How local electric field regulates C–C coupling at a single nanocavity in electrocatalytic CO2 reduction

Ruixin Yang, Yanming Cai, Yongbing Qi, Zhuodong Tang, Jun-Jie Zhu, Jinxiang Li, Wenlei Zhu () and Zixuan Chen ()
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Ruixin Yang: Nanjing University
Yanming Cai: Nanjing University
Yongbing Qi: Nanjing University
Zhuodong Tang: Nanjing University
Jun-Jie Zhu: Nanjing University
Jinxiang Li: Nanjing University
Wenlei Zhu: Nanjing University
Zixuan Chen: Nanjing University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract C–C coupling is of utmost importance in the electrocatalytic reduction of CO2, as it governs the selectivity of diverse product formation. Nevertheless, the difficulties to directly observe C–C coupling pathways at a specific nanocavity hinder the advances in catalysts and electrolyzer design for efficient high-value hydrocarbon production. Here we develop a nano-confined Raman technology to elucidate the influence of the local electric field on the evolution of C–C coupling intermediates. Through precise adjustments to the Debye length in nanocavities of a copper catalyst, the overlapping of electrical double layers drives a transition in the C–C coupling pathway at a specific nanocavity from *CHO–*CO coupling to the direct dimerization of *CO species. Experimental evidence and simulations validate that a reduced potential drop across the compact layer promotes a higher yield of CO and promotes the direct dimerization of *CO species. Our findings provide insights for the development of highly selective catalyst materials tailored to promote specific products.

Date: 2024
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DOI: 10.1038/s41467-024-51397-4

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