在硫化锡基电催化剂中，Sn
在硫化锡基电催化剂中，Sn-S 键强度强且均匀，可实现高效的 CO2 到甲酸盐转化
Science China Materials
(
IF
7.4
)
Pub Date : 2025-04-08
, DOI:
10.1007/s40843-025-3293-7
Guoyu Hou
,
Honghua Cui
,
Yicheng Li
,
Ya Liu
,
Zhenyi Yang
,
Ming Zhao
,
Zhong-Zhen Luo
,
Zhigang Zou
,
Yu Zhang
电化学 CO2 还原反应 （CO2RR） 代表了一种可持续的方法，可以缓解与过量排放 CO2 相关的全球担忧。最近，金属基硫化物作为一类用于高效甲酸盐生产的特殊电催化剂出现，然而，由于成分还原，它在 CO2RR 过程中遭受了大量的 S 损失。在此，我们合成了一系列具有高结晶度的硫化锡（即 SnS、Sn2S3 和 SnS2）作为模型催化剂，并揭示了原子构型中 Sn-S 键的强度分布对于高效甲酸盐生产至关重要。通常，SnS2 中强且均匀分布的 Sn-S 键有利于抑制 S 浸出并形成有利于 CO2RR 的 Sn/SnS2 异质界面，而 SnS 中较弱的 Sn-S 键促进还原为金属 Sn。特别是，具有混合键合强度的 Sn2S3 经历连续解离，从裂解最弱的 Sn-S 键开始，然后诱导加速还原。因此，SnS2 在 −1.0 VRHE 时实现了 93.8%±0.59% 的最高法拉第效率，在 −1.2 VRHE 时实现了 195.3 mA cm-2 的高部分电流密度。这项研究可以深入了解金属硫键在催化剂中的作用，以实现 CO2 到甲酸盐的高效转化。
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Strong and uniform Sn-S bond strength in tin sulfides-based electrocatalysts enables efficient CO2-to-formate conversion
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 VRHE and a high partial current density of 195.3 mA cm−2 at −1.2 VRHE. This study could provide insight into the role of metal-sulfur bonds in catalysts for efficient CO2-to-formate conversion.
更新日期：2025-04-08
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