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Skeleton modification on carbon nitride (g-C3N4) via organic molecules is a recognized effective strategy to improve photocatalytic performance because it can powerfully improve charge separation in the skeleton plane. Herein, a diazole with a unique conjugated structure is bonded on edge of the g-C3N4 skeleton through a moderate polymerization of urea with 4-aminoantipyrine (4AAP). Meanwhile, the Pt nanoparticles selectively deposit on edge of the g-C3N4-4AAP15 nanosheet. It reveals that the robust limbic inducted and delocalized effects of diazole not only facilitate photogenerated electrons aggregation toward skeleton edge to promote in-plane carrier separation but also effectively stabilize and delocalize photogenerated electrons to improve carrier lifetime for propelling the photocatalytic hydrogen evolution (PHE) reaction. Specifically, the PHE rate over optimal g-C3N4-4AAP15 (284.2 μmol h–1) is 10 times that of pure g-C3N4 (27.6 μmol h–1) and the apparent quantum efficiency (AQE) at 420 nm reaches up to 24.2%. Through insights into the functionalized effect of small nitrogenous heterocycles introduced into the skeleton edge of g-C3N4, this work opens a new design thought for exploiting high-efficiency g-C3N4-based photocatalysts for photocatalytic application.

Developing the modified carbon nitride (CN) with multi-bonding mode remains a pivotal challenge for the high-efficiency photocatalytic hydrogen evolution (PHE). Here, we fabricate a PYM-CN photocatalyst by doping pyrimethamine (PYM)...