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Issue 2, 2009
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Deposition of an oxomanganese water oxidation catalyst on TiO2 nanoparticles: computational modeling, assembly and characterization

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Abstract

Inexpensive water oxidation catalysts are needed to develop photocatalytic solar cells that mimic photosynthesis and produce fuel from sunlight and water. This paper reports the successful attachment of a dinuclear di-µ-oxo manganese water oxidation catalyst [H2O(terpy)MnIII(µ-O)2 MnIV(terpy)H2O](NO3)3 (1, terpy = 2,2′:6′2″-terpyridine) onto TiO2 nanoparticles (NPs) via direct adsorption, or in situ synthesis. The resulting surface complexes are characterized by EPR and UV-visible spectroscopy, electrochemical measurements and computational modeling. We conclude that the mixed-valence (III,IV) state of 1 attaches to near-amorphous TiO2 NPs by substituting one of its water ligands by the TiO2 NP, as suggested by low-temperature (7 K) EPR data. In contrast, the analogous attachment onto well-crystallized TiO2 NPs leads to dimerization of 1 forming Mn(IV) tetramers on the TiO2 surface as suggested by EPR spectroscopy and electrochemical studies.

Graphical abstract: Deposition of an oxomanganese water oxidation catalyst on TiO2 nanoparticles: computational modeling, assembly and characterization

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Publication details

The article was received on 22 Oct 2008, accepted on 04 Dec 2008 and first published on 12 Jan 2009


Article type: Paper
DOI: 10.1039/B818708H
Citation: Energy Environ. Sci., 2009,2, 230-238
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    Deposition of an oxomanganese water oxidation catalyst on TiO2 nanoparticles: computational modeling, assembly and characterization

    G. Li, E. M. Sproviero, R. C. Snoeberger III, N. Iguchi, J. D. Blakemore, R. H. Crabtree, G. W. Brudvig and V. S. Batista, Energy Environ. Sci., 2009, 2, 230
    DOI: 10.1039/B818708H

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