Effect of S vacancy in Cu3SnS4 on high selectivity and activity of photocatalytic CO2 reduction

被引:133
作者
Wang, Junyan [1 ]
Bo, Tingting [3 ]
Shao, Boyu [1 ]
Zhang, Yizhong [1 ]
Jia, Lixia [1 ]
Tan, Xin [1 ,4 ]
Zhou, Wei [3 ]
Yu, Tao [2 ,5 ]
机构
[1] Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300350, Peoples R China
[2] Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300350, Peoples R China
[3] Tianjin Univ, Sch Sci, Tianjin 300350, Peoples R China
[4] Tibet Univ, Sch Sci, Lhasa 850000, Peoples R China
[5] Tianjin Univ, Sch Mat Sci & Engn, TJU NIMS Int Collaborat Lab, Tianjin 300072, Peoples R China
基金
中国国家自然科学基金;
关键词
Photocatalytic CO2 reduction; S vacancy; Cu3SnS4; Density Functional Theory; CH4; CARBON-DIOXIDE; LIGHT; EFFICIENT; PHOTOREDUCTION; H2O; CH4; ACTIVATION; CU2O;
D O I
10.1016/j.apcatb.2021.120498
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Cu3SnS4 with S vacancy and different ratios of Cu(I/II) and Sn(II/IV) was designed for photocatalytic CO2 reduction with high selectivity and activity in this study. The conduction band (CB) position dominated by the Sn (II) 5p orbital of Cu3SnS4 could be regulated via controlling the content of Sn(II). Cu(I) and Sn(IV) in crystal lattice acted as the adsorption sites of CO2 and H2O as demonstrated by Density Functional Theory (DFT) calculations, meanwhile Cu(I) had a strong adsorption ability to CO, which was conducive to further protonation for CH4 generation (CO2 -> COOH*-> CO*-> CHO*-> CH2O*-> CH3O*-> CH4). S vacancy could result in the appearance of Cu(I) and Sn(II), which could successfully inhibit the electron-hole recombination and improve the reactivity (CH4 with yield of 22.65 mu mol/g/h) and selectivity (CH4 similar to 83.10 %). This work can shed some light on the synthetic method by controlling vacancy and elements to adjust CB position to increase reduction capability and selectivity.
引用
收藏
页数:10
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