Platinum (Pt) cocatalyst greatly enhances the photoactivity of the graphitic carbon nitride (g-C3N4) photocatalyst for photocatalytic H2 evolution where the Pt properties are critical to determine the photocatalytic activity. In this study, highly dispersed Pt was successfully loaded onto chemically oxidized g–C3N4 (OCN) via a hydrogen reduction process over different reduction time. OCN photocatalysts containing highly dispersed Pt2+/Pt0 exhibited outstanding charge separation efficiency and photocatalytic performance. Symmetrical –CO groups on the OCN surface specifically interacted with atomic Pt2+, and the Pt2+ atoms were stably reduced to Pt0 atoms along with the generation of –OH groups over time. The coexistence of Pt0 and Pt2+ promoted superior photocatalytic performance because the photoinduced charge transfer was facilitated by the Pt0 atoms, which was evidenced by the DFT calculation and the EIS, PL, and photocurrent response results. Consequently, after the 24 h reduction, the highly stable and active Pt2+/Pt0 atoms were effectively distributed over OCN, resulting in the highest HER activity at 4091.3 µmol g−1 h−1.
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