The role of supported dual-atom on graphitic carbon nitride for selective and efficient CO2electrochemical reduction

Shuang Zhu; Kaiwei Wan; Hui Wang; Ling-Ju Guo; Xinghua Shi

doi:10.1088/1361-6528/ac0be5

The role of supported dual-atom on graphitic carbon nitride for selective and efficient CO₂electrochemical reduction

Nanotechnology. 2021 Jul 2;32(38). doi: 10.1088/1361-6528/ac0be5.

Authors

Shuang Zhu^{1

2}, Kaiwei Wan^{1

2}, Hui Wang^{1

2}, Ling-Ju Guo^{1

2}, Xinghua Shi^{1

2}

Affiliations

¹ Laboratory of Theoretical and Computational Nanoscience, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Chinese Academy of Sciences, Beijing 100190, People's Republic of China.
² University of Chinese Academy of Sciences, No. 19A Yuquan Road, Beijing 100049, People's Republic of China.

PMID: 34134090
DOI: 10.1088/1361-6528/ac0be5

Abstract

The electrochemical reduction of CO₂into value-added fuels and chemicals using single atom (SACs) or dual-atom catalysts (DACs) has been extensively studied, but the reaction mechanism and design rules are still unclear. Here, we studied the role of dual-metal atoms on graphite carbon nitride (M₁M₂@g-CN, M₁M₂ = CuCu, FeFe, RuRu, RuCu, RuFe, CuFe) for selective and efficient CO₂electrochemical reduction based on density functional theory. Our results show that CO₂RR on RuRu@g-CN catalyst prefers the *COOH pathway, while for CuCu@g-CN, FeFe@g-CN, RuCu@g-CN, RuFe@g-CN, CuFe@g-CN catalysts, the *OCHO pathway is more suitable. Among all the DACs combinations, we found that RuCu@g-CN and RuFe@g-CN are the most promising electrocatalysts for CO₂RR with a lower limiting potential, which is attributed to the synergistic effect of different O- and C-affinity of the heterocenters in DACs. The selectivity of RuCu@g-CN and RuFe@g-CN to the production of CH₄is better than that of H₂evolution. In addition, we also found that the adsorption free energy of intermediate on heteroatomic DACs can be predicted by those on homoatomic DACs, which can be used to further predict the limiting potential.

Keywords: CO2 electrochemical reduction; dual-atom catalysts; g-CN.