HOF-Ni-GDY dual-ohmic-junction engineering: inducing photogenerated electron–hole dual channel separation for boosted hydrogen evolution

Abstract

Photocatalytic hydrogen evolution, as a sustainable approach to green hydrogen production, faces significant challenges related to efficiency, stability, and cost-effectiveness. In this study, a novel non-noble metal composite photocatalyst based on HOF and GDY was rationally designed. The integration of Ni nanoparticles and HOF nanorods onto layered GDY enabled multiple synergistic enhancements in catalytic performance. The presence of abundant acetylene bonds and uniformly distributed pores in GDY can significantly enhance the adsorption of reaction substrates; Ni, serving as a metal active center, efficiently captures photogenerated electrons and facilitates their participation in the hydrogen evolution reaction. Meanwhile, the flexible hydrogen-bonded network characteristic of HOF creates an “induced fit” microenvironment conducive to catalytic reactions. The DFT calculations, in conjunction with experimental results, demonstrate that the three components form the dual ohmic junctions upon compounding, thereby providing dual driving forces and an efficient charge transfer pathway for the photocatalytic hydrogen evolution reaction. Under illumination by 10 W LED, the hydrogen evolution yield of Ni8TG15 within 5 h was 28.6 times greater than that of TCP. This study presents a novel design strategy for developing high-performance, non-noble metal photocatalysts based on HOF in combination with carbon materials.