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Oxygen activation at a dicobalt centre of a dipyridylethane naphthyridine complex

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Abstract

The mechanism of oxygen activation at a dicobalt bis-μ-hydroxo core is probed by the implementation of synthetic methods to isolate reaction intermediates. Reduction of a dicobalt(III,III) core ligated by the polypyridyl ligand dipyridylethane naphthyridine (DPEN) by two electrons and subsequent protonation result in the release of one water moiety to furnish a dicobalt(II,II) center with an open binding site. This reduced core may be independently isolated by chemical reduction. Variable-temperature 1H NMR and SQUID magnetometry reveal the reduced dicobalt(II,II) intermediate to consist of two low spin Co(II) centers coupled antiferromagnetically. Binding of O2 to the open coordination site of the dicobalt(II,II) core results in the production of an oxygen adduct, which is proposed to be a dicobalt(III,III) peroxo. Electrochemical studies show that the addition of two electrons results in cleavage of the O–O bond.

Graphical abstract: Oxygen activation at a dicobalt centre of a dipyridylethane naphthyridine complex

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Publication details

The article was received on 21 Apr 2018, accepted on 12 Jun 2018 and first published on 12 Jun 2018


Article type: Paper
DOI: 10.1039/C8DT01598H
Citation: Dalton Trans., 2018, Advance Article
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    Oxygen activation at a dicobalt centre of a dipyridylethane naphthyridine complex

    C. N. Brodsky, G. Passard, A. M. Ullman, D. E. Jaramillo, E. D. Bloch, M. Huynh, D. Gygi, C. Costentin and D. G. Nocera, Dalton Trans., 2018, Advance Article , DOI: 10.1039/C8DT01598H

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