Manipulating local coordination of copper single atom catalyst enables efficient CO 2 -to-CH 4 conversion

Electrochemical CO conversion to methane, powered by intermittent renewable electricity, provides an entrancing opportunity to both store renewable electric energy and utilize emitted CO . Copper-based single atom catalysts are promising candidates to restrain C-C coupling, suggesting feasibility in...

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Bibliographic Details
Published in:Nature communications 2023-06, Vol.14 (1), p.3382
Main Authors: Dai, Yizhou, Li, Huan, Wang, Chuanhao, Xue, Weiqing, Zhang, Menglu, Zhao, Donghao, Xue, Jing, Li, Jiawei, Luo, Laihao, Liu, Chunxiao, Li, Xu, Cui, Peixin, Jiang, Qiu, Zheng, Tingting, Gu, Songqi, Zhang, Yao, Xiao, Jianping, Xia, Chuan, Zeng, Jie
Format: Article
Language:English
Subjects:
Boron
Carbon Dioxide
Copper
Electricity
Methane
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Summary:Electrochemical CO conversion to methane, powered by intermittent renewable electricity, provides an entrancing opportunity to both store renewable electric energy and utilize emitted CO . 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-N 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-N atomic configuration (Cu-N B ), where Cu-N B is resolved to be the dominant site. Compared with Cu-N motifs, as-synthesized B-doped Cu-N 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 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-N B coordination structure.
ISSN:2041-1723