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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

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

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引用本文: 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 shu
Citation:  Qinghong Cai,  Xingyan Liu,  Yuhan Li,  Youzhou He,  Xianyan Xu,  Jia Zeng,  Siping Wei. 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]. Acta Physico-Chimica Sinica, 2026, 42(11): 100329. doi: 10.1016/j.actphy.2026.100329 shu

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

  • 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

    • 通讯作者: 刘兴燕,E-mail:liuxingyan@ctbu.edu.cn; 李宇涵,E-mail:liyh@ctbu.edu.cn; 韦思平,E-mail:swei1225@swmu.edu.cn
  • 基金项目:

    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。

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。

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