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通过缺陷和可调羟基自由基的联合策略促进光催化 CO 还原为 CH。

Promoting photocatalytic CO reduction to CH via a combined strategy of defects and tunable hydroxyl radicals.

机构信息

College of Science, Hebei University of Science and Technology, Shijiazhuang 050018, China.

College of Science, Hebei University of Science and Technology, Shijiazhuang 050018, China; State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China.

出版信息

J Colloid Interface Sci. 2022 Jan 15;606(Pt 2):1477-1487. doi: 10.1016/j.jcis.2021.08.163. Epub 2021 Aug 27.

DOI:10.1016/j.jcis.2021.08.163
PMID:34500152
Abstract

A well-designed photocatalyst with excellent activity and selectivity is crucial for photocatalytic CO conversion and utilization. TiO is one of the most promising photocatalysts. However, its excessive surface oxidation potential and insufficient surface active sites inhibit its activity and photocatalytic CO reduction selectivity. In this work, highly dispersed BiTiO was introduced into defective TiO to adjust its oxidation potential and the generation of radicals, further inhibiting reverse reactions during the photocatalytic conversion of CO. Moreover, an in situ topochemical reaction etching route was designed, which achieved defective surfaces, a contacted heterophase interface, and an efficient electron transfer path. The optimized heterophase photocatalyst exhibited 93.9% CH selectivity at a photocatalytic rate of 6.8 μmol·g·h, which was 7.9 times higher than that of P25. This work proposes a feasible approach to fabricating photocatalysts with well-designed band structures, highly dispersed heterophase interfaces, and sufficient surface active sites to effectively modulate the selectivity and activity of CO photoreduction by manipulating the reaction pathways.

摘要

具有优异活性和选择性的理想光催化剂对于光催化 CO 转化和利用至关重要。TiO 是最有前途的光催化剂之一。然而,其表面氧化势过高和表面活性位点不足限制了其活性和光催化 CO 还原选择性。在这项工作中,将高度分散的 BiTiO 引入到缺陷 TiO 中,以调整其氧化势和自由基的生成,从而进一步抑制 CO 光催化转化过程中的逆反应。此外,还设计了一种原位拓扑化学反应刻蚀路线,实现了缺陷表面、接触异质相界面和有效的电子转移途径。优化后的异质相光催化剂在光催化速率为 6.8 μmol·g·h 时表现出 93.9%的 CH 选择性,比 P25 高 7.9 倍。这项工作提出了一种可行的方法来制备具有精心设计的能带结构、高度分散的异质相界面和充足表面活性位点的光催化剂,通过操纵反应途径,有效地调节 CO 光还原的选择性和活性。

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