Citation: Wei Peng, Yao Shen, Xiaolin Yu, Chenghang Zheng, Xiao Zhang, Jingkai Zhao, Jiexu Ye, Shihan Zhang, Xiang Gao. Asymmetric coupling of atop-type and hollow-type adsorbed *CO to boost electrocatalytic CO₂-to-C₂ conversion on high-index Cu₂O crystal planes[J]. Chinese Chemical Letters, ;2026, 37(1): 111187. doi: 10.1016/j.cclet.2025.111187 shu

Asymmetric coupling of atop-type and hollow-type adsorbed *CO to boost electrocatalytic CO₂-to-C₂ conversion on high-index Cu₂O crystal planes

Wei Peng ^a ,
Yao Shen ^{a, b} ,
Xiaolin Yu ^c ,
Chenghang Zheng ^d ,
Xiao Zhang ^d ,
Jingkai Zhao ^a ,
Jiexu Ye ^a ,
Shihan Zhang ^{a, b, *,} ,
Xiang Gao ^{a, b, d}

a.
College of Environment, Zhejiang University of Technology, Hangzhou 310014, China
b.
Zhejiang Key Laboratory of Clean Energy Conversion and Utilization, Science and Education Integration College of Energy and Carbon Neutralization, Zhejiang University of Technology, Hangzhou 310014, China
c.
State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
d.
Carbon Neutrality Research Institute, College of Energy Engineering, Zhejiang University, Hangzhou 310027, China

shihanzhang@zjut.edu.cn

Received Date: 27 October 2024
Revised Date: 8 February 2025
Accepted Date: 8 April 2025
Available Online: 8 April 2025

Figures(6)

Cuprous oxide (Cu₂O) is one of the most promising catalysts for electrochemical conversion of CO₂ into value-added C₂ products. The efficiency of CO₂-to-C₂ conversion is highly dependent on the Cu₂O crystal plane orientation and the corresponding adsorbed *CO species. Herein, we constructed high-index crystal planes (311) in Cu₂O (CO–Cu₂O) via a facile self-selective CO-induced strategy under a CO atmosphere, which was verified by high-resolution transmission electron microscopy (HR-TEM) and atomic force microscopy (AFM) results. By exploiting the high surface energy of the high index crystal planes, *CO species are stabilized in CO–Cu₂O during CO₂RR, resulting in exceptional catalytic performance for CO₂-to-C₂ products. In situ infrared spectroscopy revealed that both atop-type (*CO_atop) and hollow-type (*CO_hollow) adsorption of *CO species occurred on the CO–Cu₂O. The asymmetric C–C coupling energy barrier between *CO_atop and *CO_hollow in (311) crystal plane decreases by 47.8% compared to the symmetric coupling of *CO_atop in conventional (100) crystal planes. Consequently, the Faradaic efficiency of C₂ products generated with CO–Cu₂O was increased by as high as 100% compared to that with pristine Cu₂O.
- Electrocatalytic conversion,
- Adsorbed *CO,
- Asymmetric C-C coupling,
- Self-selective CO-induced strategy,
- Cu₂O-based catalysts
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Asymmetric coupling of atop-type and hollow-type adsorbed *CO to boost electrocatalytic CO2-to-C2 conversion on high-index Cu2O crystal planes

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通讯作者: 陈斌, bchen63@163.com

Asymmetric coupling of atop-type and hollow-type adsorbed *CO to boost electrocatalytic CO₂-to-C₂ conversion on high-index Cu₂O crystal planes