路易斯酸
选择性
光催化
离解(化学)
吸附
吉布斯自由能
化学键
金属
键离解能
电子转移
化学
键裂
无机化学
光化学
物理化学
催化作用
有机化学
热力学
物理
作者
Xiao Liu,Chengwei Yuan,Peng Chen,Yongyi Liu,Jianping Sheng,Shihan Zhang,Fan Dong,Yanjuan Sun
出处
期刊:ACS Sustainable Chemistry & Engineering
[American Chemical Society]
日期:2022-08-31
卷期号:10 (36): 11902-11912
被引量:20
标识
DOI:10.1021/acssuschemeng.2c02919
摘要
Due to the intrinsic chemically inert CO2 with the dissociation energy of C═O bond as high as 750 kJ mol–1, low efficiency and selectivity have become the most significant restraints for the practical application of photocatalytic CO2 reduction. Renewing the electronic structure of adsorbed CO2 on the catalyst surface through a rational catalyst design is crucial to achieving performance improvement. Herein, we prepared ZnIn2S4 and Cu-substituted ZnIn2S4 containing both Lewis acid and Lewis base sites as a model system for investigating the activation of CO2 by M–S chemical bonds (M represents a metal site). The Cu–S chemical bond can effectively activate CO2 as a vital electron channel and lower the Gibbs free energy for generating the essential intermediate *COOH. Besides, the Cu0.7-ZnIn2S4 sample displays 74.8% selectivity for reducing CO2 to CO with a rate of 47.2 μmol g–1 h–1, roughly 7.14 times that of ZnIn2S4.
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