Enriching Metal-Oxygen Species and Phosphate Modulating of Active Sites for Robust Electrocatalytical CO2 Reduction
© 2023 Wiley-VCH GmbH.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 46 vom: 24. Nov., Seite e2304379 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2023
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article CO2 electrocatalysis in situ characterization methods local microenvironment metal-oxygen species phosphate |
Zusammenfassung: | © 2023 Wiley-VCH GmbH. Direct electrochemical reduction of CO2 (CO2 RR) into value-added chemicals is a promising solution to reduce carbon emissions. The activity of CO2 RR is influenced deeply by the reaction microenvironment and electronic properties of the catalysts. Herein, the surface PO4 3- anions are tuned to modulate the local microenvironment and the electronic properties of the indium-based catalyst with abundant metal-oxygen species enabling efficient electrochemical conversion of CO2 to HCOO- . Indium nanoparticles coupled with PO4 3- anions (PO4 3- -In NPs) achieve a high selectivity of HCOO- up to 91.4% at a low potential of -0.98 V versus reversible hydrogen electrode (versus RHE) and a high HCOO- partial current density of 279.3 mA cm-2 at -1.1 V versus RHE in the electrochemical flow cell. In situ and ex situ characterizations confirm the PO4 3- anions keep stable on the surface of indium during CO2 RR, accelerating the generation of OCHO* intermediate. From density functional theory calculations, PO4 3- anions enrich the metal-oxygen species on the substrate to optimize the electronic structure of the catalysts and induce a local microenvironment with massive K+ ions on the interface, thus reducing the activation energy barrier of CO2 RR |
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Beschreibung: | Date Revised 16.11.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202304379 |