Issue 9, 2022

Elucidating electrochemical CO2 reduction reaction processes on Cu(hkl) single-crystal surfaces by in situ Raman spectroscopy

Abstract

Cupric materials are known to catalyze the electrochemical CO2 reduction reaction (CO2RR) and significantly improve the selectivity of multi-carbon products. Surface facets and structural effects play a critical role in the CO2RR. However, these surface mechanisms are poorly understood, and identifying trace intermediates on atomically-flat Cu(hkl) single-crystal surfaces, in situ, is a tremendously challenging task requiring sophisticated technical know-how. Here, in situ Raman spectroscopy was used to provide critical evidence of CO2RR intermediates, especially the selectivity-determining intermediates *OCCO and *CH2CHO on Cu(hkl) surfaces. Combining the spectroscopic results with theoretical calculations, Cu(111) facilitates the generation of C1 products through the formation of *COOH and *CO, while Cu(110) further generates C2 through the pathway of *OCCO and *CH2CHO. In addition, high KHCO3 concentrations facilitate the formation of the *OCCO structure, promoting C2 products. This work provides a significant breakthrough for understanding the CO2RR mechanism that can guide the design of high-efficiency catalysts.

Graphical abstract: Elucidating electrochemical CO2 reduction reaction processes on Cu(hkl) single-crystal surfaces by in situ Raman spectroscopy

Supplementary files

Article information

Article type
Paper
Submitted
24 Apr 2022
Accepted
05 Aug 2022
First published
05 Aug 2022

Energy Environ. Sci., 2022,15, 3968-3977

Elucidating electrochemical CO2 reduction reaction processes on Cu(hkl) single-crystal surfaces by in situ Raman spectroscopy

Y. Zhao, X. Zhang, N. Bodappa, W. Yang, Q. Liang, P. M. Radjenovica, Y. Wang, Y. Zhang, J. Dong, Z. Tian and J. Li, Energy Environ. Sci., 2022, 15, 3968 DOI: 10.1039/D2EE01334G

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