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Issue 6, 2008
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Formation of stoichiometrically 18O-labelled oxygen from the oxidation of 18O-enriched water mediated by a dinuclear manganese complex—a mass spectrometry and EPR study

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Abstract

Oxygen formation was detected for the oxidations of various multinuclear manganese complexes by oxone (HSO5) in aqueous solution. To determine to what extent water was the source of the evolved O2, H218O isotope-labelling experiments coupled with membrane inlet mass spectrometry (MIMS) were carried out. We discovered that during the reaction of oxone with [Mn2(OAc)2(bpmp)]+ (1), stoichiometrically labelled oxygen (18O2) was formed. This is the first example of a homogeneous reaction mediated by a synthetic manganese complex where the addition of a strong chemical oxidant yields 18O2 with labelling percentages matching the theoretically expected values for the case of both O-atoms originating from water. Experiments using lead acetate as an alternative oxidant supported this finding. A detailed investigation of the reaction by EPR spectroscopy, MIMS and Clark-type oxygen detection enabled us to propose potential reaction pathways.

Graphical abstract: Formation of stoichiometrically 18O-labelled oxygen from the oxidation of 18O-enriched water mediated by a dinuclear manganese complex—a mass spectrometry and EPR study

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Supplementary files

Article information


Submitted
10 Jul 2008
Accepted
14 Aug 2008
First published
18 Sep 2008

Energy Environ. Sci., 2008,1, 668-676
Article type
Paper

Formation of stoichiometrically 18O-labelled oxygen from the oxidation of 18O-enriched water mediated by a dinuclear manganese complex—a mass spectrometry and EPR study

K. Beckmann, H. Uchtenhagen, G. Berggren, M. F. Anderlund, A. Thapper, J. Messinger, S. Styring and P. Kurz, Energy Environ. Sci., 2008, 1, 668
DOI: 10.1039/B811806J

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