Issue 11, 2022

Construction of single-atom copper sites with low coordination number for efficient CO2 electroreduction to CH4

Abstract

Generally speaking, the preparation of single-atom catalysts always requires harsh conditions such as high-temperature pyrolysis or strong acid etching. In this manuscript, a simple and effective plasma-activated strategy is employed to synthesize a MOF-based single-atom copper catalyst. The bombardment of plasma forms abundant oxygen vacancies and significantly increases the number of low-coordinated catalytically active copper sites. Moreover, plasma treatment also creates a hierarchically porous structure, which can effectively adsorb the reactant molecules. The synergistic effect of the porous structure and low-coordinated copper sites dramatically improves the activity of CO2 electroreduction to CH4 with a maximum faradaic efficiency of 75.3%. Furthermore, the total faradaic efficiency of carbon-containing products (CO, CH4 and C2H4) can reach as high as 96.5% with a partial current density of 47.8 mA cm−2. Density functional theory (DFT) calculations confirm that the low-coordinated copper sites can be beneficial for the formation and further reduction of the key intermediate to CH4. This strategy provides a successful example for the preparation of single-atom catalysts under mild conditions.

Graphical abstract: Construction of single-atom copper sites with low coordination number for efficient CO2 electroreduction to CH4

Supplementary files

Article information

Article type
Paper
Submitted
30 Sept. 2021
Accepted
07 Dec. 2021
First published
08 Dec. 2021

J. Mater. Chem. A, 2022,10, 6187-6192

Construction of single-atom copper sites with low coordination number for efficient CO2 electroreduction to CH4

S. Wei, X. Jiang, C. He, S. Wang, Q. Hu, X. Chai, X. Ren, H. Yang and C. He, J. Mater. Chem. A, 2022, 10, 6187 DOI: 10.1039/D1TA08494A

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