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Spectroscopic capture and reactivity of a low-spin cobalt(IV)-oxo complex stabilized by binding redox-inactive metal ions

Authors
Hong, S.Pfaff, F.F.Kwon, E.Wang, Y.Seo, M.-S.Bill, E.Ray, K.Nam, W.
Issue Date
Sep-2014
Publisher
John Wiley and Sons Ltd
Citation
Angewandte Chemie - International Edition, v.53, no.39, pp 10403 - 10407
Pages
5
Journal Title
Angewandte Chemie - International Edition
Volume
53
Number
39
Start Page
10403
End Page
10407
URI
https://scholarworks.sookmyung.ac.kr/handle/2020.sw.sookmyung/147271
DOI
10.1002/anie.201405874
ISSN
1433-7851
Abstract
High-valent cobalt-oxo intermediates are proposed as reactive intermediates in a number of cobalt-complexmediated oxidation reactions. Herein we report the spectroscopic capture of low-spin (S = 1/2) Co-oxo species in the presence of redox-inactive metal ions, such as Sc, Ce, Y, and Zn, and the investigation of their reactivity in C-H bond activation and sulfoxidation reactions. Theoretical calculations predict that the binding of Lewis acidic metal ions to the cobaltoxo core increases the electrophilicity of the oxygen atom, resulting in the redox tautomerism of a highly unstable [(TAML)Co(O)] species to a more stable [(TAML)Co(O)(M)] core. The present report supports the proposed role of the redox-inactive metal ions in facilitating the formation of high-valent metal-oxo cores as a necessary step for oxygen evolution in chemistry and biology.
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