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Solar H2 generation in water with a CuCrO2 photocathode modified with an organic dye and molecular Ni catalyst.

Published version
Peer-reviewed

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Authors

Creissen, Charles E 
Warnan, Julien 

Abstract

Dye-sensitised photoelectrochemical (DSPEC) cells have emerged in recent years as a route to solar fuel production. However, fuel-forming photocathodes are presently limited by photo-corrodible narrow band gap semiconductors or the small range of available wide bandgap p-type semiconductors such as NiO that display low performance with dyes. Here, we introduce CuCrO2 as a suitable p-type semiconductor for visible light-driven H2 generation upon co-immobilisation of a phosphonated diketopyrrolopyrrole dye with a Ni-bis(diphosphine) catalyst. The hybrid CuCrO2 photocathode displays an early photocurrent onset potential of +0.75 V vs. RHE and delivers a photocurrent of 15 μA cm-2 at 0.0 V vs. RHE in pH 3 aqueous electrolyte solution under UV-filtered simulated solar irradiation. Controlled potential photoelectrolysis at 0.0 V vs. RHE shows good stability and yields a Ni catalyst-based turnover number of 126 ± 13 towards H2 after 2 h. This precious metal-free system outperforms an analogous NiO|dye/catalyst assembly and therefore highlights the benefits of using CuCrO2 as a novel material for DSPEC applications.

Description

Keywords

0912 Materials Engineering

Journal Title

Chem Sci

Conference Name

Journal ISSN

2041-6520
2041-6539

Volume Title

9

Publisher

Royal Society of Chemistry (RSC)
Sponsorship
Christian Doppler Forschungsgesellschaft (unknown)
Engineering and Physical Sciences Research Council (EP/J017361/1)
EPSRC (1494597)
Engineering and Physical Sciences Research Council (EP/L015978/1)