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Redox reactions of a dinuclear manganese complex: the influence of water
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Photochemistry and Molecular Science.
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2008 (English)In: European Journal of Inorganic Chemistry, ISSN 1434-1948, E-ISSN 1099-1948, no 5, 762-770 p.Article in journal (Refereed) Published
Abstract [en]

The redox properties of the dinuclear manganese complex [(Mn2L)-L-III,III(mu-OAC)(2)](+) (1) (where L is the trianion of the heptadentate ligand 2,6-bis{[(3,5-di-tert-butyl-2-hydroxybenzyl)(2-pyridylmethyl)amino]methy l)-4-methylphenol) were studied in acetonitrile solutions containing different concentrations of water. Electrochemical reactions as well as reactions with different chemical and photochemical redox reagents were monitored, using a variety of analytical techniques, namely cyclic voltammetry, UV/Vis spectroelectrochemistry, and EPR spectroscopy. We found that even small concentrations of water influence the compound's redox behaviour significantly, especially the oxidation reactions. As a consequence, the presence of water reduces the overall potential span needed to reach the highest oxidation state observed for 1 (M-2(III,IV)) from its most reduced state (Mn-2(II,II)) to about 1.1 V Higher oxidation states of I are stabilized, most likely by water coordination and the formation of mu-oxido bridge(s) between the two manganese atoms. For reducing conditions, an unprecedented 25-line EPR signal was observed, which might originate from reduced 1 in its Mn-2(II,II) or Mn-2(II,II) state after considerable ligand rearrangement. As complexes like I have been designed to act as potential water oxidation catalysts, the complicated redox- and ligand-exchange chemistry found for 1 in the presence of water, its intended substrate, might be exemplary for many of the dinuclear manganese compounds currently under investigation.

Place, publisher, year, edition, pages
2008. no 5, 762-770 p.
Keyword [en]
manganese, N, O ligands, biomimetic synthesis, redox chemistry, EPR spectroscopy
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:uu:diva-110451DOI: 10.1002/ejic.200700888ISI: 000254593800013OAI: oai:DiVA.org:uu-110451DiVA: diva2:277202
Available from: 2009-11-16 Created: 2009-11-16 Last updated: 2017-12-12Bibliographically approved

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Styring, StenbjornHuang, Ping

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