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, Jian-Hui Wang, Jie Zhou, Shun-Li Li and Ya-Qian Lan ()
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Yu Zhang: Nanjing Normal University
Long-Zhang Dong: Nanjing Normal University
Shan Li: Nanjing Normal University
Xin Huang: Nanjing Normal University
Jia-Nan Chang: Nanjing Normal University
Jian-Hui Wang: Nanjing Normal University
Jie Zhou: South China Normal University
Shun-Li Li: Nanjing Normal University
Ya-Qian Lan: Nanjing Normal University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract The electrochemical CO2 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 CH4 with superior activity and selectivity, showing a Faradaic efficiency of CH4 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-O4 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.

Date: 2021
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DOI: 10.1038/s41467-021-26724-8

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