Issue 21, 2013
From the journal:

Journal of Materials Chemistry A

Solar hydrogen evolution using metal-free photocatalytic polymeric carbon nitride/CuInS2 composites as photocathodes

Florent Yang,*a   Vadym Kuznietsov,a   Michael Lublow,b   Christoph Merschjann,ac   Alexander Steigert,a   Joachim Klaer,d   Arne Thomase  and  Thomas Schedel-Niedriga  

* Corresponding authors

a Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Institut für Heterogene Materialsysteme, Hahn-Meitner-Platz 1, 14109 Berlin, Germany
E-mail: florent.yang@helmholtz-berlin.de
Fax: +49 30 8062 43199
Tel: +49 30 8062 42175

b Leibnitz-Institut für Katalyse – LIKAT, Albert-Einstein-Straße 29a, 18059 Rostock, Germany

c Universität Rostock, Institut für Physik, Universitätsplatz 3, 18055 Rostock, Germany

d Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Institut für Technologie, Hahn-Meitner-Platz 1, 14109 Berlin, Germany

e Technische Universität Berlin, Institut für Chemie, Straße des 17. Juni 135, 10623 Berlin, Germany

Abstract

Polymeric carbon nitride (g-C3N4) films were synthesized on polycrystalline semiconductor CuInS2 chalcopyrite thin film electrodes by thermal polycondensation and were investigated as photocathodes for the hydrogen evolution reaction (HER) under photoelectrochemical conditions. The composite photocathode materials were compared to g-C3N4 powders and were characterized with grazing incidence X-ray diffraction and X-ray photoemission spectroscopy as well as Fourier transform infrared and Raman spectroscopies. Surface modification of polycrystalline CuInS2 semiconducting thin films with photocatalytically active g-C3N4 films revealed structural and chemical properties corresponding to the properties of g-C3N4 powders. The g-C3N4/CuInS2 composite photocathode material generates a cathodic photocurrent at potentials up to +0.36 V vs. RHE in 0.1 M H2SO4 aqueous solution (pH 1), which corresponds to a +0.15 V higher onset potential of cathodic photocurrent than the unmodified CuInS2 semiconducting thin film photocathodes. The cathodic photocurrent for the modified composite photocathode materials was reduced by almost 60% at the hydrogen redox potential. However, the photocurrent generated from the g-C3N4/CuInS2 composite electrode was stable for 22 h. Therefore, the presence of the polymeric g-C3N4 films composed of a network of nanoporous crystallites strongly protects the CuInS2 semiconducting substrate from degradation and photocorrosion under acidic conditions. Conversion of visible light to hydrogen by photoelectrochemical water splitting can thus be successfully achieved by g-C3N4 films synthesized on polycrystalline CuInS2 chalcopyrite electrodes.

Graphical abstract: Solar hydrogen evolution using metal-free photocatalytic polymeric carbon nitride/CuInS2 composites as photocathodes

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Article information

DOI
https://doi.org/10.1039/C3TA10360A
Article type
Paper
Submitted
23 Jan 2013
Accepted
27 Mar 2013
First published
27 Mar 2013

J. Mater. Chem. A, 2013,1, 6407-6415

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Solar hydrogen evolution using metal-free photocatalytic polymeric carbon nitride/CuInS2 composites as photocathodes

F. Yang, V. Kuznietsov, M. Lublow, C. Merschjann, A. Steigert, J. Klaer, A. Thomas and T. Schedel-Niedrig, J. Mater. Chem. A, 2013, 1, 6407 DOI: 10.1039/C3TA10360A

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