Operando evidence of Cu⁺ stabilization via a single-atom modifier for CO₂ electroreduction

Zhang, Wei; He, Peng; Wang, Chao; Ding, Tao; Chen, Tao; Liu, Xiaokang; Cao, Linlin; Huang, Tianming; Shen, Xinyi; Usoltsev, Oleg A.; Bugaev, Aram L.; Lin, Yue; Yao, Tao

Operando evidence of Cu⁺ stabilization via a single-atom modifier for CO₂ electroreduction

2020

Oxide-derived Cu materials are most commonly used as electrocatalysts for the carbon dioxide reduction reaction (CO₂RR). Previous studies have proved that Cu⁺ and residual subsurface oxygen species can enhance the CO₂RR activity; however the stable presence of Cu⁺ remains a subject of debate. Here, we design a strategy of single-atom Sn anchored on Cu₂O nanosheets to stabilize the key Cu⁺ species for electroreduction of CO₂. Operando synchrotron X-ray absorption spectroscopy and statistics analysis distinguish the active Cu⁺ and reduced Cu⁺ species, and reveal that the constructed Sn–O–Cu sites with charge transfer can significantly enhance the resistance of copper oxides to reduction. Operando infrared spectroscopy suggests that the survival of Cu⁺ species on the catalyst surface promotes the adsorption of *CO during the CO₂RR, leading to the obvious improvement of CO₂-to-CO conversion. Our results demonstrate the role of a single-atom-modifier in both stabilizing Cu⁺ species and enhancing the CO₂RR selectivity of oxide-derived Cu catalysts.

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