Promoting electrocatalytic CO2 methanation using a molecular modifier on Cu surfaces

Cheng Wang; Xiangdong Kong; Junming Huang; Yu Yang; Han Zheng; Huijuan Wang; Suiyang Dai; Shuzhen Zhang; Yongxiang Liang; Zhigang Geng; Fengwang Li; Jie Zeng

doi:10.1039/D2TA07266A

Promoting electrocatalytic CO₂ methanation using a molecular modifier on Cu surfaces†

Cheng Wang,^a Xiangdong Kong,^a Junming Huang,^a Yu Yang,^b Han Zheng,^a Huijuan Wang,^a Suiyang Dai,^a Shuzhen Zhang,^b Yongxiang Liang,^a Zhigang Geng,

*^a Fengwang Li

*^b and Jie Zeng

*^a

Author affiliations

* Corresponding authors

^a Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, Experimental Center of Engineering and Material Science, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
E-mail: zengj@ustc.edu.cn, gengzg@ustc.edu.cn

^b School of Chemical and Biomolecular Engineering, The University of Sydney Nano Institute, The University of Sydney, NSW 2006, Australia
E-mail: fengwang.li@sydney.edu.au

Abstract

The electroreduction of CO₂ to methane using renewable energy is a promising approach to achieving carbon neutrality. At commercially relevant current densities (>200 mA cm⁻²), methane selectivity is however below 50%. Herein, we reported a benzenethiol-modified Cu nanoparticle catalyst that achieved a methane faradaic efficiency of 54.5% at a partial current density of 383 mA cm⁻², 1.9-fold higher than that of Cu nanoparticle controls. In situ vibrational spectroscopy and density functional theory calculations showed that the benzenethiol modulated the electronic structure of the Cu surface to enable a lowered coverage of *CO, favouring the formation of *CHO, a key intermediate embarking on the CH₄ pathway, over the competing carbon–carbon coupling, the pathway towards multicarbons.

Journal of Materials Chemistry A

Promoting electrocatalytic CO₂ methanation using a molecular modifier on Cu surfaces†

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Promoting electrocatalytic CO₂ methanation using a molecular modifier on Cu surfaces

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Journal of Materials Chemistry A