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
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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: CatalysisWater oxidationSustainable 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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