Hidden Mechanism Behind the Roughness-Enhanced Selectivity of Carbon Monoxide Electrocatalytic Reduction.

carbon monoxide reduction electrocatalysis kinetics mechanistic studies roughness

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:
10 May 2021
Historique:
received: 09 12 2020
pubmed: 5 3 2021
medline: 5 3 2021
entrez: 4 3 2021
Statut: ppublish

Résumé

High roughness has been proved to be an effective design strategy for electrocatalyst in many systems. Especially, high selectivity of carbon monoxide reduction (CORR) in competition with the hydrogen evolution reaction has been observed on high roughness electrocatalysts. However, the two well-known mechanisms, i.e., decreasing the energy barrier of CORR and increasing local pH, failed to understand the roughness-enhanced selectivity in a recent experiment. Herein we unravel the hidden mechanism by establishing a comprehensive kinetic model for CORR on catalysts with different roughness factors. We conclude that the roughness-enhanced CORR selectivity is actually kinetic controlled by local-electric-field-directed mass transfer of adsorbed species on the electrode surface. Several ways to optimize CORR selectivity are predicted. Our work highlights the kinetics in electrocatalysis on nanocatalysts, and provides a conceptually new principle for future catalyst design.

Identifiants

pubmed: 33660382
doi: 10.1002/anie.202016332
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

11133-11137

Subventions

Organisme : Ministry of Science and Technology of the People's Republic of China
ID : 2016YFA0400904
Organisme : Ministry of Science and Technology of the People's Republic of China
ID : 2018YFA0208702
Organisme : National Science Foundation of China
ID : 21973085
Organisme : National Science Foundation of China(CN)
ID : 21833007, 21790350, 21673212, 21521001
Organisme : Anhui Initiative in Quantum Information Technologies
ID : AHY090200
Organisme : National Science Foundation of China
ID : 21973085, 21833007, 21790350, 21673212, 21521001
Organisme : Fundamental Research Funds for the Central Universities
ID : WK2340000104

Informations de copyright

© 2021 Wiley-VCH GmbH.

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Auteurs

Yinghuan Liu (Y)

Department of Chemical Physics & Hefei National Laboratory for Physical Sciences at the Microscale, iChEM, University of Science and Technology of China, Hefei, Anhui, 230026, China.

Huijun Jiang (H)

Department of Chemical Physics & Hefei National Laboratory for Physical Sciences at the Microscale, iChEM, University of Science and Technology of China, Hefei, Anhui, 230026, China.

Zhonghuai Hou (Z)

Department of Chemical Physics & Hefei National Laboratory for Physical Sciences at the Microscale, iChEM, University of Science and Technology of China, Hefei, Anhui, 230026, China.

Classifications MeSH