Tuning Multi‐Active Sites in Cu Catalyst via Ag/Ni Doping for Enhanced CO <sub>2</sub> Electroreduction to C <sub>2+</sub> Products
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.
Article Details
Authors (13)
Shuaiqiang Jia
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Hailian Cheng
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Qinggong Zhu
Institute of Chemistry, Chinese Academy of Sciences , , ,
Xiao Chen
Cheng Xue
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Ting Deng
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Mengke Dong
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Zhanghui Xia
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Jiapeng Jiao
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Chunjun Chen
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Haihong Wu
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Mingyuan He
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,