Issue 47, 2022

An accurate “metal pre-buried” strategy for constructing Ni–N2C2 single-atom sites with high metal loadings toward electrocatalytic CO2 reduction

Abstract

Although single-atom catalysts (SACs) dispersed on N-doped carbon supports with the M–N2C2 configuration have high application potential in electrocatalysis, combining this configuration with high metal loadings remains a considerable challenge. In this study, a Ni-salen polymer with a confined metal position and precise coordination mode (Ni–N2O2) serves as a precursor, which not only suppresses the aggregation of metal atoms but also promotes the creation of Ni–N2C2 centers owing to the cleavage of Ni–O bonds and formation of Ni–C bonds during high-temperature pyrolysis. A Ni–N2C2 SAC with a metal loading of 9.15 wt% exhibits excellent catalytic performance for the CO2 electroreduction to CO with a faradaic efficiency (FECO) of 98.7% at −0.82 V vs. the reversible hydrogen electrode (RHE). Theoretical calculation data have further demonstrated that the modified electronic structure of the Ni–N2C2-p model is responsible for its high intrinsic activity. This work proposes a new strategy for maintaining both the precise Ni–N2C2 structure and high metal loading.

Graphical abstract: An accurate “metal pre-buried” strategy for constructing Ni–N2C2 single-atom sites with high metal loadings toward electrocatalytic CO2 reduction

Supplementary files

Article information

Article type
Paper
Submitted
10 set 2022
Accepted
04 nov 2022
First published
04 nov 2022

J. Mater. Chem. A, 2022,10, 25047-25054

An accurate “metal pre-buried” strategy for constructing Ni–N2C2 single-atom sites with high metal loadings toward electrocatalytic CO2 reduction

X. Liu, L. Liao, G. Xia, F. Yu, G. Zhang, M. Shu and H. Wang, J. Mater. Chem. A, 2022, 10, 25047 DOI: 10.1039/D2TA07135E

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