Xue Ping, Pan Xin, Huang Jiming, Gao Yijun, Guo Wei, Li Junsheng, Tang Mi, Wang Zhengbang
Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and Ministry, School of Materials Science and Engineering, Hubei University, Wuhan, 430062, China.
Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory, Xianhu hydrogen Valley, Foshan 528200, China.
ACS Appl Mater Interfaces. 2021 Dec 22;13(50):59915-59924. doi: 10.1021/acsami.1c18238. Epub 2021 Dec 11.
Construction of porous metal-organic framework (MOF)/covalent organic framework (COF) hybrid photocatalysts for enriched structures and unprecedented properties is still a great challenge but highly desirable. Herein, a new series of Cu(HHTP)-MOF/Tp-Pa-1-COF hybrids with different MOF content are successfully fabricated. The as-prepared MOF/COF hybrids exhibit intimate interaction based on the coordination of Cu ions with the carbonyl oxygen and enamine nitrogen groups in Tp-Pa-1. The integrated conductive Cu(HHTP) is able to act as an excellent electron extractor instead of noble metal cocatalysts to significantly promote the charge transfer and inhibit the recombination of photogenerated electron-hole pairs. As a results, the optimized photocatalyst with Cu(HHTP):Tp-Pa-1 ratio of 1:15 achieves the highest hydrogen evolution rate of 1.76 mmol·h·g under visible-light irradiation, which is about 93 times higher than that of the pure Tp-Pa-1 and even slightly higher than that of the Tp-Pa-1 with Pt (3 wt %) as a cocatalyst.
构建具有丰富结构和前所未有的性能的多孔金属有机框架（MOF）/共价有机框架（COF）杂化光催化剂仍然是一个巨大的挑战，但却非常令人期待。在此，成功制备了一系列不同MOF含量的新型Cu（HHTP）-MOF/Tp-Pa-1-COF杂化物。所制备的MOF/COF杂化物基于Cu离子与Tp-Pa-1中的羰基氧和烯胺氮基团的配位表现出紧密的相互作用。集成的导电Cu（HHTP）能够作为优异 的电子提取剂，而不是贵金属助催化剂，从而显著促进电荷转移并抑制光生电子-空穴对的复合。结果，Cu（HHTP）:Tp-Pa-1比例为1:15的优化光催化剂在可见光照射下实现了最高的析氢速率1.76 mmol·h·g，这比纯Tp-Pa-1高约93倍，甚至略高于以Pt（3 wt%）作为助催化剂的Tp-Pa-1。
