Xu Shengqi, Yang Lu, Wei Yixuan, Jia Yiming, Hu Meiqi, Bai Lianxia, Zhang Junzheng, Li Xinxin, Wei Shuo, Lu Jun
College of Chemistry, Beijing Normal University, Beijing 100875, P. R. China.
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China.
Dalton Trans. 2022 May 24;51(20):8036-8045. doi: 10.1039/d2dt00972b.
Converting CO into valuable solar fuels through photocatalysis has been considered a green and sustainable technology that is promising for alleviating global warming and providing energy in an environmentally friendly manner. However, traditional photocatalysts generally suffer from low surface-reactive reaction sites, inefficient light harvesting and rapid recombination of electron-hole pairs. Lead halide perovskite materials have been considered ideal semiconductor photocatalysts for photocatalytic CO reduction due to their tunable band gaps, strong light absorption, and low cost. Herein, a series of LCsPbX (L = ba, ha, oa; X = Cl, Br, I; = 1, 2) 2D layered perovskites were synthesized by a facile solvothermal method. The effects of alkyl amine chain length, halogen atoms and inorganic layer number on their properties were studied. More importantly, these 2D materials were used as photocatalysts for CO reduction without any sacrificial agents. These 2D perovskites exhibited markedly increased performance in comparison with 3D bulk materials, benefitting from the larger surface-area-to-volume ratio and faster and more efficient exciton dissociation, which achieved the highest CO yield of 158.69 μmol g h and CH yield of 6.9 μmol g h through the design of the photocatalytic system. In addition, the influence of light source conditions on photocatalysis was studied systematically, including light source intensity and wavelength. The experimental results indicated that an appropriate solvent, high light intensity and monochromatic light source matching the wavelength of exciton absorption can effectively improve the photocatalytic efficiency.
通过光催化将一氧化碳转化为有价值的太阳能燃料被认为是一种绿色可持续技术，有望缓解全球变暖并以环境友好的方式提供能源。然而，传统光催化剂通常存在表面反应位点少、光捕获效率低以及电子 - 空穴对快速复合等问题。卤化铅钙钛矿材料因其可调带隙、强光吸收和低成本，被认为是用于光催化一氧化碳还原的理想半导体光催化剂。在此，通过简便的溶剂热法合成了一系列LCsPbX（L = ba、ha、oa；X = Cl、Br、I； = 1、2）二维层状钙钛矿。研究了烷基胺链长、卤素原子和无机层数对其性能的影响。更重要的是，这些二维材料被用作一氧化碳还原的光催化剂，无需任何牺牲剂。与三维块状材料相比，这些二维钙钛矿表现出显著提高的性能，这得益于更大的表面积与体积比以及更快更有效的激子解离，通过光催化系统的设计实现了最高一氧化碳产率为158.69 μmol g h和甲烷产率为6.9 μmol g h。此外，系统研究了光源条件对光催化的影响，包括光源强度和波长。实验结果表明，合适的溶剂、高光强度和与激子吸收波长匹配的单色光源可以有效提高光催化效率。
