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Homogeneous Water Oxidation by Half-Sandwich Iridium(III) N-Heterocyclic Carbene Complexes with Pendant Hydroxy and Amino Groups
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
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2017 (English)In: ChemSusChem, Vol. 10, no 22, p. 4616-4623Article in journal (Refereed) Published
Abstract [en]

Herein, we report three IrIIICp* complexes with hydroxy- or amino-functionalized N-heterocyclic carbene (NHC) ligands that catalyze efficient water oxidation induced by addition of ceric ammonium nitrate (CAN). The pendant hydroxy or amino groups are very important for activity, and the complexes with heteroatom-functionalized NHC ligands show up to 15 times higher rates of oxygen evolution in CAN-induced water oxidation than a reference IrIIICp* complex without heteroatom functionalization. The formation of molecular high-valent Ir intermediates that are presumably involved in the rate-determining step for water oxidation is established by UV/Vis spectroscopy and ESI-MS under turnover conditions. The hydroxy groups on the NHC ligands, as well as chloride ligands on the iridium center are proposed to structurally stabilize the high-valent species, and thereby improve the catalytic activity. The IrIII complex with a hydroxy-functionalized NHC shows the highest catalytic activity with a TON of 2500 obtained in 3 h and with ~90 % yield relative to the amount of oxidant used. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Place, publisher, year, edition, pages
2017. Vol. 10, no 22, p. 4616-4623
Keywords [en]
homogeneous catalysis, iridium, N-heterocyclic carbenes, water oxidation, water splitting
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-335939DOI: 10.1002/cssc.201701370Scopus ID: 2-s2.0-85035067371OAI: oai:DiVA.org:uu-335939DiVA, id: diva2:1164385
Funder
Knut and Alice Wallenberg FoundationSwedish Energy AgencySwedish Research Council
Note

Export Date: 11 December 2017; Article

Available from: 2017-12-11 Created: 2017-12-11 Last updated: 2017-12-11

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