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Issue 42, 2012
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Photolytic water oxidation catalyzed by a molecular carbene iridium complex

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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.

Graphical abstract: Photolytic water oxidation catalyzed by a molecular carbene iridium complex

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Publication details

The article was received on 20 Feb 2012, accepted on 16 May 2012 and first published on 16 May 2012


Article type: Paper
DOI: 10.1039/C2DT30403A
Citation: Dalton Trans., 2012,41, 13074-13080
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    Photolytic water oxidation catalyzed by a molecular carbene iridium complex

    A. Petronilho, M. Rahman, J. A. Woods, H. Al-Sayyed, H. Müller-Bunz, J. M. Don MacElroy, S. Bernhard and M. Albrecht, Dalton Trans., 2012, 41, 13074
    DOI: 10.1039/C2DT30403A

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