1D β-Ketoenamine Covalent Organic Frameworks/2D Transition Metal Sulfides Formed S-Scheme Heterojunctions Boosting Visible Light-Driven Hydrogen Production

In the design of photocatalytic materials, the catalyst should exhibit a clear nanostructure and good interface contact. Among these strategies, the ingenious combination of one-dimensional structures with two-dimensional materials to construct 1D/2D composite heterojunctions with special morphologies is widely regarded as a key approach for enhancing photocatalytic performance. In this study, MoS2 was assembled onto β-ketoenamine covalent organic frameworks (COFs) as a catalytic platform, and a 1D/2D MoS2/TpBd-COF composite material with an S-scheme heterojunction structure was constructed, enabling efficient hydrogen production without the use of noble metals. In addition, the hydrogen production rate of MT-35 can reach 2308.9 μmol g–1 h–1, with a quantum efficiency of 2.24% under 520 nm irradiation. Based on experimental results and theoretical computations, the effects of the composition, structure, specific surface area, charge differential density, Bader charge, electron transfer direction, and carrier separation efficiency on photocatalytic performance were systematically investigated. The successful formation of the S-scheme heterojunction was corroborated by both experimental verification and theoretical calculations, which also revealed the charge transfer mechanism of the catalyst. This study offers a powerful strategy and theoretical support for the design of efficient multidimensional nanocomposite heterojunction catalysts.