Defective ZnIn2S4 Nanosheets for Visible-Light and Sacrificial-Agent-Free H2O2 Photosynthesis via O2/H2O Redox

化学 光合作用 氧化还原 人工光合作用 光化学 量子效率 催化作用 光系统II 吸附 量子产额 纳米技术 化学工程 光催化 无机化学 有机化学 光电子学 材料科学 荧光 物理 工程类 量子力学 生物化学
作者
Huiping Peng,Hongcen Yang,Jiajia Han,Xiaozhi Liu,Dong Su,Yang Tang,Shangheng Liu,Chih‐Wen Pao,Zhiwei Hu,Qiaobao Zhang,Yong Xu,Hongbo Geng,Xiaoqing Huang
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:145 (50): 27757-27766 被引量:104
标识
DOI:10.1021/jacs.3c10390
摘要

H2O2 photosynthesis has attracted great interest in harvesting and converting solar energy to chemical energy. Nevertheless, the high-efficiency process of H2O2 photosynthesis is driven by the low H2O2 productivity due to the recombination of photogenerated electron-hole pairs, especially in the absence of a sacrificial agent. In this work, we demonstrate that ultrathin ZnIn2S4 nanosheets with S vacancies (Sv-ZIS) can serve as highly efficient catalysts for H2O2 photosynthesis via O2/H2O redox. Mechanism studies confirm that Sv in ZIS can extend the lifetimes of photogenerated carriers and suppress their recombination, which triggers the O2 reduction and H2O oxidation to H2O2 through radical initiation. Theoretical calculations suggest that the formation of Sv can strongly change the coordination structure of ZIS, modulating the adsorption abilities to intermediates and avoiding the overoxidation of H2O to O2 during O2/H2O redox, synergistically promoting 2e- O2 reduction and 2e- H2O oxidation for ultrahigh H2O2 productivity. The optimal catalyst displays a H2O2 productivity of 1706.4 μmol g-1 h-1 under visible-light irradiation without a sacrificial agent, which is ∼29 times higher than that of pristine ZIS (59.4 μmol g-1 h-1) and even much higher than those of reported photocatalysts. Impressively, the apparent quantum efficiency is up to 9.9% at 420 nm, and the solar-to-chemical conversion efficiency reaches ∼0.81%, significantly higher than the value for natural synthetic plants (∼0.10%). This work provides a facile strategy to separate the photogenerated electron-hole pairs of ZIS for H2O2 photosynthesis, which may promote fundamental research on solar energy harvest and conversion.
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