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

For most metal-containing CO 2 reduction reaction (CO 2 RR) electrocatalysts, the unavoidable self-reduction to zero-valence metal will promote hydrogen evolution, hence lowering the CO 2 RR selectivity. Thus it is challenging to design a stable phase with resistance to electrochemical self-reductio...

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Bibliographic Details
Published in:Nature communications 2020-07, Vol.11 (1), p.3415-3415, Article 3415
Main Authors: Shi, Yanmei, Ji, Yan, Long, Jun, Liang, Yu, Liu, Yang, Yu, Yifu, Xiao, Jianping, Zhang, Bin
Format: Article
Language:English
Subjects:
140/133
140/146
639/301/299/886
639/638/224/685
639/638/77/886
Carbon dioxide
Catalysts
Chemical reduction
Electrocatalysts
Electrochemistry
Electrode materials
Electrowinning
Humanities and Social Sciences
Hydrogen evolution
Lead
multidisciplinary
Reaction mechanisms
Science
Science (multidisciplinary)
Selectivity
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Summary:For most metal-containing CO 2 reduction reaction (CO 2 RR) electrocatalysts, the unavoidable self-reduction to zero-valence metal will promote hydrogen evolution, hence lowering the CO 2 RR selectivity. Thus it is challenging to design a stable phase with resistance to electrochemical self-reduction as well as high CO 2 RR 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 (PbCO 3 ), and sequentially to hydrocerussite (Pb 3 (CO 3 ) 2 (OH) 2 ), which finally serves as a stable and active phase under CO 2 RR 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 CO 2 RR by suppressing the self-reduction of electrode materials, but also provides a strategy for studying the reaction mechanism and active phases of electrocatalysts. While electrochemical CO2 reduction represents a renewable means to produce high-value products, catalyst transformation may compete with desirable processes. Here, authors prevent catalyst self-reduction during CO2 electroreduction and show stable, formate-selective performances of hydrocerussite.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-020-17120-9