Steering surface reconstruction of copper with electrolyte additives for CO2 electroreduction

Zishan Han, Daliang Han, Zhe Chen, Jiachen Gao, Guangyi Jiang, Xinyu Wang, Shuaishuai Lyu, Yong Guo, Chuannan Geng, Lichang Yin (), Zhe Weng () and Quan-Hong Yang ()
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Zishan Han: Tianjin University
Daliang Han: Tianjin University
Zhe Chen: Chinese Academy of Sciences
Jiachen Gao: Tianjin University
Guangyi Jiang: Tianjin University
Xinyu Wang: Tianjin University
Shuaishuai Lyu: Tianjin University
Yong Guo: Tianjin University
Chuannan Geng: Tianjin University
Lichang Yin: Chinese Academy of Sciences
Zhe Weng: Tianjin University
Quan-Hong Yang: Tianjin University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Electrocatalytic CO2 reduction to value-added hydrocarbon products using metallic copper (Cu) catalysts is a potentially sustainable approach to facilitate carbon neutrality. However, Cu metal suffers from unavoidable and uncontrollable surface reconstruction during electrocatalysis, which can have either adverse or beneficial effects on its electrocatalytic performance. In a break from the current catalyst design path, we propose a strategy guiding the reconstruction process in a favorable direction to improve the performance. Typically, the controlled surface reconstruction is facilely realized using an electrolyte additive, ethylenediamine tetramethylenephosphonic acid, to substantially promote CO2 electroreduction to CH4 for commercial polycrystalline Cu. As a result, a stable CH4 Faradaic efficiency of 64% with a partial current density of 192 mA cm−2, thus enabling an impressive CO2-to-CH4 conversion rate of 0.25 µmol cm−2 s−1, is achieved in an alkaline flow cell. We believe our study will promote the exploration of electrochemical reconstruction and provide a promising route for the discovery of high-performance electrocatalysts.

Date: 2022
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DOI: 10.1038/s41467-022-30819-1

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