Tuning Multi‐Active Sites in Cu Catalyst via Ag/Ni Doping for Enhanced CO <sub>2</sub> Electroreduction to C <sub>2+</sub> Products
Shuaiqiang Jia, Hailian Cheng, Qinggong Zhu, Xiao Chen, Cheng Xue, Ting Deng, Mengke Dong, Zhanghui Xia, Jiapeng Jiao, Chunjun Chen, Haihong Wu, Mingyuan He, Buxing Han
Abstract
Abstract Electrochemical CO 2 reduction (ECR) to C 2+ products is a promising sustainable carbon conversion pathway, yet simultaneously achieving high Faradaic efficiency (FE) and current density remains a challenge. Herein, we found that creating Cu‐Ag‐Ni multi‐metal sites could effectively modulate the adsorption energies of *H and *CO on the catalyst surface, thereby achieving highly efficient ECR to synthesize C 2+ products. In situ measurements coupling theoretical calculations indicated that by systematically altering the spatial arrangement and distribution of active sites in Cu‐Ag‐Ni catalysts, the electronic structure and the local *CO coverage on the Cu surface could be tuned, consequently steering the ECR to C 2+ pathway. In particular, Cu‐Ag‐Ni catalyst with dispersed multi‐sites (Cu x AgNi DNPs) could more effectively reduce the energy barrier for C─C coupling than Cu‐Ag‐Ni catalyst with phase‐separated multi‐sites (Cu x AgNi PNPs). As a result, the Cu 40 AgNi DNPs catalyst with dispersed multi‐sites yielded C 2+ products with a FE of 93.2% and a current density up to 818.1 mA cm −2 at −1.38 V versus reversible hydrogen electrode (vs. RHE), which are higher than most reported up to date for C 2+ production. This work provides a methodology for designing robust multi‐metallic ECR catalysts with tailored multi‐active site configurations.