Transition-metal phosphides have been demonstrated as cocatalysts with great promise for photocatalytic H 2 production materials, but the insurmountable issue remains maintaining outstanding stability while achieving high photocatalytic efficiency. Herein, the rhodium phosphide (RhP x ) nanospecies as cocatalyst is firmly mounted on graphitic carbon nitride (g-C 3 N 4 ) nanosheets to realize the improved activity and stability for photocatalytic H 2 production. The maximum H 2 production rate over RhP x / g-C 3 N 4 driven by visible light diplays a 5.6-fold improvement compared with Pt/g-C 3 N 4 . Meanwhile, the apparent quantum efficiency of 18.4% is achieved at a fixed wavelength of 420 nm that far exceeds the reported g-C 3 N 4 modified with other single-transition-metal phosphides. Particularly, RhP x /g-C 3 N 4 can maintain consistently stable H 2 production when enduring over 25 cyclic reactions with a total of 100 h. The deep insight into the modification effect of RhP x nanospecies reveals that it dramatically facilitates migration and separation of photoinduced electron−hole pairs and heightens interaction at the heterointerfaces between RhP x nanospecies and g-C 3 N 4 nanosheets. This contribution extends the broad potential application of transition-metal phosphides as cocatalysts in the photocatalytic conversion from solar to hydrogen energy.

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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.