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Promoting Electrochemical CO 2 Reduction to Formate via Sulfur‐Assisted Electrolysis
Author(s) -
Liu Yuhang,
Wei Zhiming,
Su Xiaozhi,
Shi Xiuwen,
Liu Lingyue,
Wang Tianyu,
Xu Xueting,
Zhao Ming,
Zhai Yueming,
Yang Hong Bin,
Liu Bin
Publication year - 2025
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.202403547
Abstract Electrochemical CO 2 reduction reaction (CO 2 RR) provides a renewable approach to transform CO 2 to produce chemicals and fuels. Unfortunately, it faces the challenges of sluggish CO 2 activation and slow water dissociation. This study reports the modification of Bi‐based electrocatalyst by S, which leads to a remarkable enhancement in activity and selectivity during electrochemical CO 2 reduction to formate. Based on comprehensive in situ examinations and kinetic evaluations, it is observed that the presence of S species over Bi catalyst can significantly enhance its interaction with K + (H 2 O) n , facilitating fast dissociation of water molecules to generate protons. Further in situ attenuated total reflectance surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS) and in situ Raman spectroscopy measurements reveal that S modification is able to decrease the oxidation state of Bi active site, which can effectively enhance CO 2 activation and facilitate HCOO * intermediate formation while suppressing competing hydrogen evolution reaction. Consequently, the S‐modified Bi catalyst achieves impressive electrochemical CO 2 RR performance, reaching a formate Faradaic efficiency (FE formate ) of 91.2% at a formate partial current density of ≈135 mA cm −2 and a potential of −0.8 V versus RHE in an alkaline electrolyte.