Jump to main content
Jump to site search

Issue 7, 2017
Previous Article Next Article

Photoelectrocatalytic H2 evolution in water with molecular catalysts immobilised on p-Si via a stabilising mesoporous TiO2 interlayer

Author affiliations

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. However, 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 molecular catalysts (>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 ∼1 × 103 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 and a hydrogenase as catalyst, highlighting the flexible platform it represents for many potential reductive catalysis transformations.

Graphical abstract: Photoelectrocatalytic H2 evolution in water with molecular catalysts immobilised on p-Si via a stabilising mesoporous TiO2 interlayer

Back to tab navigation

Supplementary files

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., 2017,8, 5172-5180
  • Open access: Creative Commons BY license
  •   Request permissions

    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, 8, 5172
    DOI: 10.1039/C7SC01277B

    This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material.

    Reproduced material should be attributed as follows:

    • For reproduction of material from NJC:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
    • For reproduction of material from PCCP:
      [Original citation] - Published by the PCCP Owner Societies.
    • For reproduction of material from PPS:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
    • For reproduction of material from all other RSC journals:
      [Original citation] - Published by The Royal Society of Chemistry.

    Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.

Search articles by author

Spotlight

Advertisements