Charge redistribution dynamics in chalcogenide-stabilized cuprous electrocatalysts unleash ampere-scale partial current toward formate production

Feng-Ze Tian, Wen-Jui Chang, Pei-Jung Liang, Yi-An Lai, Chia-Shuo Hsu, Sheng-Chih Lin, Yu-Hsin Chen, You-Chiuan Chu, Shih-Wen Huang (), Hui-Lung Chen () and Hao Ming Chen ()
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Feng-Ze Tian: National Taiwan University
Wen-Jui Chang: National Taiwan University
Pei-Jung Liang: National Taiwan University
Yi-An Lai: National Taiwan University
Chia-Shuo Hsu: National Synchrotron Radiation Research Center
Sheng-Chih Lin: National Taiwan University
Yu-Hsin Chen: National Taiwan University
You-Chiuan Chu: National Taiwan University
Shih-Wen Huang: Paul Scherrer Institute
Hui-Lung Chen: Chinese Cultural University
Hao Ming Chen: National Taiwan University

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Electrochemical CO2 reduction to formate offers a sustainable route, but achieving high selectivity on transition metal catalysts remains a significant challenge, which is typically favored on p-block metals. Here, we demonstrate that chalcogenide-stabilized cuprous enables near-complete formate selectivity through a charge redistribution mechanism induced by chalcogenides. Using in situ X-ray absorption spectroscopy, high-energy-resolution fluorescence-detected XAS, Raman, and infrared spectroscopy, we reveal that Cu-chalcogen interactions stabilize Cu+, preventing over-reduction to Cu0 and thereby modulating CO2 adsorption and intermediate binding. This stabilization enhances the *OCHO pathway, shifting product distribution entirely toward formate. CuS exhibits the highest selectivity, achieving a notable 90% faradaic efficiency at −0.6 V and an ampere-scale formate partial current of 1.36 A, demonstrating industrial feasibility. In contrast, CuO, lacking a charge redistribution effect, promotes a mixture of CO and C2 products, underscoring the critical role of chalcogenides in steering product selectivity. This work provides fundamental insights into charge redistribution in CO2RR and introduces a catalyst design strategy leveraging chalcogen-induced electronic modifications for scalable formate production.

Date: 2025
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DOI: 10.1038/s41467-025-64472-1

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