Ruiqi Gao, Rongchen Shen, Can Huang, Kaihui Huang, Prof. Guijie Liang, Prof. Peng Zhang, Prof. Xin Li
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引用次数: 0
Abstract
Hydrogen-bonded organic frameworks (HOFs) demonstrate significant potential for application in photocatalysis. However, the low efficiency of electron-hole separation and limited stability inhibit their practical utilization in photocatalytic hydrogen evolution from water splitting. Herein, the novel dual-pyrene-base supramolecular HOF/COF 2D/2D S-scheme heterojunction between HOF-H4TBAPy (Py-HOF, H4TBAPy represents the 1,3,6,8-tetrakis (p-benzoic acid) pyrene) and Py-COF was successfully established using a rapid self-assembly solution dispersion method. Experimental and theoretical investigations confirm that the size-matching of two crystalline porous materials enables the integrated heterostructure material with abundant surface reaction sites, strong interaction, and an enhanced S-scheme built-in electric field, thus significantly improving the efficiency of photogenerated charge carrier separation and stability. Notably, the optimal HOF/COF heterojunction achieves a photocatalytic hydrogen evolution rate of 390.68 mmol g−1 h−1, which is 2.28 times higher than that of pure Py-HOF and 9.24 times higher than that of pure COF. These findings precisely acquire valuable atomic-scale insights into the ingenious design of dual-pyrene-based S-scheme heterojunction. This work presents an innovative perspective for forming supramolecular S-scheme heterojunctions over HOF-based semiconductors, offering a protocol for designing the powerful and strong-coupling S-scheme built-in electric fields for efficient solar energy utilization.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.