Facile Synthesis of Defect-Modified Thin-Layered and Porous g‑C₃N₄ with Synergetic Improvement for Photocatalytic H₂ Production

Modulating and optimizing the diverse parameters of photocatalysts synergistically as well as exerting these advantages fully in photocatalytic reactions are crucial for the sufficient utilization of solar energy but still face various challenges. Herein, a novel and facile urea- and KOH-assisted thermal polymerization (UKATP) strategy is first developed for the preparation of defect-modified thin-layered and porous g-C₃N₄ (DTLP-CN), wherein the thickness of g-C₃N₄ was dramatically decreased, and cyano groups, nitrogen vacancies, and mesopores were simultaneously introduced into g-C₃N₄. Importantly, the roles of thickness, pores, and defects can be targetedly modulated and optimized by changing the mass ratio of urea, KOH, and melamine. This can remarkably increase the specific area, improve the light-harvesting capability, and enhance separation efficiency of photoexcited charge carriers, strengthening the mass transfer in g-C₃N₄. Consequently, the photocatalytic hydrogen evolution efficiency of the DTLP-CN (1.557 mmol h^–1 g^–1, λ > 420 nm) was significantly improved more than 48.5 times with the highest average apparent quantum yield (AQY) of 18.5% and reached as high as 0.82% at 500 nm. This work provides an effective strategy for synergistically regulating the properties of g-C₃N₄, and opens a new horizon to design g-C₃N₄-based catalysts for highly efficient solar-energy conversion.