Regulating reconstruction of oxide-derived Cu for electrochemical CO <sub>2</sub> reduction toward n-propanol
Chang Long, X.L. Liu, Kaiwei Wan, Yuheng Jiang, Pengfei An, Caoyu Yang, Guoling Wu, Wenyang Wang, Jun Guo, Lei Li, Kanglei Pang, Qun Li, Chunhua Cui, Shaoqin Liu, Ting Tan, Zhiyong Tang
Abstract
Oxide-derived copper (OD-Cu) is the most efficient and likely practical electrocatalyst for CO 2 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 Cu 2 O 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 Cu 2 O-derived Cu (Cu 2 OD-Cu) because of the vigorous oxygen removal. In situ spectroscopes disclose that the coordination number of CuOD-Cu is considerably lower than that of Cu 2 OD-Cu, enabling the fast kinetics of CO 2 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 ~17.9%, whereas the Cu 2 OD-Cu dominantly generates formate.