Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites
By V. W. Lau, I. Moudrakovski, T. Botari, Simon Weinberger, Maria B. Mesch, V. Duppel, J. Senker, Volker Blum, Bettina V. Lotsch. Nature Communications, 2016
684 citations recorded by the source corpus.
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 improves coordination (and, in turn, charge transfer kinetics) to the platinum co-catalyst and enhances the separation of the photogenerated charge carriers. The demonstrated knowledge transfer for rational catalyst design presented here provides the conceptual framework for engineering high-performance heptazine-based photocatalysts. Graphitic carbon nitride is a promising hydrogen evolution photocatalyst, although there is limited understanding of its mechanistic operation. Here, the authors employ molecular heptazine-based model catalysts to identify catalytically relevant defects and to rationally design a highly active carbon nitride photocatalyst.
Subfields: Materials Chemistry, Renewable Energy, Sustainability and the Environment
View Paper: https://www.semanticscholar.org/paper/c5c9aa108c0169b4e638e6dc1e38a9d80e7f2b64
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In Materials Chemistry
In Renewable Energy, Sustainability and the Environment
Citations in the corpus
- Electronic defects in metal oxide photocatalysts (2022, background): “On the other hand, in melamine derived carbon nitride, long-lived trapped electrons were found to retain sufficient chemical potential to drive proton reduction even after 12 hours in the dark.(220,221)”