Synthesis and reactivity of a mononuclear non-haem cobalt(IV)-oxo complex

Bin Wang, Yong-Min Lee, Woon-Young Tcho, Samat Tussupbayev, Seoung-Tae Kim, Yujeong Kim, Mi Sook Seo, Kyung-Bin Cho, Yavuz Dede, Brenna C. Keegan, Takashi Ogura, Sun Hee Kim (), Takehiro Ohta (), Mu-Hyun Baik (), Kallol Ray (), Jason Shearer () and Wonwoo Nam ()
Additional contact information
Bin Wang: Center for Biomimetic Systems, Ewha Womans University
Yong-Min Lee: Center for Biomimetic Systems, Ewha Womans University
Woon-Young Tcho: Center for Biomimetic Systems, Ewha Womans University
Samat Tussupbayev: Center for Catalytic Hydrocarbon Functionalizations, Institute for Basic Science (IBS)
Seoung-Tae Kim: Center for Catalytic Hydrocarbon Functionalizations, Institute for Basic Science (IBS)
Yujeong Kim: Western Seoul Center, Korea Basic Science Institute
Mi Sook Seo: Center for Biomimetic Systems, Ewha Womans University
Kyung-Bin Cho: Center for Biomimetic Systems, Ewha Womans University
Yavuz Dede: Faculty of Science, Gazi University
Brenna C. Keegan: University of Nevada
Takashi Ogura: Picobiology Institute, Graduate School of Life Science, University of Hyogo, RSC-UH LP Center
Sun Hee Kim: Western Seoul Center, Korea Basic Science Institute
Takehiro Ohta: Picobiology Institute, Graduate School of Life Science, University of Hyogo, RSC-UH LP Center
Mu-Hyun Baik: Center for Catalytic Hydrocarbon Functionalizations, Institute for Basic Science (IBS)
Kallol Ray: Humboldt-Universität zu Berlin, Brook Taylor Strasse 2
Jason Shearer: University of Nevada
Wonwoo Nam: Center for Biomimetic Systems, Ewha Womans University

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: Abstract Terminal cobalt(IV)–oxo (CoIV–O) species have been implicated as key intermediates in various cobalt-mediated oxidation reactions. Herein we report the photocatalytic generation of a mononuclear non-haem [(13-TMC)CoIV(O)]2+ (2) by irradiating [CoII(13-TMC)(CF3SO3)]+ (1) in the presence of [RuII(bpy)3]2+, Na2S2O8, and water as an oxygen source. The intermediate 2 was also obtained by reacting 1 with an artificial oxidant (that is, iodosylbenzene) and characterized by various spectroscopic techniques. In particular, the resonance Raman spectrum of 2 reveals a diatomic Co–O vibration band at 770 cm−1, which provides the conclusive evidence for the presence of a terminal Co–O bond. In reactivity studies, 2 was shown to be a competent oxidant in an intermetal oxygen atom transfer, C–H bond activation and olefin epoxidation reactions. The present results lend strong credence to the intermediacy of CoIV–O species in cobalt-catalysed oxidation of organic substrates as well as in the catalytic oxidation of water that evolves molecular oxygen.

Date: 2017
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DOI: 10.1038/ncomms14839

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