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Insight into coupled Ni-Co dual-metal atom catalysts for efficient synergistic electrochemical CO_(2)reduction

Journal of Energy Chemistry 2023年第12期87卷 509-517,I0013页

作者： Qingchun Zhang Di Liu Yaping Zhang Zhiliang Guo Minpeng Chen Yuyun Chen Bo Jin Yingze Song Hui Pan State Key Laboratory of Environment-Friendly Energy Materials School of Materials and ChemistryTianfu Institute of Research and InnovationSouthwest University of Science and TechnologyMianyang 621010SichuanChina Institute of Applied Physics and Materials Engineering University of MacaoMacao 999078China School of Chemistry and Chemical Engineering Southeast UniversityNanjing 211189JiangsuChina

The development of highly active,selective,and stable electrocatalysts can facilitate the effective implementation of electrocatalytic CO_(2)conversion into fuels or chemicals for mitigating the energy crisis and climate ***,it is necessary to achieve the goal through reasonable material design based on the actuality of the operational active site at the molecular *** by the stimulating synergistic effect of coupled heteronuclear metal atoms,a novel Ni-Co atomic pairs configuration(denoted as NiN_(3)?CoN_(3)-NC)active site was theoretically screened out for improving electrochemical CO_(2)reduction reaction(CO_(2)RR).The structure of NiN_(3)?CoN_(3)-NC was finely regulated by adjusting Zn content in the precursors Zn/Co/Ni-zeolite imidazolate frameworks(Zn/Co/Ni-ZIFs)and pyrolysis *** structural features of NiN_(3)?CoN_(3)-NC were systematically confirmed by aberration-corrected HAADF-STEM coupled with 3D atom-overlapping Gaussian-function fitting mapping,XAFS,and *** results of theoretical calculations reveal that the synergistic effect of Ni-Co atomic pairs can effectively promote the*COOH intermediate formation and thus the overall CO_(2)RR kinetic was improved,and also restrained the competitive hydrogen evolution *** to the attributes of Ni-Co atomic pairs configuration,the developed NiN_(3)?CoN_(3)-NC with superior catalytic activity,selectivity,and durability,with a high turnover frequency of 2265 h^(-1)at-1.1 V(***)and maximum Faradaic efficiency of 97.7%for CO *** work demonstrates the great potential of DACs as highly efficient catalysts for CO_(2)RR,provides a useful strategy to design heteronuclear DACs,exploits the synergistic effect of multiple metal sites to facilitate complex CO_(2)RR catalytic reactions,and inspires more efforts to develop the potential of DACs in various fields.

关键词： coupled dual-metal atom catalysts CO_(2)reduction reaction Electrocatalysts Density functional theory

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