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Catalytic Water Oxidation by a Molecular Ruthenium Complex: Unexpected Generation of a Single-Site Water Oxidation Catalyst
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 Materials and Environmental Chemistry (MMK).
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2015 (English)In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 54, no 10, 4611-4620 p.Article in journal (Refereed) Published
Abstract [en]

The increasing energy demand calls for the development of sustainable energy conversion processes. Here, the splitting of H2O to O-2 and H-2, or related fuels, constitutes an excellent example of solar-to-fuel conversion schemes. The critical component in such schemes has proven to be the catalyst responsible for mediating the four-electron oxidation of H2O to O-2. Herein, we report on the unexpected formation of a single-site Ru complex from a ligand envisioned to accommodate two metal centers. Surprising N-N bond cleavage of the designed dinuclear ligand during metal complexation resulted in a single-site Ru complex carrying a carboxylate amide motif. This ligand lowered the redox potential of the Ru complex sufficiently to permit H2O oxidation to be carried out by the mild one-electron oxidant [Ru(bpy)(3)](3+) (bpy = 2,2'-bipyridine). The work thus highlights that strongly electron-donating ligands are important elements in the design of novel, efficient H2O :oxidation catalysts.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2015. Vol. 54, no 10, 4611-4620 p.
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:su:diva-118542DOI: 10.1021/ic502755cISI: 000354908000008OAI: oai:DiVA.org:su-118542DiVA: diva2:826016
Funder
Swedish Research CouncilKnut and Alice Wallenberg FoundationCarl Tryggers foundation
Available from: 2015-06-24 Created: 2015-06-22 Last updated: 2017-12-04Bibliographically approved

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Rabten, WangchukKärkäs, Markus D.Åkermark, TorbjörnTinnis, FredrikSun, JunliangSiegbahn, Per E. M.Andersson, Pher G.Åkermark, Björn
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Department of Organic ChemistryDepartment of Materials and Environmental Chemistry (MMK)
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