期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 1, 期 6, 页码 668-676出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/b811806j
关键词
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资金
- Swedish Energy Agency
- Knut and Alice Wallenberg Foundation
- NEST-STRP SOLARH [516510]
- Deutsche Forschungsgemeinschaft [Me 1629/2-4]
- Max-Planck-Gesellschaft
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 O-2, (H2O)-O-18 isotope-labelling experiments coupled with membrane inlet mass spectrometry (MIMS) were carried out. We discovered that during the reaction of oxone with [Mn-2(OAc)(2)(bpmp)](+) (1), stoichiometrically labelled oxygen (O-18(2)) 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 O-18(2) 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.
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