In situ stabilization of Cu+ for CO2 Electroreduction via Environmental-molecules-induced ZnO1-x shield

Fanxing Zhang, Ning Cao, Chentao Wang, Shengxiang Wang, Yi He, Yao Shi, Mi Yan, Ying Bao, Zhenglong Li () and Pengfei Xie ()
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Fanxing Zhang: Zhejiang University
Ning Cao: Zhejiang University
Chentao Wang: Zhejiang University
Shengxiang Wang: Spallation Neutron Source Science Center
Yi He: Zhejiang University
Yao Shi: Zhejiang University
Mi Yan: Zhejiang University
Ying Bao: Western Washington University
Zhenglong Li: Institute of Zhejiang University-Quzhou
Pengfei Xie: Zhejiang University

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Electrochemical CO2-to-ethanol conversion is challenged by sluggish C-C coupling kinetics and wide products distribution. Although Cu+ has been demonstrated to enhance multi-carbon (C2+) formation, the stabilization of Cu+ under reduction conditions is difficult. Here, we report a hydrogen-ethanol pretreatment strategy to obtain Cu nanoparticles covered by highly dispersed and disordered ZnO1-x clusters. Ethanol-induced ZnO1-x redispersion gives rise to abundant Cu+ on the subsurface. The optimal catalyst delivers a 73.0% ethanol Faradaic efficiency (FE) and 86.0% total C2+ FE at −0.9 V, with a 2.3 mmol cm−2 h−1 ethanol formation rate and single-pass ethanol yield of 18.0%. The catalyst also exhibits stability beyond 500 h, attributed to the stabilization of Cu+ by the ZnO1-x shield that requires a high energy barrier for lattice oxygen removal. In situ X-ray spectroscopy and calculations reveal a volcano relationship between Cu+ ratio in Cu species and ethanol FE. Optimal Cu+ density not only facilitates *OC-COH coupling but also optimizes the adsorption energy of *CH2CH2O on catalyst for ethanol electrosynthesis.

Date: 2025
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DOI: 10.1038/s41467-025-61189-z

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