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Boosting Cascade Electron Transfer for Highly Efficient CO2 Photoreduction
Solar RRL ( IF 7.9 ) Pub Date : 2021-09-16 , DOI: 10.1002/solr.202100558
Na Li 1 , Xin-Ping Zhai 1 , Wen-Kai Yan 2 , Ya-Jun Zhang 2 , Zheng-Tao Zhang 1 , Ming-Jun Xiao 1 , Xiao-Dong Zhang 3 , Qiang Wang 1 , Hao-Li Zhang 1
Affiliation  

Artificial photosynthesis converting carbon dioxide into chemical fuels with a high added value is a promising solution to both fossil fuel shortage/pollution and global climate change; however, the development of highly efficient photocatalysts toward this goal is still largely bereft of fresh ideas. Herein, we propose a “cascade electron transfer” strategy through spurring both interfacial and inner electron transfer rates for a 0D/2D photocatalyst of CsPbBr3/CuTCPP metal organic framework (MOF). Upon photoexcitation, the heterojunction structure with an appropriate band alignment facilitates an ultrafast interfacial electron transfer rate of 1.4 ps from CsPbBr3 segment to CuTCPP MOF and subsequent ultrafast internal electron transfer of 21 ps from CuTCPP ligand to the Cu node within the enlarged 2D framework. The efficient electron transfer ensures efficient charge separation favorable for photocatalytic reactions: The photocatalyst exhibits an outstanding yield of 47.2 μmol g−1 h−1 (CO and CH4 combined) superior to previous reports. Rational design of hierarchical heterojunctions with matching electronic bandgap not only expedites cascade charge transfer but also prevents holes from recombining with electrons or oxidizing the photocatalysts without the necessity of sacrificial reagents. This work thus provides useful insight for boosting photocatalytic efficacy from a dynamic perspective.

中文翻译:

促进级联电子转移以实现高效的 CO2 光还原

将二氧化碳转化为具有高附加值的化学燃料的人工光合作用是解决化石燃料短缺/污染和全球气候变化的有希望的解决方案;然而,为实现这一目标而开发高效光催化剂仍然在很大程度上缺乏新的想法。在此,我们提出了一种“级联电子转移”策略,通过刺激 CsPbBr 3 /CuTCPP 金属有机骨架 (MOF)的 0D/2D 光催化剂的界面和内部电子转移速率。在光激发时,具有适当能带排列的异质结结构促进了 CsPbBr 3的超快界面电子转移速率为 1.4 ps段到 CuTCPP MOF 以及随后从 CuTCPP 配体到扩大的 2D 框架内的 Cu 节点的 21 ps 超快内部电子转移。有效的电子转移确保了有利于光催化反应的有效电荷分离:该光催化剂的产率高达 47.2 μmol g -1  h -1(CO 和 CH 4结合),优于之前的报道。具有匹配电子带隙的分级异质结的合理设计不仅可以加速级联电荷转移,而且可以防止空穴与电子复合或氧化光催化剂,而无需牺牲试剂。因此,这项工作为从动态角度提高光催化功效提供了有用的见解。
更新日期:2021-11-04
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