Chen Taoran, Li Mengqing, Shen Lijuan, Roeffaers Maarten B J, Weng Bo, Zhu Haixia, Chen Zhihui, Yu Dan, Pan Xiaoyang, Yang Min-Quan, Qian Qingrong
College of Environmental Science and Engineering, Fujian Key Laboratory of Pollution Control & Resource Reuse, Fujian Normal University, Fuzhou, China.
CMACS, Department of Microbial and Molecular Systems, Leuven, Belgium.
Front Chem. 2022 Mar 15;10:833784. doi: 10.3389/fchem.2022.833784. eCollection 2022.
Metal halide perovskites (MHPs) have been widely investigated for various photocatalytic applications. However, the dual-functional reaction system integrated selective organic oxidation with H production over MHPs is rarely reported. Here, we demonstrate for the first time the selective oxidation of aromatic alcohols to aldehydes integrated with hydrogen (H) evolution over Pt-decorated CsPbBr. Especially, the functionalization of CsPbBr with graphene oxide (GO) further improves the photoactivity of the perovskite catalyst. The optimal amount of CsPbBr/GO-Pt exhibits an H evolution rate of 1,060 μmol g h along with high selectivity (>99%) for benzyl aldehyde generation (1,050 μmol g h) under visible light ( > 400 nm), which is about five times higher than the CsPbBr-Pt sample. The enhanced activity has been ascribed to two effects induced by the introduction of GO: 1) GO displays a structure-directing role, decreasing the particle size of CsPbBr and 2) GO and Pt act as electron reservoirs, extracting the photogenerated electrons and prohibiting the recombination of the electron-hole pairs. This study opens new avenues to utilize metal halide perovskites as dual-functional photocatalysts to perform selective organic transformations and solar fuel production.
金属卤化物钙钛矿（MHPs）已被广泛研究用于各种光催化应用。然而，将选择性有机氧化与MHPs上的产氢相结合的双功能反应体系鲜有报道。在此，我们首次展示了在Pt修饰的CsPbBr上，芳香醇选择性氧化为醛并伴有析氢反应。特别是，用氧化石墨烯（GO）对CsPbBr进行功能化进一步提高了钙钛矿催化剂的光活性。在可见光（>400nm）下，最佳量的CsPbBr/GO-Pt的析氢速率为1060μmol g⁻¹ h⁻¹，同时对苯甲醛生成具有高选择性（>99%）（1050μmol g⁻¹ h⁻¹），这比CsPbBr-Pt样品高出约五倍。活性增强归因于GO引入所引起的两种效应：1）GO起到结构导向作用，减小了CsPbBr的粒径；2）GO和Pt作为电子库，提取光生电子并抑制电子-空穴对的复合。这项研究为利用金属卤化物钙钛矿作为双功能光催化剂进行选择性有机转化和太阳能燃料生产开辟了新途径。
