1. Regulating reconstruction of oxide-derived Cu for electrochemical CO2 reduction toward n-propanol
- Author
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Long, Chang, Liu, Xiaolong, Wan, Kaiwei, Jiang, Yuheng, An, Pengfei, Yang, Caoyu, Wu, Guoling, Wang, Wenyang, Guo, Jun, Li, Lei, Pang, Kanglei, Li, Qun, Cui, Chunhua, Liu, Shaoqin, Tan, Ting, Tang, Zhiyong, Long, Chang, Liu, Xiaolong, Wan, Kaiwei, Jiang, Yuheng, An, Pengfei, Yang, Caoyu, Wu, Guoling, Wang, Wenyang, Guo, Jun, Li, Lei, Pang, Kanglei, Li, Qun, Cui, Chunhua, Liu, Shaoqin, Tan, Ting, and Tang, Zhiyong
- Abstract
Oxide-derived copper (OD-Cu) is the most efficient and likely practical electrocatalyst for CO2 reduction toward multicarbon products. However, the inevitable but poorly understood reconstruction from the pristine state to the working state of OD-Cu under strong reduction conditions largely hinders the rational construction of catalysts toward multicarbon products, especially C-3 products like n-propanol. Here, we simulate the reconstruction of CuO and Cu2O into their derived Cu by molecular dynamics, revealing that CuO-derived Cu (CuOD-Cu) intrinsically has a richer population of undercoordinated Cu sites and higher surficial Cu atom density than the counterpart Cu2O-derived Cu (Cu2OD-Cu) because of the vigorous oxygen removal. In situ spectroscopes disclose that the coordination number of CuOD-Cu is considerably lower than that of Cu2OD-Cu, enabling the fast kinetics of CO2 reaction and strengthened binding of *C-2 intermediate(s). Benefiting from the rich undercoordinated Cu sites, CuOD-Cu achieves remarkable n-propanol faradaic efficiency up to similar to 17.9%, whereas the Cu2OD-Cu dominantly generates formate.
- Published
- 2023
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