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Photosystem II Like Water Oxidation Mechanism in a Bioinspired Tetranuclear Manganese Complex
Stockholm University, Faculty of Science, Department of Organic Chemistry.
Stockholm University, Faculty of Science, Department of Organic Chemistry.
Stockholm University, Faculty of Science, Department of Organic Chemistry.
Stockholm University, Faculty of Science, Department of Organic Chemistry.
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2015 (English)In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 54, no 1, 342-351 p.Article in journal (Refereed) Published
Abstract [en]

The synthesis of Mn-based catalysts to mimic the structural and catalytic properties of the oxygen-evolving complex in photosystem II is a long-standing goal for researchers. An interesting result in this field came with the synthesis of a Mn complex that enables water oxidation driven by the mild single-electron oxidant [Ru(bpy)(3)](3+). On the basis of hybrid density functional calculations, we herein propose a water oxidation mechanism for this bioinspired Mn catalyst, where the crucial O-O bond formation proceeds from the formal Mn-4(IV,IV,IV,V) state by direct coupling of a Mn-IV-bound terminal oxyl radical and a di-Mn bridging oxo group, a mechanism quite similar to the presently leading suggestion for the natural system. Of importance here is that the designed ligand is shown to be redox-active and can therefore store redox equivalents during the catalytic transitions, thereby alleviating the redox processes at the Mn centers.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2015. Vol. 54, no 1, 342-351 p.
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:su:diva-113952DOI: 10.1021/ic5024983ISI: 000347506500042OAI: oai:DiVA.org:su-113952DiVA: diva2:790054
Funder
Swedish Research CouncilKnut and Alice Wallenberg Foundation
Note

AuthorCount:5;

Available from: 2015-02-23 Created: 2015-02-16 Last updated: 2017-12-04Bibliographically approved

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Liao, Rong-ZhenKärkäs, Markus D.Lee, Bao-LinÅkermark, BjörnSiegbahn, Per E. M.
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