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Molecular ruthenium water oxidation catalysts carrying non-innocent ligands: mechanistic insight through structure-activity relationships and quantum chemical calculations
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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Number of Authors: 7
2016 (English)In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 6, no 5, 1306-1319 p.Article in journal (Refereed) Published
Abstract [en]

Robust catalysts that mediate H2O oxidation are of fundamental importance for the development of novel carbon-neutral energy technologies. Herein we report the synthesis of a group of single-site Ru complexes. Structure-activity studies revealed that the individual steps in the oxidation of H2O depended differently on the electronic properties of the introduced ligand substituents. The mechanistic details associated with these complexes were investigated experimentally along with quantum chemical calculations. It was found that O-O bond formation for the developed Ru complexes proceeds via high-valent Ru-VI species, where the capability of accessing this species is derived from the non-innocent ligand architecture. This cooperative catalytic involvement and the ability of accessing Ru-VI are intriguing and distinguish these Ru catalysts from a majority of previously reported complexes, and might generate unexplored reaction pathways for activation of small molecules such as H2O.

Place, publisher, year, edition, pages
2016. Vol. 6, no 5, 1306-1319 p.
National Category
Organic Chemistry
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URN: urn:nbn:se:su:diva-129099DOI: 10.1039/c5cy01704aISI: 000371607600006OAI: oai:DiVA.org:su-129099DiVA: diva2:921095
Available from: 2016-04-19 Created: 2016-04-14 Last updated: 2016-04-19Bibliographically approved

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Kärkäs, Markus D.Laine, Tanja M.Siegbahn, Per E. M.Åkermark, Björn
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Department of Organic Chemistry
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