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Giant Electron-Hole Interactions in Confined Layered Structures for Molecular Oxygen Activation
2017-06-02
J. Am. Chem. Soc. 139(13):4737-4742 Apr 2017

Wang, Hui; Chen, Shichuan; Yong, Dingyu; Zhang, Xiaodong; Li, Shuang; Shao, Wei; Sun, Xianshun; Pan, Bicai; Xie, Yi

Abstract:
Numerous efforts have been devoted to understanding the excitation processes of photocatalysts, whereas the potential Coulomb interactions between photogenerated electrons and holes have been long ignored. Once these interactions are considered, excitonic effects will arise that undoubtedly influence the sunlight-driven catalytic processes. Herein, by taking bismuth oxyhalide as examples, we proposed that giant electron–hole interactions would be expected in confined layered structures, and excitons would be the dominating photoexcited species. Photocatalytic molecular oxygen activation tests were performed as a proof of concept, where singlet oxygen generation via energy transfer process was brightened. Further experiments verify that structural confinement is curial to the giant excitonic effects, where the involved catalytic process could be readily regulated via facet-engineering, thus enabling diverse reactive oxygen species generation. This study not only provides an excitonic prospective on photocatalytic processes, but also paves a new approach for pursuing systems with giant electron–hole interactions.

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