Issue 8, 2024

Highly efficient CO2 electrochemical reduction on dual metal (Co–Ni)–nitrogen sites

Abstract

The electrochemical reduction (ECR) of CO2 is a promising approach for CO2 removal and utilization, which is a critical component of the circular carbon economy. However, developing efficient and selective electrocatalysts is still challenging. Single-atom catalysts (SACs) have gained attention because they offer high metal atom utilization and uniform active sites. However, tuning the active metal centres to achieve high activity and selectivity in CO2 reduction remains a significant challenge. This study presents a novel electrocatalyst (Co–Ni–N–C) for CO2 ECR on the diatomic metal–nitrogen sites prepared through ion exchange using a zeolitic imidazolate framework (ZIF) as a precursor. During pyrolysis, nitrogen-doped graphitic carbon serves as the host material, anchoring the diatomic Co–Ni sites. The resulting bimetallic active sites demonstrate exceptional performance, achieving a high CO yield rate of 53.36 mA mgcat.−1 and an impressive CO faradaic efficiency of 94.1% at an overpotential of −0.27 V. Spectroscopic, microscopic, and density functional theory (DFT) analyses collectively unveil the crucial synergistic role of the Co–Ni–N6 moiety in promoting and sustaining exceptional electrocatalytic activities. The successful utilization of bimetallic sites in enhancing catalyst performance highlights the potential of this approach in developing efficient electrocatalysts for various other reactions.

Graphical abstract: Highly efficient CO2 electrochemical reduction on dual metal (Co–Ni)–nitrogen sites

Supplementary files

Article information

Article type
Paper
Submitted
18 Sep 2023
Accepted
17 Jan 2024
First published
18 Jan 2024
This article is Open Access
Creative Commons BY-NC license

J. Mater. Chem. A, 2024,12, 4601-4609

Highly efficient CO2 electrochemical reduction on dual metal (Co–Ni)–nitrogen sites

J. Chen, M. R. Ahasan, J. Oh, J. A. Tan, S. Hennessey, M. M. Kaid, H. M. El-Kaderi, L. Zhou, K. U. Lao, R. Wang and W. Wang, J. Mater. Chem. A, 2024, 12, 4601 DOI: 10.1039/D3TA05654F

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