由HOFs/MOFs S型异质结中π-π堆叠电荷转移通道促进的强内置电场用于提升光催化产氢或过氧化氢

doi:10.1016/j.actphy.2026.100329

物理化学学报 >> 2026, Vol. 42 >> Issue (11): 100329.doi: 10.1016/j.actphy.2026.100329

由HOFs/MOFs S型异质结中π-π堆叠电荷转移通道促进的强内置电场用于提升光催化产氢或过氧化氢

蔡清红¹, 刘兴燕¹, 李宇涵¹, 贺有周¹, 徐先燕², 曾嘉¹, 韦思平³

1 重庆工商大学环境与资源学院、智能环境前沿交叉研究院、大数据学院, 环境催化重庆市重点实验室, 重庆 400067;
2 韶关学院化学与土木工程学院, 广东韶关 512005;
3 西南医科大学药学院, 绿色制药技术泸州市重点实验室, 四川泸州 646000

收稿日期:2026-03-26 修回日期:2026-05-08 录用日期:2026-05-21 发布日期:2026-09-29
通讯作者: 刘兴燕, 李宇涵, 韦思平 E-mail:liuxingyan@ctbu.edu.cn;liyh@ctbu.edu.cn;swei1225@swmu.edu.cn
基金资助:
国家自然科学基金(22001026, 52370109和22171233)；重庆市自然科学基金(CSTB2025YITP-QCRCX0064, CSTB2025NSCQ-GPX0827, CSTB2024NSCQ-LZX0073, CSTB2025NSCQ-GPX0816)；重庆市教委科学技术研究计划(KJZD-M202400802和KJZD-K202300806)资助。

Strong built-in electric field promoted by π-π stacking charge-transfer channels in HOFs/MOFs S-scheme heterojunction for boosting photocatalytic H₂ or H₂O₂ production

Qinghong Cai¹, Xingyan Liu¹, Yuhan Li¹, Youzhou He¹, Xianyan Xu², Jia Zeng¹, Siping Wei³

1 Chongqing Key Laboratory of Environmental Catalysis, College of Environment and Resources, Institute for Frontier Interdisciplinary Research in Intelligence and Environment, School of Big Data, Chongqing Technology and Business University, Chongqing 400067, China;
2 School of Chemistry and Civil Engineering, Shaoguan University, Shaoguan 512005, Guangdong Province, China;
3 Green Pharmaceutical Technology Key Laboratory of Luzhou City, School of Pharmacy, Southwest Medical University, Luzhou 646000, Sichuan Province, China

Received:2026-03-26 Revised:2026-05-08 Accepted:2026-05-21 Published:2026-09-29
Contact: Xingyan Liu, Yuhan Li, Siping Wei E-mail:liuxingyan@ctbu.edu.cn;liyh@ctbu.edu.cn;swei1225@swmu.edu.cn

1. ACTPHY-2026.100329-SI-10p-周排.pdf(2168KB)

摘要/Abstract

摘要： 尽管氢键有机框架(HOFs)与金属有机框架(MOFs)在光催化领域各具优势，但HOFs/MOFs异质结的构建仍鲜有研究。特别是此类异质结中深层次的电荷转移动力学机制尚不明确。本研究通过π-π相互作用原位耦合HOFs(SA-TCPP)与MOFs(ZnTCPP)，构建了具有强内置电场(IEF)的卟啉基HOFs/MOFs(SA-TCPP/ZnTCPP)S型异质结，其最优IEF强度较单一SA-TCPP和ZnTCPP分别提升11.5倍和4.9倍。在该S型异质结体系中，接触界面作为电荷调控中心，通过π-π堆叠的HOMO-LUMO电荷转移通道增强IEF泵浦强度，精准调控光生载流子的空间分离方向，并经由“光激发-迁移通道-泵浦加速”策略触发级联反应。相较于单一组分，SA-TCPP/ZnTCPP的H₂ (2307 μmol g^-1 h^-1)和H₂O₂ (295.2 μmol g^-1 h^-1)光催化产率分别提升7.02倍/5.6倍与3.09倍/2.85倍。飞秒瞬态吸收光谱(fs-TAS)、开尔文探针力显微镜(KPFM)、原位X射线光电子能谱(in situ XPS)及密度泛函理论(DFT)证实，该显著提升源于载流子的高效分离效率。本工作实现了框架材料的跨功能集成，为开发高性能多功能人工光合系统提供了新策略。

关键词: HOFs/MOFs, 内置电场, S型异质结, π-π堆叠电荷传输通道, 光催化

Abstract: Despite hydrogen-bonded organic frameworks (HOFs) and metal-organic framework (MOFs) exhibit distinct advantages in photocatalysis, the fabrication of HOFs/MOFs heterojunction remains scarcely explored. In particular, the deep-seated charge transfer dynamics in such heterojunctions remain unclear. Herein, in situ coupling HOFs (SA-TCPP) and MOFs (ZnTCPP) through π-π interaction to fabricate the porphyrin-based HOFs/MOFs (SA-TCPP/ZnTCPP) S-scheme heterojunction with strong built-in electric field (IEF), in which the optimal IEF intensity for SA-TCPP/ZnTCPP was increased by 11.5 and 4.9 times compared to individual SA-TCPP and ZnTCPP, respectively. Within the SA-TCPP/ZnTCPP S-scheme heterojunction system, the contact interface serves as the charge carriers regulation centers to promote IEF pumps strength via π-π stacking HOMO-LOMO charge-transfer channels, which adjusts the precise direction of spatial separation for photogenerated charge carriers and triggers a sophisticated cascade reactions via “photoexcitation-migration channel-pump acceleration” strategy. Compared with the individual SA-TCPP and ZnTCPP, the photocatalytic rate of H₂ (2307 μmol g^-1 h^-1) and H₂O₂ (295.2 μmol g^-1 h^-1) for SA-TCPP/ZnTCPP increased 7.02 times, 5.6 times and 3.09 times, 2.85 times, respectively. The significant improvement can be ascribed to the efficient separation efficiency of charge carriers, which has been elucidated by femtosecond transient absorption spectroscopy (fs-TAS), kelvin probe force microscopy (KPFM), in situ X-ray photoelectron spectroscopy (in situ XPS) and density functional theory (DFT). This work achieves the cross-functional integration of frameworks, providing a novel design strategy for developing excellent and multifunctional artificial photosynthesis systems.

Key words: HOFs/MOFs, Built-in electric field, S-scheme heterojunctions, π-π stacking charge-transfer channels, Photocatalysis

蔡清红, 刘兴燕, 李宇涵, 贺有周, 徐先燕, 曾嘉, 韦思平. 由HOFs/MOFs S型异质结中π-π堆叠电荷转移通道促进的强内置电场用于提升光催化产氢或过氧化氢[J]. 物理化学学报, 2026, 42(11), 100329. doi: 10.1016/j.actphy.2026.100329

Qinghong Cai, Xingyan Liu, Yuhan Li, Youzhou He, Xianyan Xu, Jia Zeng, Siping Wei. Strong built-in electric field promoted by π-π stacking charge-transfer channels in HOFs/MOFs S-scheme heterojunction for boosting photocatalytic H₂ or H₂O₂ production[J]. Acta Phys. -Chim. Sin. 2026, 42(11), 100329. doi: 10.1016/j.actphy.2026.100329

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2026.100329

https://www.whxb.pku.edu.cn/CN/Y2026/V42/I11/100329

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由HOFs/MOFs S型异质结中π-π堆叠电荷转移通道促进的强内置电场用于提升光催化产氢或过氧化氢

Strong built-in electric field promoted by π-π stacking charge-transfer channels in HOFs/MOFs S-scheme heterojunction for boosting photocatalytic H₂ or H₂O₂ production

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由HOFs/MOFs S型异质结中π-π堆叠电荷转移通道促进的强内置电场用于提升光催化产氢或过氧化氢

Strong built-in electric field promoted by π-π stacking charge-transfer channels in HOFs/MOFs S-scheme heterojunction for boosting photocatalytic H2 or H2O2 production

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Strong built-in electric field promoted by π-π stacking charge-transfer channels in HOFs/MOFs S-scheme heterojunction for boosting photocatalytic H₂ or H₂O₂ production