Dye-sensitised semiconductors modified with molecular catalysts for light-driven H₂ production

This is the final version of the article. It was first available from RSC via http://dx.doi.org/10.1039/C5CS00733JThe development of synthetic systems for the conversion of solar energy into chemical fuels is a research goal that continues to attract growing interest owing to its potential to provide renewable and storable energy in the form of a ?solar fuel?. Dye-sensitised photocatalysis (DSP) with molecular catalysts is a relatively new approach to convert sunlight into a fuel such as H? and is based on the self-assembly of a molecular dye and electrocatalyst on a semiconductor nanoparticle. DSP systems combine advantages of both homogenous and heterogeneous photocatalysis, with the molecular components providing an excellent platform for tuning activity and understanding performance at defined catalytic sites, whereas the semiconductor bridge ensures favourable multi-electron transfer kinetics between the dye and the fuel-forming electrocatalyst. In this tutorial review, strategies and challenges for the assembly of functional molecular DSP systems and experimental techniques for their evaluation are explained. Current understanding of the factors governing electron transfer across inorganic-molecular interfaces is described and future directions and challenges for this field are outlined.This work was supported by the EPSRC (EP/H00338X/2 to E.R.; DTG scholarship to E.P.), the Christian Doppler Research Association (Austrian Federal Ministry of Science, Research and Economy and National Foundation for Research, Technology and Development; E.R. and J.W.), the OMV Group (E.R. and J.W.), the Advanced Institute for Materials ResearchCambridge Joint Research Centre (K.O.), European Commission Marie Curie CIG (303650 to A.R.) and the ERC (291482 to J.D.)

Dye-sensitised semiconductors modified with molecular catalysts for light-driven H2 production.

The development of synthetic systems for the conversion of solar energy into chemical fuels is a research goal that continues to attract growing interest owing to its potential to provide renewable and storable energy in the form of a 'solar fuel'. Dye-sensitised photocatalysis (DSP) with molecular catalysts is a relatively new approach to convert sunlight into a fuel such as H2 and is based on the self-assembly of a molecular dye and electrocatalyst on a semiconductor nanoparticle. DSP systems combine advantages of both homogenous and heterogeneous photocatalysis, with the molecular components providing an excellent platform for tuning activity and understanding performance at defined catalytic sites, whereas the semiconductor bridge ensures favourable multi-electron transfer kinetics between the dye and the fuel-forming electrocatalyst. In this tutorial review, strategies and challenges for the assembly of functional molecular DSP systems and experimental techniques for their evaluation are explained. Current understanding of the factors governing electron transfer across inorganic-molecular interfaces is described and future directions and challenges for this field are outlined.This work was supported by the EPSRC (EP/H00338X/2 to E.R.; DTG scholarship to E.P.), the Christian Doppler Research Association (Austrian Federal Ministry of Science, Research and Economy and National Foundation for Research, Technology and Development; E.R. and J.W.), the OMV Group (E.R. and J.W.), the Advanced Institute for Materials ResearchCambridge Joint Research Centre (K.O.), European Commission Marie Curie CIG (303650 to A.R.) and the ERC (291482 to J.D.).This is the final version of the article. It was first available from RSC via http://dx.doi.org/10.1039/C5CS00733