELLANEOUS
Abstract

Molecular imprinting of polymer matrices enables the creation of template-shaped cavities with high affinity for molecules of given shape and size. Here we introduce a surface molecular imprinting strategy to control the hydrogenation selectivity of various aromatic molecules over a supported palladium catalyst. This strategy involves the sequential adsorption over the metal surface of an aromatic template molecule followed by poisoners, resulting in the formation of non-poisoned active islands of predetermined shape and size. Because of steric constraints, these active islands exhibit high selectivity in the chemical conversion of aromatic molecules that correspond in size and shape to the templates. The elaborated strategy enables a practical application relevant to selective hydrogenation and removal of carcinogenic benzene from mixtures of aromatics. Molecular imprinting can facilitate size- and shape-selective reactions beyond traditional approaches based on porous materials, but is still not fully established for heterogeneous catalysts. Here a molecular imprinting approach is introduced to generate a supported palladium catalyst for the selective hydrogenation of benzene from mixtures of aromatic molecules.

Published
2021
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2. Direct aerobic oxidation of monoalcohol and diols to acetals using tandem Ru@MOF catalysts

Author

Dan Wu, Jingpeng Zhao, Vitaly V. Ordomsky, Yi Yu, Willinton Y. Hernández, Tao He, Songwei Zhang, Jerry Pui Ho Li, Biao Yuan, Yong Yang, Wen-Juan Zhou, Tao Li, Solvay (France), 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), Laboratoire pluridisciplinaire de recherche en ingénierie des systèmes, mécanique et énergétique (PRISME), Université d'Orléans (UO)-Institut National des Sciences Appliquées - Centre Val de Loire (INSA CVL), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), 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), 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 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

Subjects
Tandem, Acetal, Diol, Nanoparticle, Alcohol, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Atomic and Molecular Physics, and Optics, 0104 chemical sciences, Catalysis, chemistry.chemical_compound, chemistry, Organic chemistry, [CHIM]Chemical Sciences, General Materials Science, Metal-organic framework, Lewis acids and bases, Electrical and Electronic Engineering, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

The aerobic oxidation of monoalcohols and diols to acetals is an important academic and industrial challenge for the production of fine chemicals and intermediates. The existing methods usually rely on a two-step process in which alcohols are first oxidized to aldehydes over metal catalysts (Ru, Pt, Pd) and then acetalized using acids. Due to the instability of aldehydes, how to avoid over-oxidation to their respective carboxylic acids and esters is a long-standing challenge. For this reason, certain non-conjugated dialdehydes have never been successfully produced from diol oxidation. Hereby we report a Ru@metal-organic framework (MOF) tandem catalyst containing ultra-fine Ru nanoparticles (< 2 nm) for direct alcohol to acetal conversion of monoalcohol and diols with no formation of carboxylic acids. Mechanistic study reveals that the presence of Lewis acid sites in the MOF work in concert with Ru active sites to promptly convert aldehydes to acetals thereby effectively suppressing the formation of over-oxidation byproducts.

Published
2021
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3. Quinone Shuttling Impels Selective Electrocatalytic Alcohol Oxidation: A Hydrogen Bonding-Directed Electrosynthesis

Author

Linjie Zhang, Alexis Grimaud, Renate Schwiedernoch, Vitaly V. Ordomsky, Negar Naghavi, Willinton Y. Hernández, 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), Université de Lille, Centre National de la Recherche Scientifique (CNRS), Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, 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, Institut Photovoltaïque d’Ile-de-France (UMR) (IPVF), École polytechnique (X)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-TOTAL FINA ELF-EDF (EDF)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Photovoltaïque d’Ile-de-France (ITE) (IPVF)-Air Liquide [Siège Social], Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-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
General Chemical Engineering, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, Electrosynthesis, 010402 general chemistry, Aldehyde, 01 natural sciences, [SPI.MAT]Engineering Sciences [physics]/Materials, Analytical Chemistry, Furfuryl alcohol, Catalysis, chemistry.chemical_compound, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Electrochemistry, [CHIM]Chemical Sciences, Dehydrogenation, Hydrogen production, chemistry.chemical_classification, [CHIM.ORGA]Chemical Sciences/Organic chemistry, 010405 organic chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, Combinatorial chemistry, Quinone, 0104 chemical sciences, chemistry, 13. Climate action, Alcohol oxidation, 0210 nano-technology
Abstract

International audience; Today development of efficient catalytic systems for selective oxidation of alcohols to aldehydes remains not only a major concern in basic chemistry research but also a significant challenge for the chemical industry. One promising green and sustainable approach to increase the selectivity as well as waste reduction and to minimize the use of toxic and/or hazardous substances is the development of selective electro-catalytic acceptorless dehydrogenation method. By that, it will be possible to facilitate catalyst recovery and reutilization as well as producing only hydrogen as the by-product. Quinones as principal redox-active moieties within natural organic materials play a key role in electron-transport processes of biological systems. Herein, by taking the oxidation of furfuryl alcohol (FA) in dimethyl sulfoxide (DMSO) as a model reaction, 14 quinone derivatives from 3 families (benzoquinones (BQs), naphthoquinones (NQs), and anthraquinones (AQs)) have been surveyed as a hydrogen acceptor mediators. We demonstrate that, only for three-member ring quinones such as 9,10-anthraquinone-2,6-disulfonic acid (AQDS), which are stable during electrocatalysis, a significant increase of the selectivity to furfural with addition of AQDS is achieved. The effect is assigned to strong intermolecular interaction between FA and quinone dianion (Q 2−) with selective transformation to aldehyde its regeneration to quinone and hydrogen production over cathode surface. This study assesses and validates the potential of quinones as electrocatalytic hydrogen acceptor mediators to impel the selective oxidation of alcohol to aldehydes.

Published
2021
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4. Nanocell type Ru@quinone core-shell catalyst for selective oxidation of alcohols to carbonyl compounds

Author

M. Wu, Vitaly V. Ordomsky, Willinton Y. Hernández, Evgeny I. Vovk, Jingpeng Zhao, Mickaël Capron, Wen-Juan Zhou, N. Naghavi, Yong Yang, Ecole Nationale Supérieure de Chimie de Lille (ENSCL), Université de Lille, 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 d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Eco-Efficient Products and Processes Laboratory (E2P2L), École normale supérieure - Lyon (ENS Lyon)-Solvay-Centre National de la Recherche Scientifique (CNRS), Université Lille Nord de France (COMUE)-École normale supérieure - Lyon (ENS Lyon)-Solvay-Centre National de la Recherche Scientifique (CNRS), School of Physical Science and Technology (SPST), ShanghaiTech University [Shanghai], Unité de Catalyse et de Chimie du Solide - UMR 8181 (UCCS), and Université d'Artois (UA)-Ecole Centrale de Lille-Ecole Nationale Supérieure de Chimie de Lille (ENSCL)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille

Subjects
chemistry.chemical_classification, 010405 organic chemistry, Chemistry, Process Chemistry and Technology, Ru, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, Electrochemistry, Hydrogen atom abstraction, 01 natural sciences, Redox, Aldehyde, Catalysis, 0104 chemical sciences, Quinone, [SPI.MAT]Engineering Sciences [physics]/Materials, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Alcohol oxidation, Alcohols, Polymer chemistry, Nanocell, Selectivity
Abstract

International audience; Selective aerobic oxidation of alcohols to corresponding carbonyl compounds is one of the most important challenges in the modern chemical industry. The existing metal based heterogeneous catalysts provide low selectivity due to over-oxidation of aldehydes to acids and esters. We have found that coating of Ru nanoparticles by disodium anthraquinone-2,6-disulfonate (SQ) results in selective oxidation of aliphatic, unsaturated and aromatic alcohols to aldehydes. Analysis of core-shell Ru@SQ catalyst shows strong interaction between Ru and SQ leading to change of their electronic state and structure. In-situ study of alcohol oxidation using FTIR and electrochemistry indicates on hydrogen abstraction by shell quinone species with hydrogen transfer by quinone to Ru core for water generation. Thus, the catalyst behavior mimics nano-electrocell by separation of oxidation reaction over quinone and reduction of oxygen over Ru providing higher selectivity to aldehyde.

Published
2020
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5. Solid micellar Ru single-atom catalysts for the water-free hydrogenation of CO2 to formic acid

Author

Willinton Y. Hernández, Olga V. Safonova, Vitaly V. Ordomsky, Evgeny I. Vovk, César A. Urbina-Blanco, Mark Saeys, Maya Marinova, Marianne Impéror-Clerc, Walid Baaziz, Qiyan Wang, Sara Santos, Andrei Y. Khodakov, Ovidiu Ersen, 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, Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, Laboratoire de Physique des Solides (LPS), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), 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), 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), Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Universiteit Gent = Ghent University (UGENT), University of Shanghai for Science and Technology, 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), Université de Strasbourg (UNISTRA)-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)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, 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)-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 d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), and ANR-16-CE06-0013,NANO4FuT,Synthèse des carburants alternatifs et des molécules plateforme sur nanoréacteurs(2016)

Subjects
Tertiary amine, Hydrogen, Formic acid, CO2 hydrogenation, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, Photochemistry, 01 natural sciences, 7. Clean energy, Micelle, Heterolysis, Catalysis, chemistry.chemical_compound, [CHIM]Chemical Sciences, Formate, ComputingMilieux_MISCELLANEOUS, General Environmental Science, Hydride, Process Chemistry and Technology, Ru, 021001 nanoscience & nanotechnology, Solid micelles, 0104 chemical sciences, chemistry, 0210 nano-technology, Single-atom catalysts
Abstract

International audience; The catalytic hydrogenation of CO2 to formic acid is one of the most promising pathways towards a renewable hydrogen-storage system. The reaction is usually performed in aqueous phase in the presence of basic molecules over homogeneous or heterogeneous catalysts, generating relatively dilute formate solutions (

Published
2021
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6. One-pot preparation of Ni-Cu nanoparticles supported on γ-Al2O3 as selective and stable catalyst for the Guerbet reaction of 1-octanol

Author

Sander Clerick, Pascal Van Der Voort, Willinton Y. Hernández, An Verberckmoes, and Kevin De Vlieger

Subjects
1-Octanol, Nanocomposite, Process Chemistry and Technology, Kinetics, Inorganic chemistry, Nanoparticle, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Catalysis, 0104 chemical sciences, chemistry.chemical_compound, Guerbet reaction, chemistry, Chemisorption, 0210 nano-technology, Selectivity, Nuclear chemistry
Abstract

This paper reports on the “in-situ” preparation-deposition and reduction of Ni-Cu nanoparticles (NPs) on γ-Al 2 O 3 as support, using a green and elegant one-pot synthesis approach. Pristine and supported Ni-Cu NPs were evaluated as (de)hydrogenation catalysts for the Guerbet reaction of 1-octanol and compared with a classic impregnated and “ex-situ” reduced NiCu on γ-Al 2 O 3 catalyst. XRD reavealed that the degree of Ni-Cu nano-alloying was insignificant in the one-pot preparation method, resulting in Ni-Cu nanocomposites, while the degree of nano-alloying was resp. low and very high in the pristine nanoparticles (NPs) and the classic impregnated catalyst. The degree of reduction was very similar for both the in-situ and ex-situ reduction treatments of the supported catalysts as demonstrated by H 2 chemisorption. The “in-situ” prepared supported Ni-Cu NPs showed an enhanced kinetics when compared to the unsupported pristine Ni-Cu NPs, showing a beneficial effect of the metal-support interaction, however the classic impregnated catalyst showed overall the best kinetics, selectivity and stability for the Guerbet reaction of 1-octanol.

Published
2017
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7. Dual Metal-Acid Pd-Br Catalyst for Selective Hydrodeoxygenation of 5-Hydroxymethylfurfural (HMF) to 2, 5-Dimethylfuran at Ambient Temperature

Author

Dan Wu, Maya Marinova, Andrei Y. Khodakov, Songwei Zhang, Willinton Y. Hernández, Vitaly V. Ordomsky, Ovidiu Ersen, Walid Baaziz, Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), 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), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-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)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, 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)-Centre National de la Recherche Scientifique (CNRS), Institut Michel Eugène Chevreul - FR 2638 (IMEC), 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), 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), ShanghaiTech University [Shanghai], Ecole Nationale Supérieure de Chimie de Lille (ENSCL), Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, 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), 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), 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), 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, and univOAK, Archive ouverte

Subjects
2,5-Dimethylfuran, chemistry.chemical_element, hydrodeoxygenation, 010402 general chemistry, Heterogeneous catalysis, 01 natural sciences, Catalysis, Metal, chemistry.chemical_compound, [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS, biomass, 010405 organic chemistry, Chemistry, [CHIM.CATA] Chemical Sciences/Catalysis, General Chemistry, bifunctional catalysis, [CHIM.CATA]Chemical Sciences/Catalysis, Combinatorial chemistry, 0104 chemical sciences, Bifunctional catalyst, heterogeneous catalysis, dimethylfuran, visual_art, visual_art.visual_art_medium, Brønsted–Lowry acid–base theory, Hydrodeoxygenation, Palladium
Abstract

Supported metal catalysts have found broad applications in heterogeneous catalysis. In the conventional bifunctional catalyst, the active metal sites are associated with the metal nanoparticles, while the acid sites are usually localized over the oxide support. Herein, we report a novel type of supported metal bifunctional catalyst, which combined the advantages of the promotion and bifunctionality. The catalyst was designed by the pretreatment of supported palladium catalysts with bromobenzene. The promotion with bromine creates Bronsted acid sites, which are localized directly on the surface of metal nanoparticles. An intimacy between metal and acid functions in this bifunctional catalyst generates unique catalytic properties in hydrodeoxygenation of 5-hydroxymethylfurfural to dimethylfuran, occurring with the yield up to 96% at ambient temperature under 5 bar of H-2. The catalyst exhibits stable catalytic performance.

Published
2020
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8. In Situ Generation of Brønsted Acidity in the Pd-I Bifunctional Catalysts for Selective Reductive Etherification of Carbonyl Compounds under Mild Conditions

Author

Dan Wu, Willinton Y. Hernández, Xiaohong Zhou, Andrei Y. Khodakov, Vitaly V. Ordomsky, Evgeny I. Vovk, Yong Yang, Songwei Zhang, East China Jiaotong University (ECJU), Faculty of Animal Husbandry and Veterinary Medicine, Shenyang Agricultural University, 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 d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), and Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille

Subjects
Hydrogen, 010405 organic chemistry, Chemistry, [CHIM.ORGA]Chemical Sciences/Organic chemistry, chemistry.chemical_element, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, Heterogeneous catalysis, 01 natural sciences, Heterolysis, Catalysis, Dissociation (chemistry), 0104 chemical sciences, chemistry.chemical_compound, Surface modification, Organic chemistry, [CHIM]Chemical Sciences, Brønsted–Lowry acid–base theory, Bifunctional, ComputingMilieux_MISCELLANEOUS
Abstract

Selective synthesis of ethers from biomass derived carbonyl compounds is an important academic and industrial challenge. The existing processes based on strong acid or metallic catalysts cannot provide high selectivity to ethers due to the occurrence of side reactions. Hereby we propose a Pd-I bifunctional heterogeneous catalyst for the selective reductive etherification of aldehydes with alcohols. Extensive catalyst characterizations uncovered the presence of iodine species on the surface of Pd nanoparticles. Heterolytic dissociation of hydrogen on the I-Pd surface sites leads to the "in situ" generation of a Bronsted acid, which promotes the reaction toward the corresponding ethers with extremely high selectivity under very mild reaction conditions.

Published
2019
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9. Structural and catalytic properties of Au/MgO-type catalysts prepared in aqueous or methanol phase: application in the CO oxidation reaction

Author

Miguel Ángel Centeno, Funda Aliç, Willinton Y. Hernández, Pieter Vermeir, Pascal Van Der Voort, Sara Navarro-Jaén, An Verberckmoes, and Agency for Innovation by Science and Technology (Belgium)

Subjects
Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Catalysis, chemistry.chemical_compound, Gold catalyst, Phase (matter), Gold nanoparticles, Hydrothermal synthesis, General Materials Science, Other hand, Aqueous solution, Magnesium, Mechanical Engineering, Brucite, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Solvent, chemistry, Mechanics of Materials, Methanol, 0210 nano-technology, Dispersion (chemistry), XANES spectrum
Abstract

Au/MgO and Au/Mg(OH)-type catalysts for CO oxidation reaction were prepared by using two different synthesis methods in presence of either an aqueous or methanol phase. The influence of the porous and morphological properties of the starting magnesium oxide supports was analyzed and correlated with the catalytic performances of the final gold-supported catalysts. It was found that the deposition of gold in the presence of methanol as a solvent avoids the total rehydration of the MgO support and maintains the textural and morphological properties of the starting oxides. The support synthesized by a surfactant-assisted hydrothermal route, having a combined meso-macroporous structure (i.e., MgO-P) showed a positive influence on the CO oxidation reaction as it favored the dispersion of gold and the surface-to-gas phase interaction during the catalytic process., This work was partially funded by the IWT—Belgium.

Published
2016
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10. Ni−Cu Hydrotalcite-Derived Mixed Oxides as Highly Selective and Stable Catalysts for the Synthesis of β-Branched Bioalcohols by the Guerbet Reaction

Author

Willinton Y. Hernández, Pascal Van Der Voort, An Verberckmoes, and Kevin De Vlieger

Subjects
inorganic chemicals, Magnesium Hydroxide, General Chemical Engineering, chemistry.chemical_element, Aluminum Hydroxide, Alcohol, Chemistry Techniques, Synthetic, engineering.material, 010402 general chemistry, 01 natural sciences, Catalysis, Rhodium, chemistry.chemical_compound, Guerbet reaction, Drug Stability, Nickel, Environmental Chemistry, Organic chemistry, heterocyclic compounds, General Materials Science, Hydrotalcite, 010405 organic chemistry, Isobutanol, organic chemicals, Butanol, Layered double hydroxides, Oxides, 0104 chemical sciences, General Energy, chemistry, Alcohols, engineering, Dimerization, Copper
Abstract

A series of Ni-Cu hydrotalcite-derived mixed oxides have been synthesized and evaluated as heterogeneous catalysts for the dimerization of linear aliphatic alcohols to afford beta-branched Guerbet alcohols. The use of the hydrotalcite-structured catalyst precursor highly favors the catalyst stability. This Cu/Ni catalyst has an enhanced reducibility of Ni2+ species under reaction conditions, favoring the hydrogen transfer and hydrogenation capacity of the catalyst system. Catalytic results are reported for C-8, mixed C-8/C-10, and C-18 alcohol feeds, with full conversions and Guerbet product purities of 72.5-96 %.

Published
2016
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11. Alkyl coupling in tertiary amines as analog of Guerbet condensation reaction

Author

Changru Ma, Vitaly V. Ordomsky, Dan Wu, Willinton Y. Hernández, Huangyang Su, Yage Zhou, East China University of Science and Technology, Eco-Efficient Products &Processes Laboratory (E2PL2), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-RHODIA, Solvay (France), 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, Eco-Efficient Products & Processes Laboratory (E2P2L), RHODIA-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
chemistry.chemical_classification, Chemistry, [CHIM.ORGA]Chemical Sciences/Organic chemistry, General Chemical Engineering, 02 engineering and technology, General Chemistry, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensation reaction, 01 natural sciences, Medicinal chemistry, 0104 chemical sciences, 3. Good health, Catalysis, Guerbet reaction, Molecule, Dehydrogenation, 0210 nano-technology, Long chain, Alkyl
Abstract

International audience; We report here that CC coupling in tertiary amines for the synthesis of long chain and hindered amines might be efficiently performed over Pt and Pd catalysts. The mechanism study confirms similarity with the Guerbet reaction through dehydrogenation of the alkyl group and subsequent attack of the acarbon atom by an alkyl group of another molecule. Finally, secondary amines and tertiary amines with longer alkyl chains are formed.

Published
2019
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12. Silver-modified manganite and ferrite perovskites for catalyzed gasoline particulate filters

Author

Philippe Vernoux, Willinton Y. Hernández, Antoinette Boreave, Diego Lopez-Gonzalez, C. Zhao, Spyridon Ntais, IRCELYON-Catalytic and Atmospheric Reactivity for the Environment (CARE), 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), and Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Process Chemistry and Technology, chemistry.chemical_element, 02 engineering and technology, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, 021001 nanoscience & nanotechnology, medicine.disease_cause, Manganite, 01 natural sciences, Redox, Oxygen, [SDE.ES]Environmental Sciences/Environmental and Society, Catalysis, Soot, 0104 chemical sciences, Adsorption, Chemical engineering, chemistry, Agglomerate, medicine, Ferrite (magnet), 0210 nano-technology, General Environmental Science
Abstract

Silver modified manganite (LaSrAgMn) and ferrite (LaSrAgFe) perovskites were synthesized with different Ag loadings and tested for the soot oxidation reaction at low oxygen concentrations (i.e. 1 vol%), as encountered in gasoline direct injection (GDI) engines application. The state and location of Ag determine the catalytic performances of perovskites. On ferrites, Ag is either partially incorporated on the structure or present on the surface as large agglomerates. Lattice Ag+ cations are not catalytically active. Furthermore, large surface Ag particles partially cover surface oxygen vacancies and block their ability to adsorb oxygen. On the other hand, small clusters of Ag and AgO as well as a surface Ag1.8Mn8O16 additional hollandite-type phase are stabilized on manganites surface, improving the reducibility and acting as active sites for soot oxidation.

Published
2018
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13. Non-metallic Aerobic Oxidation of Alcohols over Anthraquinone Based Compounds

Author

Vitaly V. Ordomsky, Dan Wu, Mickaël Capron, Wen-Juan Zhou, Willinton Y. Hernández, Jingpeng Zhao, 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), 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, 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 d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)

Subjects
chemistry.chemical_classification, 010405 organic chemistry, Chemistry, Process Chemistry and Technology, Cyclohexanol, Cyclohexanone, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Aldehyde, Anthraquinone, Catalysis, 0104 chemical sciences, chemistry.chemical_compound, Catalytic oxidation, Benzyl alcohol, Alcohol oxidation, Organic chemistry, ComputingMilieux_MISCELLANEOUS
Abstract

The catalytic performances of substituted anthraquinones were investigated in catalytic oxidation of alcohols like cyclohexanol, benzyl alcohol and 5-hydroxymethylfurfural (HMF) to carbonyl compounds (cyclohexanone, benzyl aldehyde and diformylfuran). The reduction potential of anthraquinone plays the key role in the oxidation reactions. TOF numbers and selectivities to carbonyl compounds pass through the maximum with increase of the reduction potential. The maximum activity and selectivity (>80 %) is observed for sulfonated and carboxylated anthraquinones having intermediate reduction potentials (≈ 0.1-0.2 V vs SHE). Grafted 2-carboxyanthraquinone catalyst has demonstrated comparable catalytic performance to the parent molecule and might be used as heterogeneous catalyst. The oxidation reaction was found to have radical character with transfer of hydrogen from alcohol to anthraquinone and subsequent oxidation of hydrogenated anthraquinone by oxygen.

Published
2020
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14. Recent advances on the utilization of layered double hydroxides (LDHs) and related heterogeneous catalysts in a lignocellulosic-feedstock biorefinery scheme

Author

Willinton Y. Hernández, An Verberckmoes, Pascal Van Der Voort, and Jeroen Lauwaert

Subjects
Materials science, FISCHER-TROPSCH SYNTHESIS, One-pot synthesis, Lignocellulosic biomass, Biomass, engineering.material, Raw material, HIGHLY EFFICIENT HYDROGENATION, 010402 general chemistry, SOLID-BASE CATALYSTS, 01 natural sciences, Catalysis, CO-PRECIPITATED CATALYSTS, Environmental Chemistry, Organic chemistry, BIOMASS-DERIVED COMPOUNDS, 010405 organic chemistry, Layered double hydroxides, Fischer–Tropsch process, Biorefinery, Pollution, TRANSITION-METAL-COMPLEXES, 0104 chemical sciences, ONE-POT SYNTHESIS, MG-AL HYDROTALCITES, Chemistry, IRON ALLOY NANOPARTICLES, engineering, Biochemical engineering, HYDROTALCITE-LIKE PRECURSORS
Abstract

Layered double hydroxides (LDHs) and derived materials have been widely used as heterogeneous catalysts for different types of reactions either in gas or in liquid phase. Among these processes, the valorization/upgrading of lignocellulosic biomass and derived molecules have attracted enormous attention because it constitutes a pivotal axis in the transition from an economic model based on fossil resources to one based on renewable biomass resources with preference for biomass waste streams. Proof of this is the increasing amount of literature reports regarding the rational design and implementation of LDHs and related materials in catalytic processes such as: depolymerization, hydrogenation, selective oxidations, and C–C coupling reactions, among others, where biomass-derived compounds are used. The major aim of this contribution is to situate the most recent advances on the implementation of these types of catalysts into a lignocellulosic-feedstock biorefinery scheme, highlighting the versatility of LDHs and derived materials as multifunctional, tunable, cheap and easy to produce heterogeneous catalysts.

Published
2017

15. Application toward Confocal Full-Field Microscopic X-ray Absorption Near Edge Structure Spectroscopy

Author

Pascal Van Der Voort, Bart Vekemans, J. Rudloff-Grund, Pieter Tack, Brecht Laforce, Jan Garrevoet, Frank E. Brenker, Willinton Y. Hernández, Laszlo Vincze, and Gerald Falkenberg

Subjects
business.industry, Chemistry, Confocal, 010401 analytical chemistry, Detector, Analytical chemistry, Diamond, engineering.material, 010402 general chemistry, 01 natural sciences, Sample (graphics), XANES, 0104 chemical sciences, Analytical Chemistry, Chemical state, Optics, ddc:540, engineering, Absorption (electromagnetic radiation), Spectroscopy, business
Abstract

Analytical chemistry 89(3), 2123 - 2130 (2017). doi:10.1021/acs.analchem.6b04828, Using X-ray absorption near edge structure (XANES) spectroscopy, information on the local chemical structure and oxidation state of an element of interest can be acquired. Conventionally, this information can be obtained in a spatially resolved manner by scanning a sample through a focused X-ray beam. Recently, full-field methods have been developed to obtain direct 2D chemical state information by imaging a large sample area. These methods are usually in transmission mode, thus restricting the use to thin and transmitting samples. Here, a fluorescence method is displayed using an energy-dispersive pnCCD detector, the SLcam, characterized by measurement times far superior to what is generally applicable. Additionally, this method operates in confocal mode, thus providing direct 3D spatially resolved chemical state information from a selected subvolume of a sample, without the need of rotating a sample. The method is applied to two samples: a gold-supported magnesia catalyst (Au/MgO) and a natural diamond containing Fe-rich inclusions. Both samples provide XANES spectra that can be overlapped with reference XANES spectra, allowing this method to be used for fingerprinting and linear combination analysis of known XANES reference compounds., Published by American Chemical Society, Columbus, Ohio

Published
2017
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16. Tuning the acidic-basic properties by Zn-substitution in Mg-Al hydrotalcites as optimal catalysts for the aldol condensation reaction

Author

Funda Aliç, Willinton Y. Hernández, An Verberckmoes, and Pascal Van Der Voort

Subjects
REHYDRATION, SURFACE, Inorganic chemistry, engineering.material, 010402 general chemistry, 01 natural sciences, Aldehyde, Catalysis, chemistry.chemical_compound, TRANSITION-METAL, General Materials Science, HALIDES, ALDEHYDES, chemistry.chemical_classification, Hydrotalcite, ACETONE, 010405 organic chemistry, Mechanical Engineering, Thermal decomposition, Layered double hydroxides, MIXED OXIDES, 0104 chemical sciences, Chemistry, LAYERED DOUBLE HYDROXIDES, Octanal, chemistry, Mechanics of Materials, HETEROGENEOUS CATALYSIS, engineering, Mixed oxide, Aldol condensation, ANIONIC CLAYS
Abstract

Mg-Zn-Al hydrotalcites and derived mixed oxides with different Mg2+-to-Zn2+ ratios were prepared by co-precipitation in super-saturated conditions, followed by thermal decomposition at 500 A degrees C. The synthesized materials were evaluated as catalysts for the self-condensation of octanal in order to establish structure-to-functionality properties of the prepared materials. The presence of zinc affects the structural and textural properties of the as-synthesized hydrotalcites and derived mixed oxides, and provokes a remarkable modification on the acidic-basic properties of the materials as studied by CO2 and NH3-TPD. The presence of Zn2+ caused an increment in the concentration of surface acidic sites compared to the binary Mg-Al system. The samples characterized by a Zn/Mg ratio aecurrency sign1 showed the optimal ratio of acidic and basic sites and the best catalytic performance for the production of the alpha,beta-unsaturated aldehyde. The reconstruction of the layered materials (starting from the mixed oxides) caused an increment in the concentration of surface OH- groups, further modifying the selectivity of the reaction.

Published
2017

17. Structural and catalytic properties of lanthanide (La, Eu, Gd) doped ceria

Author

Willinton Y. Hernández, Miguel Ángel Centeno, Óscar H. Laguna, José Antonio Odriozola, AIR (AIR), 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)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)

Subjects
Lanthanide, Materials science, Coprecipitation, Inorganic chemistry, 02 engineering and technology, Crystal structure, 010402 general chemistry, 01 natural sciences, Catalysis, Inorganic Chemistry, symbols.namesake, Materials Chemistry, Physical and Theoretical Chemistry, Ionic radius, Dopant, Doping, [CHIM.CATA]Chemical Sciences/Catalysis, 021001 nanoscience & nanotechnology, Condensed Matter Physics, [SDE.ES]Environmental Sciences/Environmental and Society, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Crystallography, Ceramics and Composites, symbols, 0210 nano-technology, Raman spectroscopy
Abstract

Ce{sub 0.9}M{sub 0.1}O{sub 2-{delta}} mixed oxides (M=La, Eu and Gd) were synthesized by coprecipitation. Independent of the dopant cation, the obtained solids maintain the F-type crystalline structure, characteristic of CeO{sub 2} (fluorite structure) without phase segregation. The ceria lattice expands depending on the ionic radii of the dopant cation, as indicated by X-ray diffraction studies. This effect also agrees with the observed shift of the F{sub 2g} Raman vibrational mode. The presence of the dopant cations in the ceria lattice increases the concentration of structural oxygen vacancies and the reducibility of the redox pair Ce{sup 4+}/Ce{sup 3+}. All synthesized materials show higher catalytic activity for the CO oxidation reaction than that of bare CeO{sub 2}, being Eu-doped solid the one with the best catalytic performances despite of its lower surface area. - Graphical abstract: In this work, Ce{sub 0.9}M{sub 0.1}O{sub 2-{delta}} mixed oxides (M=La, Eu and Gd) were synthesized by coprecipitation. Independent of the dopant cation, the obtained solids maintain the F-type crystalline structure, characteristic of CeO{sub 2} (fluorite structure) without phase segregation. The ceria lattice expands depending on the ionic radii of the dopant cation, as indicated by X-ray diffraction studies. This effect also agrees with the observed shiftmore » of the F{sub 2g} Raman vibrational mode. The presence of the dopant cations in the ceria lattice increases the concentration of structural oxygen vacancies and the reducibility of the redox pair Ce{sup 4+}/Ce{sup 3+}. All synthesized materials show higher catalytic activity for the CO oxidation reaction than that of bare CeO{sub 2}, being Eu-doped solid the one with the best catalytic performances despite of its lower surface area. Highlights: > Lanthanide doped ceria as catalytic supports for CO oxidation reaction. > A higher concentration of oxygen vacancies promotes a higher catalytic activity. > Eu-doped ceria shows improved catalytic properties for the CO oxidation reaction.« less

Published
2011
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18. La/Sr-based perovskites as soot oxidation catalysts for Gasoline Particulate Filters

Author

Françoise Bosselet, Antoinette Boreave, Willinton Y. Hernández, Philippe Vernoux, Mihalis N. Tsampas, C. Zhao, 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), IRCELYON-Catalytic and Atmospheric Reactivity for the Environment (CARE), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL), and IRCELYON-Diffraction des rayons X (RX)

Subjects
Thermal decomposition, Inorganic chemistry, chemistry.chemical_element, [CHIM.CATA]Chemical Sciences/Catalysis, 02 engineering and technology, General Chemistry, Partial pressure, 010402 general chemistry, 021001 nanoscience & nanotechnology, medicine.disease_cause, [SDE.ES]Environmental Sciences/Environmental and Society, 01 natural sciences, Oxygen, Redox, Catalysis, Soot, 0104 chemical sciences, chemistry, Oxidation state, medicine, Gasoline, 0210 nano-technology
Abstract

RX+CARE+MTS:CZA:ABO:FBS:PVE; International audience; La0.6Sr0.4BO3 type-perovskites (with B = Fe, Mn or Ti) were synthesized by a complex route from the thermal decomposition of the chelated nitrate precursors, as soot oxidation catalysts under low oxygen partial pressures. The nature of the B-site cation modifies the morphology, the structural symmetry, the charge compensation mechanism and the redox properties. The generation of oxygen vacancies is predominant in LSF while an increase in the oxidation state of B cations occurs in LSM and LST, respectively. A direct link was established between the reducibility of the perovskites and their ability to oxidize soot. Fe and Mn-based perovskites exhibit similar catalytic behaviors, superior to LET, which are attributed to the presence of oxygen vacancies in LSF and Mn4+ cations in ISM. This latter redox property is particularly suitable to oxidize soot at low oxygen partial pressures, as encountered in gasoline direct injection engine exhausts. (C) 2014 Elsevier B.V. All rights reserved.

Published
2015
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19. Light-Driven Water Oxidation with Metal Hexacyanometallate Heterogeneous Catalysts

Author

Willinton Y. Hernández, José Ramón Galán-Mascarós, Sara Goberna-Ferrón, and Bárbara Rodríguez-García

Subjects
010405 organic chemistry, Chemistry, Inorganic chemistry, Oxygen evolution, chemistry.chemical_element, General Chemistry, Manganese, 010402 general chemistry, Heterogeneous catalysis, Photochemistry, Persulfate, 01 natural sciences, Catalysis, 0104 chemical sciences, Artificial photosynthesis, Metal, visual_art, visual_art.visual_art_medium, Cobalt
Abstract

The catalytic activity of metal hexacyanometallates (Prussian blue-type coordination polymers) was tested in photoactivated water oxidation by [Ru(2-2′-bpy)3]2+/persulfate system at pH close to neutrality. This screening shows that manganese and cobalt N-coordinated compounds are able to catalyze the oxygen evolution reaction. Mn hexacyanometalates show low activity. Co hexacyanometalates, in contrast, appear highly active and promote robust catalysis with excellent quantum yield (≤88%), even in acidic media. Our results indicate that these catalysts are viable candidates for a photoactivated water oxidation process as part of an artificial photosynthesis scheme.

Published
2014
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20. Cu-modified cryptomelane oxide as active catalyst for CO oxidation reactions

Author

Miguel Ángel Centeno, Pierre Eloy, Svetlana Ivanova, Eric M. Gaigneaux, Willinton Y. Hernández, José Antonio Odriozola, AIR (AIR), 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)-Université Claude Bernard Lyon 1 (UCBL), and Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)

Subjects
Thermogravimetric analysis, Chemistry, Process Chemistry and Technology, PROX, Inorganic chemistry, Oxide, 02 engineering and technology, [CHIM.CATA]Chemical Sciences/Catalysis, engineering.material, 010402 general chemistry, 021001 nanoscience & nanotechnology, Molecular sieve, 7. Clean energy, 01 natural sciences, Redox, [SDE.ES]Environmental Sciences/Environmental and Society, Catalysis, 0104 chemical sciences, chemistry.chemical_compound, engineering, Cryptomelane, Temperature-programmed reduction, 0210 nano-technology, General Environmental Science
Abstract

AIR+WHE; Manganese oxide octahedral molecular sieves (cryptomelane structure) were synthesized by a solvent-free method and tested in the total oxidation of CO (TOX), and preferential oxidation of CO in presence of hydrogen (PROX). The influence of Cu in the cryptomelane structure was evaluated by several characterization techniques such as: X-ray fluorescence (XRF), thermogravimetric analysis (TGA), hydrogen temperature programmed reduction (TPR-H-2) and X-ray photoelectron spectroscopy (XPS). The Cu-modified manganese oxide material (OMS-Cu) showed very high catalytic activity for CO oxidation in comparison to the bare manganese oxide octahedral molecular sieve (OMS). The improved catalytic activity observed in OMS-Cu catalyst was associated to a high lattice oxygen mobility and availability due to the formation of Cu-Mn-O bridges. In addition, under PROX reaction conditions the catalytic activity considerably decreases in the presence of 10% (v/v) CO2 in the feed while the same amount of water provokes an improvement in the CO conversion and O-2 selectivity. (c) 2012 Elsevier B.V. All rights reserved.

Published
2012
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21. Electrochemical activation of Pt-Ba/YSZ NO(x)TRAP catalyst under lean-burn conditions

Author

Philippe Vernoux, Caroline Tardivat, Agnès Princivalle, Christian Guizard, A. Hadjar, Willinton Y. Hernández, Laboratoire de Synthèse et Fonctionnalisation de Céramiques (LSFC), Saint Gobain-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), and Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)

Subjects
Inorganic chemistry, chemistry.chemical_element, 02 engineering and technology, Partial pressure, [CHIM.CATA]Chemical Sciences/Catalysis, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrocatalyst, 01 natural sciences, Oxygen, [SDE.ES]Environmental Sciences/Environmental and Society, 0104 chemical sciences, Catalysis, lcsh:Chemistry, chemistry, lcsh:Industrial electrochemistry, lcsh:QD1-999, Electrochemistry, Non-faradaic electrochemical modification of catalytic activity, 0210 nano-technology, Polarization (electrochemistry), Lean burn, NOx, lcsh:TP250-261
Abstract

9 Hadjar, A. Hernandez, W. Y. Princivalle, A. Tardivat, C. Guizard, C. Vernoux, P.; The NO(x) abatement efficiency of an electrochemical NO(x)TRAP catalyst Pt-Ba/YSZ was investigated at 500 degrees C with different oxygen partial pressures in the storage phase. Cathodic polarization was found to promote the NO(x) storage capacity even under lean-burn conditions. The duration until full NO(x) storage was drastically increased by similar to 80 s in the presence of 6% of oxygen. During regeneration phases. NO electrochemical reduction occurs and can remove similar to 10% of NO(x). Electrochemical activation of the NO(x) storage capacity was linked with the generation of oxygen vacancies on the YSZ surface induced by negative polarization. (C) 2011 Elsevier B.V. All rights reserved.

Published
2011
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