Dynamic Stability of Copper Single-Atom Catalysts under Working Conditions

• DOI: 10.1021/jacs.2c07178
• Publication Date: 2022-09-12T04:51:13Z
• Authors: Xiaowan Bai; Xunhua Zhao; Yehui Zhang; Chongyi Ling; Yipeng Zhou; Jinlan Wang; Yuanyue Liu
• Keywords: 01 natural sciences; 0104 chemical sciences

The long-term stability of single-atom catalysts is a major factor affecting their large-scale commercial application. How to evaluate the dynamic under working conditions still lacking. Here, taking single copper atom embedded in N-doped graphene as an example, "constant-potential hybrid-solvation model" used reversible transformation between atoms and clusters realistic reaction conditions. It revealed that adsorption H vital driving force for leaching Cu from catalyst surface. more negative electrode potential, stronger H. As result, competitive hydrogen evolution inhibited, Cu-N bonds are weakened, resulting some being tethered on surface dissolved aqueous solution. collision two states forms transient cluster structure true catalytic active site promote CO2 reduction ethanol. applied potential released or switched positive value, hydroxyl radicals (OH•) play dominant role oxidation process cluster, then returns initial atomic dispersion state by redeposition, completing reconstruction cycle catalyst. Our work provides fundamental understanding at level calls reassessment currently reported considering