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

Publication ,  Journal Article
Lau, VWH; Moudrakovski, I; Botari, T; Weinberger, S; Mesch, MB; Duppel, V; Senker, J; Blum, V; Lotsch, BV
Published in: Nature Communications
July 8, 2016

The heptazine-based polymer melon (also known as graphitic carbon nitride, g-C 3 N 4) 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.

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Published In

Nature Communications

DOI

EISSN

2041-1723

Publication Date

July 8, 2016

Volume

7
 

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Lau, V. W. H., Moudrakovski, I., Botari, T., Weinberger, S., Mesch, M. B., Duppel, V., … Lotsch, B. V. (2016). Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites. Nature Communications, 7. https://doi.org/10.1038/ncomms12165
Lau, V. W. H., I. Moudrakovski, T. Botari, S. Weinberger, M. B. Mesch, V. Duppel, J. Senker, V. Blum, and B. V. Lotsch. “Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites.” Nature Communications 7 (July 8, 2016). https://doi.org/10.1038/ncomms12165.
Lau VWH, Moudrakovski I, Botari T, Weinberger S, Mesch MB, Duppel V, et al. Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites. Nature Communications. 2016 Jul 8;7.
Lau, V. W. H., et al. “Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites.” Nature Communications, vol. 7, July 2016. Scopus, doi:10.1038/ncomms12165.
Lau VWH, Moudrakovski I, Botari T, Weinberger S, Mesch MB, Duppel V, Senker J, Blum V, Lotsch BV. Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites. Nature Communications. 2016 Jul 8;7.

Published In

Nature Communications

DOI

EISSN

2041-1723

Publication Date

July 8, 2016

Volume

7