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The heptazine-based polymer melon (also known as graphitic carbon nitride,g-C3N4), is a promising photocatalyst for hydrogen evolution. Nonetheless,attempts to improve its inherently low activity are rarely based on rationalapproaches due to a lack of fundamental understanding of its mechanisticoperation. Here, we employ molecular heptazine-based model catalysts toidentify the cyanamide moiety as a photocatalytically relevant "defect". Weexploit this knowledge for the rational design of a carbon nitride polymerpopulated with cyanamide groups, yielding a material with 12- and 16-times thehydrogen evolution rate and apparent quantum efficiency (400 nm), respectively,compared to the benchmark melon. Computational modelling and materialcharacterization suggest this moiety improves co-ordination (and, in turn,charge transfer kinetics) to the platinum co-catalyst and enhances theseparation of the photo-generated charge carriers. The demonstrated knowledgetransfer for rational catalyst design presented here provides the conceptualframework for engineering high performance heptazine-based photocatalysts.

Towards rational design of carbon nitride photocatalysts: Identification of cyanamide "defects" as catalytically relevant sites