Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 32, Pages 13236-13239Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja306089q
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Funding
- Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan [21350037]
- Creating Research Center for Advanced Molecular Biochemistry, Strategic Development of Research Infrastructure for Private Universities, from MEXT
- Grants-in-Aid for Scientific Research [21350037] Funding Source: KAKEN
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The conversion of peroxodiiron(III) to high-spin S = 2 oxodiiron(IV) via reversible O-O bond scission in a diiron complex with a bis-tpa dinucleating ligand, 6-hpa, has been characterized by elemental analysis; kinetic measurements for alkene epoxidation; cold-spray ionization mass spectrometry; and electronic absorption, Mossbauer, and resonance Raman spectroscopy to gain insight into the O-2 activation mechanism of soluble methane monooxygenases. This is the first synthetic example of a high-spin S = 2 oxodiiron(IV) species that oxidizes alkenes to epoxides efficiently. The bistability of the peroxodiiron(III) and high-spin S = 2 oxodiiron(IV) moieties is the key feature for the reversible O-O bond scission.
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