Unveiling hydrocerussite as an electrochemically stable active phase for efficient carbon dioxide electroreduction to formate

Yanmei Shi, Yan Ji, Jun Long, Yu Liang, Yang Liu, Yifu Yu, Jianping Xiao () and Bin Zhang ()
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Yanmei Shi: Tianjin University
Yan Ji: Tianjin University
Jun Long: University of Chinese Academy of Sciences
Yu Liang: Tianjin University
Yang Liu: Tianjin University
Yifu Yu: Tianjin University
Jianping Xiao: University of Chinese Academy of Sciences
Bin Zhang: Tianjin University

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract For most metal-containing CO2 reduction reaction (CO2RR) electrocatalysts, the unavoidable self-reduction to zero-valence metal will promote hydrogen evolution, hence lowering the CO2RR selectivity. Thus it is challenging to design a stable phase with resistance to electrochemical self-reduction as well as high CO2RR activity. Herein, we report a scenario to develop hydrocerussite as a stable and active electrocatalyst via in situ conversion of a complex precursor, tannin-lead(II) (TA-Pb) complex. A comprehensive characterization reveals the in situ transformation of TA-Pb to cerussite (PbCO3), and sequentially to hydrocerussite (Pb3(CO3)2(OH)2), which finally serves as a stable and active phase under CO2RR condition. Both experiments and theoretical calculations confirm the high activity and selectivity over hydrocerussite. This work not only offers a new approach of enhancing the selectivity in CO2RR by suppressing the self-reduction of electrode materials, but also provides a strategy for studying the reaction mechanism and active phases of electrocatalysts.

Date: 2020
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DOI: 10.1038/s41467-020-17120-9

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