Harvesting Solar Light with Crystalline Carbon Nitrides for Efficient Photocatalytic Hydrogen Evolution

Described herein is the photocatalytic hydrogen evolution using crystalline carbon nitrides (CNs) obtained by supramolecular aggregation followed by ionic melt polycondensation (IMP) using melamine and 2,4,6‐triaminopyrimidine as a dopant. The solid state NMR spectrum of ¹⁵N‐enriched CN confirms the triazine as a building unit. Controlling the amount and arrangements of dopants in the CN structure can dramatically enhance the photocatalytic performance for H₂ evolution. The polytriazine imide (PTI) exhibits the apparent quantum efficiency (AQE) of 15 % at 400 nm. This method successfully enables a substantial amount of visible light to be harvested for H₂ evolution, and provides a promising route for the rational design of a variety of highly active crystalline CN photocatalysts.