In Situ Fabrication of Porous MOF/COF Hybrid Photocatalysts for Visible-Light-Driven Hydrogen Evolution

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 Cu3(HHTP)2-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 Cu3(HHTP)2 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 Cu3(HHTP)2:Tp-Pa-1 ratio of 1:15 achieves the highest hydrogen evolution rate of 1.76 mmol·h–1·g–1 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.