General strategy for enhanced CH4 selectivity in photocatalytic CO2 reduction reactions by surface oxophilicity engineering
General strategy for enhanced CH4 selectivity in photocatalytic CO2 reduction reactions by surface oxophilicity engineering
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通过表面亲氧工程增强光催化 CO2 还原反应中 CH4 选择性的总体策略
DOI：
10.1016/j.jcat.2022.10.004
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发表时间：
2022
影响因子：
7.3
通讯作者：
Zheng, Weiwei
中科院分区：
文献类型：
--
作者：
Li, Wenhao;Ma, De-Kun;Hu, Xia;Gou, Faliang;Yang, Xiaogang;MacSwain, Walker;Qi, ChenZe;Zheng, Weiwei
合理设计和控制反应中间体与光催化剂表面的相互作用是光催化中获得高产物选择性的关键。本文以基于cds的光催化co2还原反应（CO2RR）为模型体系，证明了通过在光催化剂表面引入高亲氧性的La3+离子可以显著提高ch4选择性。光催化剂的高表面亲氧性可以提高CO*的解吸能，促进进一步加氢生成CH4。相反，当在CdS中掺杂低亲氧性的Au3+离子时，在CO2RR中观察到ch4选择性降低。值得注意的是，将亲氧La3+离子掺杂到包括ZnO、SnS2、BiOBr、BiVO4、TaON和CsPbBr3在内的多种可选光催化剂中可以提高ch4选择性，这表明稀土La3+离子掺杂可以提高光催化剂的表面亲氧性，从而提高CO2RR的ch4选择性。
Rationally designing and controlling the interactions between reaction intermediates and the surface of photocatalysts is critical to obtain high product selectivity in photocatalysis. Herein, using CdS-based photocatalytic CO2reduction reaction (CO2RR) as a model system, we demonstrate that CH4selectivity can be significantly enhanced through the introduction of La3+ions with high oxophilicity on the surface of the photocatalysts. The high surface oxophilicity of the photocatalysts can increase CO* desorption energy and promote further hydrogenation to CH4. In contrast, when Au3+ions with low oxophilicity were doped in CdS, reduced CH4selectivity was observed in the CO2RR. Significantly, enhanced CH4selectivity can be achieved by doping oxophilic La3+ions into a broad range of alternative photocatalysts including ZnO, SnS2, BiOBr, BiVO4, TaON, and CsPbBr3, which demonstrates the general strategy to enhance CH4selectivity of photocatalytic CO2RR through increased surface oxophilicity of the photocatalysts by rare earth La3+ion doping.