2D/2D Hydrogen-Bonded Organic Frameworks/Covalent Organic Frameworks S-Scheme Heterojunctions for Photocatalytic Hydrogen Evolution

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Ruiqi Gao, Rongchen Shen, Can Huang, Kaihui Huang, Prof. Guijie Liang, Prof. Peng Zhang, Prof. Xin Li
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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.

Abstract Image

用于光催化氢转化的二维/二维氢键有机框架/共价有机框架 S 型异质结
氢键有机框架(HOFs)在光催化领域的应用潜力巨大。然而,电子-空穴分离的低效率和有限的稳定性阻碍了它们在光催化水分离制氢中的实际应用。本文采用快速自组装溶液分散法,成功建立了HOF-H4TBAPy(Py-HOF,H4TBAPy代表1,3,6,8-四(对苯甲酸)芘)和Py-COF之间的新型双芘基超分子HOF/COF 2D/2D S型异质结。实验和理论研究证实,两种晶体多孔材料的尺寸匹配使得集成异质结构材料具有丰富的表面反应位点、较强的相互作用和增强的 S 型内置电场,从而显著提高了光生电荷载流子的分离效率和稳定性。值得注意的是,最佳 HOF/COF 异质结的光催化氢进化率达到 390.68 mmol g-1 h-1,是纯 Py-HOF 的 2.28 倍,纯 COF 的 9.24 倍。这些发现恰恰为基于双苯乙烯的 S 型异质结的巧妙设计提供了宝贵的原子尺度启示。这项工作提出了在基于 HOF 的半导体上形成超分子 S 型异质结的创新观点,为设计内置电场的强大强耦合 S 型异质结以高效利用太阳能提供了方案。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
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.
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