Manipulating local coordination of copper single atom catalyst enables efficient CO2-to-CH4 conversion

Yizhou Dai, Huan Li, Chuanhao Wang, Weiqing Xue, Menglu Zhang, Donghao Zhao, Jing Xue, Jiawei Li, Laihao Luo, Chunxiao Liu, Xu Li, Peixin Cui, Qiu Jiang, Tingting Zheng, Songqi Gu, Yao Zhang, Jianping Xiao (), Chuan Xia () and Jie Zeng ()
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Yizhou Dai: University of Science and Technology of China
Huan Li: Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences
Chuanhao Wang: University of Science and Technology of China
Weiqing Xue: University of Science and Technology of China
Menglu Zhang: University of Science and Technology of China
Donghao Zhao: University of Science and Technology of China
Jing Xue: University of Science and Technology of China
Jiawei Li: University of Science and Technology of China
Laihao Luo: University of Science and Technology of China
Chunxiao Liu: University of Electronic Science and Technology of China
Xu Li: University of Electronic Science and Technology of China
Peixin Cui: Institute of Soil Science, Chinese Academy of Sciences
Qiu Jiang: University of Electronic Science and Technology of China
Tingting Zheng: University of Electronic Science and Technology of China
Songqi Gu: Chinese Academy of Sciences
Yao Zhang: University of Science and Technology of China
Jianping Xiao: Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences
Chuan Xia: University of Electronic Science and Technology of China
Jie Zeng: University of Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract Electrochemical CO2 conversion to methane, powered by intermittent renewable electricity, provides an entrancing opportunity to both store renewable electric energy and utilize emitted CO2. Copper-based single atom catalysts are promising candidates to restrain C-C coupling, suggesting feasibility in further protonation of CO* to CHO* for methane production. In theoretical studies herein, we find that introducing boron atoms into the first coordination layer of Cu-N4 motif facilitates the binding of CO* and CHO* intermediates, which favors the generation of methane. Accordingly, we employ a co-doping strategy to fabricate B-doped Cu-Nx atomic configuration (Cu-NxBy), where Cu-N2B2 is resolved to be the dominant site. Compared with Cu-N4 motifs, as-synthesized B-doped Cu-Nx structure exhibits a superior performance towards methane production, showing a peak methane Faradaic efficiency of 73% at −1.46 V vs. RHE and a maximum methane partial current density of −462 mA cm−2 at −1.94 V vs. RHE. Extensional calculations utilizing two-dimensional reaction phase diagram analysis together with barrier calculation help to gain more insights into the reaction mechanism of Cu-N2B2 coordination structure.

Date: 2023
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DOI: 10.1038/s41467-023-39048-6

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