Synthesis, characterisation and application of iridium(III) photosensitisers for catalytic water reduction |
| |
Authors: | Gärtner Felix Cozzula Daniela Losse Sebastian Boddien Albert Anilkumar Gopinatan Junge Henrik Schulz Thomas Marquet Nicolas Spannenberg Anke Gladiali Serafino Beller Matthias |
| |
Institution: | 1. Leibniz‐Institut für Katalyse e.V. Albert‐Einstein‐Stra?e 29a, 18059 Rostock (Germany), Fax: (+49)?381‐1281‐5000;2. Università di Sassari, Dipartimento di Chimica, Via Vienna 2, 07100 Sassari (Italy) |
| |
Abstract: | The synthesis of novel, monocationic iridium(III) photosensitisers (Ir-PSs) with the general formula Ir(III)(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 HNEt(3)]HFe(3)(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)]PF(6) (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 HNEt(3)]HFe(3)(CO)(11)] and tris3,5-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. |
| |
Keywords: | hydrogen iridium iron photochemistry photosensitizers water splitting |
本文献已被 PubMed 等数据库收录! |
|