纳米团簇
电催化剂
过电位
法拉第效率
硫黄
电化学
材料科学
格式化
无机化学
催化作用
化学工程
锡
选择性
化学
纳米技术
电极
物理化学
有机化学
冶金
工程类
作者
Xin Wang,Fengli Li,Yin Wang,Yubing Si,Ming Miao,Yongzhu Fu
标识
DOI:10.1016/j.apcatb.2021.120936
摘要
Electrochemical CO2 conversion into fuels is highly desirable to achieve carbon artificial cycles. Among electrocatalyst candidates, earth-abundant tin is subject to unsatisfied efficiency and selectivity. In this work, atomically-dispersed Sn nanoclusters modified with the trace of sulfur doping are proposed to efficiently electroreduce CO2 to C1 chemicals. This electrocatalyst is in situ derived from bis(benzene-1,2-dithiolato). It exhibits a high Faradaic efficiency (90%) for carbonaceous products at a moderate overpotential (0.75 V). Importantly, it is exploited for the formate formation with unprecedented partial current density (90 mA cm−2) and long-term stability (50 h) using the flow cell, better than most Sn-based catalysts. Electrochemical experiments and theoretical calculations manifest the promoting effect of trace sulfur on Sn nanoclusters, which stabilizes the *HCOOH intermediate and favors CO2 electroreduction. Hence, it emphasizes the importance of dopants and charge modulating for performance enhancement. This work unfolds a promising candidate for Sn electrocatalysts towards CO2 electroreduction.
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