Carbon nitride embedded in carbon layer with interconnected porous nanosheets structure for solar-driven photocatalytic reaction

The implementation of multiple strategies that involve constructing a beneficial morphological structure and coupling with the thermal field can significantly promote photogenerated charge separation in carbon nitride (CN) and enhance solar irradiation utilization, which are effective approaches to improve its solar-driven photocatalytic reaction efficiency. CN embedded in carbon layer with an interconnected nanosheet architecture was obtained by coaxial electrostatic spraying. In which, carbon layer not only exhibit photothermal effects: elevating the surface/interface temperature of material and accelerating the thermodynamic rate of reactions, but also offer expedited pathways for the photogenerated charges. In addition, the interconnected nanosheets, with a thickness of ∼30 nm and abundant mesoporous-dominated porosity, also facilitate rapid mass transfer processes. The hydrogen evolution reaction (HER) rate of the composite photocatalyst used for solar-driven water splitting reached 6.48 mmol h⁻¹ g⁻¹ and it demonstrated good cyclic stability and remarkable dye degradation efficiency. Photoelectrochemical test results indicated that, catalysts featuring an embedded structure of interconnected nanosheets can effectively reduce ohmic resistance and suppress the recombination of photogenerated charges. Ultimately, the intrinsic mechanisms underpinning this enhancement were elucidated through theoretical calculations. This work introduces novel strategies and perspectives for multi-field synergy in the pursuit of efficient solar-driven water splitting for HER.