Ultrathin porous carbon nitride with molecular structure regulation for excellent photocatalytic water splitting

Developing universal strategy for designing novel photocatalysts with precise structure regulation is a promising approach to realizing efficient hydrogen production from water splitting, while great challenges remain since fundamental understanding of the internal mechanism is required. Herein, we demonstrate the universality of asymmetry supramolecular precursor-based route to synthesize ultrathin porous carbon nitride photocatalysts by incorporating various amino acids, which promises simultaneous production and spontaneous separation of H₂ and H₂O₂ from pure water splitting. Through detailed controlled experimental investigation together with theoretical analysis, the mechanism of improved photocatalytic performance is illustrated, which is attributed to the promoted adsorption/desorption process and charge-carrier dynamics upon the molecular structure regulation of carbon nitride photocatalysts with aldehyde functional groups.