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Electrochemical CO2 reduction reaction (CO2RR) represents a sustainable approach to alleviate the global concern associated with excessive CO2 emission. Recently, metal-based sulfides are emerged as a special class of electrocatalysts for efficient formate production, which however suffer from massive S loss during CO2RR due to the compositional reduction. Herein, we synthesize a series of tin sulfides with high crystallinity (i.e., SnS, Sn2S3, and SnS2) as model catalysts, and reveal that the strength distribution of Sn-S bonds in atomic configurations is essential for efficient formate production. Typically, the strong and uniformly distributed Sn-S bonds in SnS2 are beneficial for inhibiting S leaching and forming favorable Sn/SnS2 heterointerfaces for CO2RR, while the weaker Sn-S bonds in SnS promote the reduction into metallic Sn. Specially, the Sn2S3 with mixed bonding strengths undergoes consecutive dissociation, starting from cleaving the weakest Sn-S bonds and then inducing accelerative reduction. Resultantly, the SnS2 achieves the highest Faraday efficiency of 93.8%+/- 0.59% at -1.0 V-RHE and a high partial current density of 195.3 mA cm(-2) at -1.2 V-RHE. This study could provide insight into the role of metal-sulfur bonds in catalysts for efficient CO2-to-formate conversion.
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SCIENCE CHINA-MATERIALS
ISSN: 2095-8226
Year: 2025
Issue: 5
Volume: 68
Page: 1602-1610
6 . 8 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 3
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