格式化
催化作用
密度泛函理论
材料科学
纳米材料
可逆氢电极
法拉第效率
表面改性
氢
电化学
无机化学
化学
电极
化学工程
纳米技术
物理化学
计算化学
有机化学
工程类
参比电极
作者
An Zhang,Yongxiang Liang,Huiping Li,Shilong Wang,Qixuan Chang,Kaiyue Peng,Zhigang Geng,Jie Zeng
出处
期刊:Nano Letters
[American Chemical Society]
日期:2021-08-30
卷期号:21 (18): 7789-7795
被引量:32
标识
DOI:10.1021/acs.nanolett.1c02757
摘要
Surface functionalization with atoms serves as an important strategy to modulate the catalytic activities of low-dimensional nanomaterials. Herein, we developed a facile hydrogen incorporation strategy for improving the catalytic activities of SnS2 nanosheets toward CO2 electroreduction. Compared with SnS2 nanosheets, the hydrogen-incorporated SnS2 (denoted as H-SnS2) nanosheets exhibited high current density and Faradaic efficiency (FE) for formate. At −0.9 V vs RHE, H-SnS2 nanosheets displayed a maximum FE of 93% for carbonaceous product, which rivals the activities of most Sn-based catalysts in CO2 electroreduction. Mechanistic studies disclosed that the incorporation of surface hydrogen induced the electron injection into the structures of H-SnS2 nanosheets, which largely facilitates the process of CO2 activation. Density functional theory (DFT) calculations further revealed that hydrogen incorporation decreased the energy barrier for the formation of HCOO* intermediates, thus contributing to the CO2-to-formate conversion on H-SnS2 nanosheets.
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