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Photoelectrocatalytic H2 Evolution in Water with Molecular Catalysts Immobilised on p-Si via a Stabilising Mesoporous TiO2 Interlayer

Abstract

The development of photoelectrodes capable of light-driven hydrogen evolution from water is an important approach for the storage of solar energy in the form of a chemical energy carrier. Nevertheless, molecular catalyst-based photocathodes remain scarcely reported and typically suffer from low efficiencies and/or stabilities due to inadequate strategies for interfacing the molecular component with the light-harvesting material. In this study, we report the straightforward preparation of a p-silicon|mesoporous titania|molecular catalyst photocathode assembly that is active towards proton reduction in aqueous media with an onset potential of +0.4 V vs. RHE. The mesoporous TiO2 scaffold acts as an electron shuttle between the silicon and the catalyst, while also stabilising the silicon from passivation and enabling a high loading of the molecular catalysts of more than 30 nmol (geometrical cm)−2. When a Ni bis(diphosphine)-based catalyst is anchored on the surface of the electrode, a high turnover number of 646 was obtained from photoelectrolysis under UV-filtered simulated solar irradiation at 1 Sun after 24 h at pH 4.5. Notwithstanding its aptitude for molecular catalyst immobilisation, the p-Si|TiO2 photoelectrode showed great versatility towards different catalysts and pH conditions, with photoelectrocatalytic H2 generation also being achieved with platinum or a hydrogenase enzyme as catalyst, highlighting the flexible platform it represents for many potential reductive catalysis transformations.

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Publication details

The article was received on 21 Mar 2017, accepted on 30 Apr 2017 and first published on 04 May 2017


Article type: Edge Article
DOI: 10.1039/C7SC01277B
Citation: Chem. Sci., 2017, Accepted Manuscript
  • Open access: Creative Commons BY license
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    Photoelectrocatalytic H2 Evolution in Water with Molecular Catalysts Immobilised on p-Si via a Stabilising Mesoporous TiO2 Interlayer

    J. J. Leung, J. Warnan, D. H. Nam, J. Z. Zhang, J. Willkomm and E. Reisner, Chem. Sci., 2017, Accepted Manuscript , DOI: 10.1039/C7SC01277B

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