Abstract
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 N-15-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 H-2 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 H-2 evolution, and provides a promising route for the rational design of a variety of highly active crystalline CN photocatalysts.