Coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of Mo-based oxide catalysts
This work aimed to develop in a two-step strategy the deoxygenation of benzoic acid as a new probe reaction of the oxidation catalysts "at work". This choice was based on the experimental fact that the distribution of the potential main products, namely benzaldehyde, toluene and benzene de...
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Universite catholique de Louvain
2005
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ndltd-BICfB-oai-ucl.ac.be-ETDUCL-BelnUcetd-11222005-1934142013-01-07T15:41:29Z Coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of Mo-based oxide catalysts Dury, Frédéric Characterization Active site Benzoic acid Propylene Oxidation This work aimed to develop in a two-step strategy the deoxygenation of benzoic acid as a new probe reaction of the oxidation catalysts "at work". This choice was based on the experimental fact that the distribution of the potential main products, namely benzaldehyde, toluene and benzene depends on the presence and the mutual disposition of oxygen vacancies at the surface of the oxide catalysts. Indeed, it is claimed in the literature that single oxygen vacancies selectively produces benzaldehyde, twin oxygen vacancies (i.e. two oxygen vacancies separated by about 2Å) induce the formation of toluene while the benzene production does not need the presence of any oxygen vacancies. Two molybdenum based catalytic systems were chosen to test the new probe reaction : the molybdenum (sub)oxides and the metal molybdates. By the way of a new and original coupling between the probe reaction and the oxidation of propylene, we planned to correlate in real time the formation of the superficial oxygen vacancies monitored by the deoxygenation of benzoic acid and the activity in an oxidation reaction. Such an experimental coupling is a promising and a powerful tool which allows the fine characterization of the active catalytic site at work in an oxidation reaction. Universite catholique de Louvain 2005-12-07 text application/pdf http://edoc.bib.ucl.ac.be:81/ETD-db/collection/available/BelnUcetd-11222005-193414/ http://edoc.bib.ucl.ac.be:81/ETD-db/collection/available/BelnUcetd-11222005-193414/ en unrestricted J'accepte que le texte de la thèse (ci-après l'oeuvre), sous réserve des parties couvertes par la confidentialité, soit publié dans le recueil électronique des thèses UCL. A cette fin, je donne licence à l'UCL : - le droit de fixer et de reproduire l'oeuvre sur support électronique : logiciel ETD/db - le droit de communiquer l'oeuvre au public Cette licence, gratuite et non exclusive, est valable pour toute la durée de la propriété littéraire et artistique, y compris ses éventuelles prolongations, et pour le monde entier. Je conserve tous les autres droits pour la reproduction et la communication de la thèse, ainsi que le droit de l'utiliser dans de futurs travaux. Je certifie avoir obtenu, conformément à la législation sur le droit d'auteur et aux exigences du droit à l'image, toutes les autorisations nécessaires à la reproduction dans ma thèse d'images, de textes, et/ou de toute oeuvre protégés par le droit d'auteur, et avoir obtenu les autorisations nécessaires à leur communication à des tiers. Au cas où un tiers est titulaire d'un droit de propriété intellectuelle sur tout ou partie de ma thèse, je certifie avoir obtenu son autorisation écrite pour l'exercice des droits mentionnés ci-dessus. |
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Characterization Active site Benzoic acid Propylene Oxidation |
spellingShingle |
Characterization Active site Benzoic acid Propylene Oxidation Dury, Frédéric Coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of Mo-based oxide catalysts |
description |
This work aimed to develop in a two-step strategy the deoxygenation of benzoic acid as a new probe reaction of the oxidation catalysts "at work". This choice was based on the experimental fact that the distribution of the potential main products, namely benzaldehyde, toluene and benzene depends on the presence and the mutual disposition of oxygen vacancies at the surface of the oxide catalysts. Indeed, it is claimed in the literature that single oxygen vacancies selectively produces benzaldehyde, twin oxygen vacancies (i.e. two oxygen vacancies separated by about 2Å) induce the formation of toluene while the benzene production does not need the presence of any oxygen vacancies. Two molybdenum based catalytic systems were chosen to test the new probe reaction : the molybdenum (sub)oxides and the metal molybdates.
By the way of a new and original coupling between the probe reaction and the oxidation of propylene, we planned to correlate in real time the formation of the superficial oxygen vacancies monitored by the deoxygenation of benzoic acid and the activity in an oxidation reaction. Such an experimental coupling is a promising and a powerful tool which allows the fine characterization of the active catalytic site at work in an oxidation reaction. |
author |
Dury, Frédéric |
author_facet |
Dury, Frédéric |
author_sort |
Dury, Frédéric |
title |
Coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of Mo-based oxide catalysts |
title_short |
Coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of Mo-based oxide catalysts |
title_full |
Coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of Mo-based oxide catalysts |
title_fullStr |
Coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of Mo-based oxide catalysts |
title_full_unstemmed |
Coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of Mo-based oxide catalysts |
title_sort |
coupling of the deoxygenation of benzoic acid with the oxidation of propylene as a new tool to elucidate the architecture of mo-based oxide catalysts |
publisher |
Universite catholique de Louvain |
publishDate |
2005 |
url |
http://edoc.bib.ucl.ac.be:81/ETD-db/collection/available/BelnUcetd-11222005-193414/ |
work_keys_str_mv |
AT duryfrederic couplingofthedeoxygenationofbenzoicacidwiththeoxidationofpropyleneasanewtooltoelucidatethearchitectureofmobasedoxidecatalysts |
_version_ |
1716393755287748608 |