Photolytic water oxidation catalyzed by a molecular carbene iridium complex
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Title: | Photolytic water oxidation catalyzed by a molecular carbene iridium complex | Authors: | Petronilho, Ana Rahman, Mahfujur Woods, James A. Al-Sayyed, Haris Müller-Bunz, Helge MacElroy, J. M. Don Bernhard, Stefan Albrecht, Martin |
Permanent link: | http://hdl.handle.net/10197/6606 | Date: | 10-Oct-2012 | Online since: | 2015-06-16T14:03:22Z | Abstract: | The complex IrCl2(Cp*)(trz) (trz = triazolylidene), 2, was prepared from readily available 1,3-dimethyl-4-phenyl-1,2,3-triazolium salt. Under basic conditions, the C-bound phenyl group readily cyclometalates, while under acidic conditions, cyclometalation is reversed. The sensitivity of the Caryl–Ir bond but not the Ctrz–Ir bond towards acidolysis provided a basis for using 2 as a catalyst in CeIV-mediated water oxidation. The catalytic activity is characterized by a robust catalytic cycle, affording excellent turnover numbers (TON > 20 000). Under cerium-free conditions and in the presence of hematite as a photoelectrode, light-induced activity was observed. The photoelectrochemical reaction is strongly pH-dependent, which requires pH adjustments when running multiple cycle experiments to regenerate the catalytic activity. Analogous chelating complexes display better stability and higher catalytic activity than the monodentate complex 2. | Funding Details: | European Research Council Science Foundation Ireland |
Type of material: | Journal Article | Publisher: | Royal Society of Chemistry | Journal: | Dalton Transactions | Volume: | 41 | Issue: | 42 | Start page: | 13074 | End page: | 13080 | Copyright (published version): | 2012 The Royal Society of Chemistry | Keywords: | Catalysis; Water oxidation; Sustainable energy sources | DOI: | 10.1039/C2DT30403A | Language: | en | Status of Item: | Peer reviewed |
Appears in Collections: | Solar Energy Conversion (SEC) Cluster Research Collection Chemical and Bioprocess Engineering Research Collection Chemistry Research Collection |
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