A Balancing Act: Stability versus Reactivity of Mn(O) Complexes

Accounts of Chemical Research
Heather M NeuDavid P Goldberg

Abstract

A large class of heme and non-heme metalloenzymes utilize O2 or its derivatives (e.g., H2O2) to generate high-valent metal-oxo intermediates for performing challenging and selective oxidations. Due to their reactive nature, these intermediates are often short-lived and very difficult to characterize. Synthetic chemists have sought to prepare analogous metal-oxo complexes with ligands that impart enough stability to allow for their characterization and an examination of their inherent reactivity. The challenge in designing these molecules is to achieve a balance between their stability, which should allow for their in situ characterization or isolation, and their reactivity, in which they can still participate in interesting chemical transformations. This Account focuses on our recent efforts to generate and stabilize high-valent manganese-oxo porphyrinoid complexes and tune their reactivity in the oxidation of organic substrates. Dioxygen can be used to generate a high-valent Mn(V)(O) corrolazine (Mn(V)(O)(TBP8Cz)) by irradiation of Mn(III)(TBP8Cz) with visible light in the presence of a C-H substrate. Quantitative formation of the Mn(V)(O) complex occurs with concomitant selective hydroxylation of the benzylic substrate hexame...Continue Reading

References

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Citations

Apr 14, 2016·International Journal of Molecular Sciences·Sam P de Visser, Martin J Stillman
Jun 4, 2016·Organic Letters·Hiroto OmoriHiroshi Shinokubo
Jul 28, 2016·Journal of the American Chemical Society·Surin KimWonwoo Nam
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Sep 5, 2018·Accounts of Chemical Research·Wonwoo NamShunichi Fukuzumi
Jun 16, 2018·Journal of the American Chemical Society·Namita SharmaShunichi Fukuzumi
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