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

Title data

Lau, Vincent Wing-hei ; Moudrakovski, Igor ; Botari, Tiago ; Weinberger, Simon ; Mesch, Maria B. ; Duppel, Viola ; Senker, Jürgen ; Blum, Volker ; Lotsch, Bettina V.:
Rational design of carbon nitride photocatalysts by identification of cyanamide defects as catalytically relevant sites.
In: Nature Communications. Vol. 7 (8 July 2016) .
ISSN 2041-1723
DOI: https://doi.org/10.1038/ncomms12165

Official URL: Volltext

Abstract in another language

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.

Further data

Item Type: Article in a journal
Refereed: Yes
Additional notes: Artikel-Nr. 12165
Institutions of the University: Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Anorganic Chemistry III > Chair Anorganic Chemistry III - Univ.-Prof. Dr. Jürgen Senker
Faculties
Faculties > Faculty of Biology, Chemistry and Earth Sciences
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Anorganic Chemistry III
Result of work at the UBT: No
DDC Subjects: 500 Science > 540 Chemistry
Date Deposited: 12 Sep 2016 07:24
Last Modified: 21 Nov 2017 10:37
URI: https://eref.uni-bayreuth.de/id/eprint/34693