Issue 23, 2024

Origin of copper as a unique catalyst for C–C coupling in electrocatalytic CO2 reduction

Abstract

High yields of C2 products through electrocatalytic CO2 reduction (eCO2R) can only be obtained using Cu-based catalysts. Here, we adopt the generalized frontier molecular orbital (MO) theory based on first-principles calculations to identify the origin of this unique property of Cu. We use the grand canonical ensemble (or fixed potential) approach to ensure that the calculated Fermi level, which serves as the frontier orbital of the metal catalyst, accurately represents the applied electrode potentials. We determine that the key intermediate OCCO assumes a U-shape configuration with the two C atoms bonded to the Cu substrate. We identify the frontier MOs that are involved in the C–C coupling. The good alignment of the Fermi level of Cu with these frontier MOs is perceived to account for the excellent catalytic performance of Cu for C–C coupling. It is expected that these new insights could provide useful guidance in tuning Cu-based catalysts as well as designing non-Cu catalysts toward high-efficiency eCO2R.

Graphical abstract: Origin of copper as a unique catalyst for C–C coupling in electrocatalytic CO2 reduction

Supplementary files

Article information

Article type
Edge Article
Submitted
28 Mar 2024
Accepted
05 May 2024
First published
13 May 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2024,15, 8835-8840

Origin of copper as a unique catalyst for C–C coupling in electrocatalytic CO2 reduction

J. Chen, B. W. J. Chen, J. Zhang, W. Chen and Y. Sun, Chem. Sci., 2024, 15, 8835 DOI: 10.1039/D4SC02056A

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