Coordination environment dependent selectivity of single-site-Cu enriched crystalline porous catalysts in CO2 reduction to CH4
Yu Zhang, Long‐Zhang Dong, Shan Li, Xin Huang, Jia‐Nan Chang, Jianhui Wang, Jie Zhou, Shun‐Li Li, Ya‐Qian Lan
Abstract
Abstract The electrochemical CO 2 reduction to high-value-added chemicals is one of the most promising and challenging research in the energy conversion field. An efficient ECR catalyst based on a Cu-based conductive metal-organic framework (Cu-DBC) is dedicated to producing CH 4 with superior activity and selectivity, showing a Faradaic efficiency of CH 4 as high as ~80% and a large current density of −203 mA cm −2 at −0.9 V vs. RHE. The further investigation based on theoretical calculations and experimental results indicates the Cu-DBC with oxygen-coordinated Cu sites exhibits higher selectivity and activity over the other two crystalline ECR catalysts with nitrogen-coordinated Cu sites due to the lower energy barriers of Cu-O 4 sites during ECR process. This work unravels the strong dependence of ECR selectivity on the Cu site coordination environment in crystalline porous catalysts, and provides a platform for constructing highly selective ECR catalysts.