Unveiling the CO Oxidation Mechanism over a Molecularly Defined Copper Single-Atom Catalyst Supported on a Metal-Organic Framework.
Density Functional Theory
In Situ/Operando Spectroscopies
Metal-Organic Frameworks
Reaction Mechanisms
Single-Atom Catalysts
Journal
Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543
Informations de publication
Date de publication:
24 Jul 2023
24 Jul 2023
Historique:
received:
08
02
2023
medline:
19
4
2023
pubmed:
19
4
2023
entrez:
19
04
2023
Statut:
ppublish
Résumé
Elucidating the reaction mechanism in heterogeneous catalysis is critically important for catalyst development, yet remains challenging because of the often unclear nature of the active sites. Using a molecularly defined copper single-atom catalyst supported by a UiO-66 metal-organic framework (Cu/UiO-66) allows a detailed mechanistic elucidation of the CO oxidation reaction. Based on a combination of in situ/operando spectroscopies, kinetic measurements including kinetic isotope effects, and density-functional-theory-based calculations, we identified the active site, reaction intermediates, and transition states of the dominant reaction cycle as well as the changes in oxidation/spin state during reaction. The reaction involves the continuous reactive dissociation of adsorbed O
Identifiants
pubmed: 37074965
doi: 10.1002/anie.202301920
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
e202301920Subventions
Organisme : National Science and Technology Development Agency (NSTDA) Thailand
ID : P1851755
Organisme : EU Framework Programme Horizon 2020
ID : 730872
Informations de copyright
© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
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