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Homogeneous Water Oxidation by Half-Sandwich Iridium(III) N-Heterocyclic Carbene Complexes with Pendant Hydroxy and Amino Groups
Stockholm University, Faculty of Science, Department of Organic Chemistry.ORCID iD: 0000-0002-2856-5295
Stockholm University, Faculty of Science, Department of Organic Chemistry.
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2017 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 10, no 22, p. 4616-4623Article in journal (Refereed) Published
Abstract [en]

Herein, we report three (IrCp)-Cp-III* 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 (IrCp)-Cp-III* 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 highvalent species, and thereby improve the catalytic activity. The Ir-III 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.

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, GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:su:diva-149973DOI: 10.1002/cssc.201701370ISI: 000416158500039OAI: oai:DiVA.org:su-149973DiVA, id: diva2:1169668
Funder
Swedish Research CouncilKnut and Alice Wallenberg FoundationSwedish Energy AgencyAvailable from: 2017-12-29 Created: 2017-12-29 Last updated: 2018-03-12Bibliographically approved

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González Miera, GrecoMartínez-Castro, ElisaMartín-Matute, Belén
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