Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 17, Issue 25, Pages 6998-7006Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201100235
Keywords
hydrogen; iridium; iron; photochemistry; photosensitizers; water splitting
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Funding
- Evonik Degussa GmbH
- State of North Rhine-Westphalia
- European Union
- BMBF (Spitzenforschung und Innovation in den neuen Landern)
- Fonds der Chemischen Industrie (FCI)
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The synthesis of novel, monocationic iridium(III) photosensitisers (Ir-PSs) with the general formula [Ir-III (C boolean AND N)(2)(N boolean AND N)](+) (C boolean AND N: cyclometal-lating phenylpyridine ligand, N boolean AND 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.
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