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

Author

Listed:
  • 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)
    Korea Advanced Institute of Science and Technology)

  • Seoung-Tae Kim

    (Center for Catalytic Hydrocarbon Functionalizations, Institute for Basic Science (IBS)
    Korea Advanced Institute of Science and Technology)

  • 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)
    Korea Advanced Institute of Science and Technology)

  • Kallol Ray

    (Humboldt-Universität zu Berlin, Brook Taylor Strasse 2)

  • Jason Shearer

    (University of Nevada)

  • Wonwoo Nam

    (Center for Biomimetic Systems, Ewha Womans University
    State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences)

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.

Suggested Citation

  • 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, 2017. "Synthesis and reactivity of a mononuclear non-haem cobalt(IV)-oxo complex," Nature Communications, Nature, vol. 8(1), pages 1-10, April.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_ncomms14839
    DOI: 10.1038/ncomms14839
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    Cited by:

    1. Qianbao Wu & Junwu Liang & Mengjun Xiao & Chang Long & Lei Li & Zhenhua Zeng & Andraž Mavrič & Xia Zheng & Jing Zhu & Hai-Wei Liang & Hongfei Liu & Matjaz Valant & Wei Wang & Zhengxing Lv & Jiong Li &, 2023. "Non-covalent ligand-oxide interaction promotes oxygen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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