Issue 6, 2013

Solar fuels generation and molecular systems: is it homogeneous or heterogeneous catalysis?

Abstract

Catalysis is a key enabling technology for solar fuel generation. A number of catalytic systems, either molecular/homogeneous or solid/heterogeneous, have been developed during the last few decades for both the reductive and oxidative multi-electron reactions required for fuel production from water or CO2 as renewable raw materials. While allowing for a fine tuning of the catalytic properties through ligand design, molecular approaches are frequently criticized because of the inherent fragility of the resulting catalysts, when exposed to extreme redox potentials. In a number of cases, it has been clearly established that the true catalytic species is heterogeneous in nature, arising from the transformation of the initial molecular species, which should rather be considered as a pre-catalyst. Whether such a situation is general or not is a matter of debate in the community. In this review, covering water oxidation and reduction catalysts, involving noble and non-noble metal ions, we limit our discussion to the cases in which this issue has been directly and properly addressed as well as those requiring more confirmation. The methodologies proposed for discriminating homogeneous and heterogeneous catalysis are inspired in part by those previously discussed by Finke in the case of homogeneous hydrogenation reaction in organometallic chemistry [J. A. Widegren and R. G. Finke, J. Mol. Catal. A, 2003, 198, 317–341].

Graphical abstract: Solar fuels generation and molecular systems: is it homogeneous or heterogeneous catalysis?

  • This article is part of the themed collection: Solar fuels

Article information

Article type
Review Article
Submitted
13 Aug 2012
First published
20 Nov 2012

Chem. Soc. Rev., 2013,42, 2338-2356

Solar fuels generation and molecular systems: is it homogeneous or heterogeneous catalysis?

V. Artero and M. Fontecave, Chem. Soc. Rev., 2013, 42, 2338 DOI: 10.1039/C2CS35334B

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