Modulation of Polymeric Carbon Nitrides through Supramolecular Preorganization for Efficient Photocatalytic Hydrogen Generation

Supramolecular pre-assembly by design is an effective strategy to adapt the physicochemical properties of polymeric carbon nitrides (PCNs) to improve their solar conversion performance. A new supramolecular preorganization protocol, which employs H2O as the self-assembly medium and sodium persulfate as a modifier, is proposed to modulate the textural and photoelectronic features of PCNs for efficient visible-light H-2 evolution. Sodium persulfate is revealed to precisely tailor the final carbon nitride polymers with unusual porous layered structures and promoted charge separation and migration kinetics. As a result, the modulated PCNs with optimized structures show a greatly enriched activity for photocatalytic H-2 generation compared to the analogous materials derived from melamine without the modifier.