Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites.

ABSTRACT: 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 rational approaches because of a lack of fundamental understanding of its mechanistic operation. Here we employ molecular heptazine-based model catalysts to identify the cyanamide moiety as a photocatalytically relevant 'defect'. We exploit this knowledge for the rational design of a carbon nitride polymer populated with cyanamide groups, yielding a material with 12 and 16 times the hydrogen evolution rate and apparent quantum efficiency (400 nm), respectively, compared with the unmodified melon. Computational modelling and material characterization suggest that this moiety im

SUBMITTER: Lau VW 

PROVIDER: S-EPMC4941108 | biostudies-literature | 2016 Jul

REPOSITORIES: biostudies-literature