Planar chlorination engineering induced symmetry-broken single-atom site catalyst for enhanced CO2 electroreduction

Shengjie Wei, Jiexin Zhu (), Xingbao Chen, Rongyan Yang, Kailong Gu, Lei Li (), Ching-Yu Chiang (), Liqiang Mai () and Shenghua Chen ()
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Shengjie Wei: Beijing University of Technology
Jiexin Zhu: Xi’an Jiaotong University
Xingbao Chen: Wuhan University of Technology
Rongyan Yang: College of Environmental Science and Engineering of Nankai University
Kailong Gu: Xi’an Jiaotong University
Lei Li: University of Science and Technology of China
Ching-Yu Chiang: National Synchrotron Radiation Research Center
Liqiang Mai: Wuhan University of Technology
Shenghua Chen: Xi’an Jiaotong University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Breaking the geometric symmetry of traditional metal-N4 sites and further boosting catalytic activity are significant but challenging. Herein, planar chlorination engineering is proposed for successfully converting the traditional Zn-N4 site with low activity and selectivity for CO2 reduction reaction (CO2RR) into highly active Zn-N3 site with broken symmetry. The optimal catalyst Zn-SA/CNCl-1000 displays a highest faradaic efficiency for CO (FECO) around 97 ± 3% and good stability during 50 h test at high current density of 200 mA/cm2 in zero-gap membrane electrode assembly (MEA) electrolyzer, with promising application in industrial catalysis. At -0.93 V vs. RHE, the partial current density of CO (JCO) and the turnover frequency (TOF) value catalyzed by Zn-SA/CNCl-1000 are 271.7 ± 1.4 mA/cm2 and 29325 ± 151 h-1, as high as 29 times and 83 times those of Zn-SA/CN-1000 without planar chlorination engineering. The in-situ extended X-ray absorption fine structure (EXAFS) measurements and density functional theory (DFT) calculation reveal the adjacent C-Cl bond induces the self-reconstruction of Zn-N4 site into the highly active Zn-N3 sites with broken symmetry, strengthening the adsorption of *COOH intermediate, and thus remarkably improving CO2RR activity.

Date: 2025
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DOI: 10.1038/s41467-025-56271-5

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