posted on 2024-02-10, 14:12authored byChang Long, Kaiwei Wan, Yu Chen, Lei Li, Yuheng Jiang, Caoyu Yang, Qianbao Wu, Guoling Wu, Peng Xu, Jiong Li, Xinghua Shi, Zhiyong Tang, Chunhua Cui
As
fuel and an important chemical feedstock, n-propanol
is highly desired in electrochemical CO2/CO
reduction on Cu catalysts. However, the precise regulation of the
Cu localized structure is still challenging and poorly understood,
thus hindering the selective n-propanol electrosynthesis.
Herein, by decorating Au nanoparticles (NPs) on CuO nanosheets (NSs),
we present a counterintuitive transformation of CuO into undercoordinated
Cu sites locally around Au NPs during CO reduction. In situ spectroscopic
techniques reveal the Au-steered formation of abundant undercoordinated
Cu sites during the removal of oxygen on CuO. First-principles accuracy
molecular dynamic simulation demonstrates that the localized Cu atoms
around Au tend to rearrange into disordered layer rather than a Cu
(111) close-packed plane observed on bare CuO NSs. These Au-steered
undercoordinated Cu sites facilitate CO binding, enabling selective
electroreduction of CO into n-propanol with a high
Faradaic efficiency of 48% in a flow cell. This work provides new
insight into the regulation of the oxide-derived catalysts reconstruction
with a secondary metal component.