Pyrolysis-free synthesis of a high-loading single-atom Cu catalyst for efficient electrocatalytic CO2-to-CH4 conversion

Jiawei Li; Yawen Jiang; Jiayi Li; Xinyu Wang; Hengjie Liu; Ning Zhang; Ran Long; Yujie Xiong

doi:10.1039/d3nr05228a

Pyrolysis-free synthesis of a high-loading single-atom Cu catalyst for efficient electrocatalytic CO₂-to-CH₄ conversion

Nanoscale. 2023 Dec 21;16(1):171-179. doi: 10.1039/d3nr05228a.

Authors

Jiawei Li^{1

2}, Yawen Jiang³, Jiayi Li¹, Xinyu Wang^{1

2}, Hengjie Liu¹, Ning Zhang^{1

2}, Ran Long¹, Yujie Xiong^{1

2}

Affiliations

¹ National Synchrotron Radiation Laboratory, Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, Anhui 230026, China. [email protected].
² Sustainable Energy and Environmental Materials Innovation Center, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, Jiangsu 215123, China.
³ Deep Space Exploration Laboratory, Hefei, Anhui 230026, China.

PMID: 38086688
DOI: 10.1039/d3nr05228a

Abstract

Electrocatalytic CO₂-to-CH₄ conversion provides a promising means of addressing current carbon resource recycling and intermittent energy storage. Cu-based single-atom catalysts have attracted extensive attention owing to their high intrinsic activity toward CH₄ production; however, they suffer from uncontrollable metal loading and aggregation during the conventional pyrolysis process of carbon-based substrates. Herein, we developed a pyrolysis-free method to prepare a single-atom Cu catalyst anchored on a formamide polymer substrate with a high loading amount and well atomic dispersion through a mild polycondensation reaction. Owing to the isolation of copper active sites, efficient CO₂-to-CH₄ conversion is achieved over the single-atom Cu catalyst, along with the significant suppression of C-C coupling. As a result, the optimal single-atom catalyst with 5.87 wt% of Cu offers high CH₄ faradaic efficiencies (FEs) of over 70% in a wide current density range from 100 to 600 mA cm^-2 in the flow cell, together with a maximum CH₄ partial current density of 415.8 mA cm^-2. Moreover, the CH₄ FE can reach 74.2% under optimized conditions in a membrane electrode assembly electrolyzer. This work provides new insights into the subtle design of highly efficient electrocatalyst for CO₂ reduction.