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Synthesis, characterisation and application of iridium(III) photosensitisers for catalytic water reduction

Gärtner, Felix and Cozzula, Daniela and Losse, Sebastian and Boddien, Albert and Anilkumar, Gopinatan and Junge, Henrik and Schulz, Thomas and Marquet, Nicolas and Spannenberg, Anke and Gladiali, Serafino Gabriele and Beller, Matthias (2011) Synthesis, characterisation and application of iridium(III) photosensitisers for catalytic water reduction. Chemistry: a European Journal, Vol. 17 (25), p. 6998-7006. ISSN 0947-6539. eISSN 1521-3765. Article.

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DOI: 10.1002/chem.201100235

Abstract

The synthesis of novel, monocationic iridium (III) photosensitisers (Ir-PSs) with the general formula [IrIII(C^N)2(N^N)]+ (C^N: cyclometallating phenylpyridine ligand, N^N: neutral bidentate ligand) is described. The structures obtained were examined by cyclic voltammetry, UV/Vis and photoluminescence spectroscopy and X-ray analysis. All iridium complexes were tested for their ability as photosensitisers to promote homogeneously catalysed hydrogen generation from water. In the presence of [HNEt3]-[HFe3(CO)11] as a water-reduction catalyst (WRC) and triethylamine as a sacrificial reductant (SR), seven of the new iridium complexes showed activity. [Ir(6-iPr-bpy)(ppy)2]PF6 (bpy: 2,2’-bipyridine, ppy: 2-phenylpyridine) turned out to be the most efficient photosensitiser. This complex was also tested in combination with other WRCs based on rhodium, platinum, cobalt and manganese. In all cases, significant hydrogen evolution took place. Maximum turnover numbers of 4550 for this Ir-PS and 2770 for the Fe WRC generated in situ from [HNEt3][HFe3(CO)11] and tris[3,5-bis(trifluoromethyl)phenyl]-phosphine was obtained. These are the highest overall efficiencies for any Ir/Fe water-reduction system reported to date. The incident photon to hydrogen yield reaches 16.4% with the best system.

Item Type:Article
ID Code:6185
Status:Published
Refereed:Yes
Uncontrolled Keywords:Hydrogen, iridium, iron, photochemistry, photosensitizers, water splitting
Subjects:Area 03 - Scienze chimiche > CHIM/04 Chimica industriale
Divisions:001 Università di Sassari > 01 Dipartimenti > Chimica
Publisher:Wiley
ISSN:0947-6539
eISSN:1521-3765
Copyright Holders:© 2011 Wiley-VCH Verlag GmbH&Co. KGaA, Weinheim
Deposited On:23 Jun 2011 18:05

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