Dioxygenase-like reactivity of an isolable superoxo-nickel(II) complex

Chemistry : a European Journal
Anna CompanyMatthias Driess

Abstract

Although O(2) activation by metals such as iron and copper has been a matter of intensive research in the last decades, this type of chemistry for nickel systems is still in its infancy. Moreover, studies regarding the oxidizing ability of the resulting "Ni(n)-O(2)" species towards exogenous substrates are scarce. In this work, we report on the reactivity of an isolable and thermally stable mononuclear superoxo-nickel compound [Ni(II)(beta-diketiminato)(O(2))] (1) towards different types of organic substrates. In addition, we have been able to prove that the beta-diketiminato ligand can undergo partial intramolecular oxidation due to close proximity between the isopropyl groups of the beta-diketiminato-aryl and the superoxo subunits. Compound 1 performs hydrogen-atom abstraction from O-H and N-H groups and most importantly it shows an unprecedented dioxygenase-like reactivity in the oxidation of 2,4,6-tri-tert-butylphenol. The latter reaction most likely occurs through the mediation of a putative [Ni(III)-oxo] intermediate, affording an unprecedented oxidation product of the phenol that incorporates two oxygen atoms from a single O(2) subunit. Results presented herein provide evidence of the striking oxidizing ability of dioxyg...Continue Reading

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Citations

Jul 30, 2016·Angewandte Chemie·Subrata KunduTimothy H Warren
Mar 24, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Lin-Lin ZhangChi-Ming Che
Jan 5, 2019·Chemical Communications : Chem Comm·Jireh Joy D Sacramento, David P Goldberg
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Jan 23, 2014·Dalton Transactions : an International Journal of Inorganic Chemistry·Samir Ghorai, Chandan Mukherjee
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Nov 27, 2010·ChemSusChem·Sebastian Losse, Henrik Junge
Aug 4, 2016·Chemistry : a European Journal·Teresa Corona, Anna Company
Oct 17, 2017·Chemical Communications : Chem Comm·Teresa CoronaAnna Company
Aug 18, 2017·Chemistry : a European Journal·Frauke MöllerUlf-Peter Apfel
Aug 12, 2014·Dalton Transactions : an International Journal of Inorganic Chemistry·Lisa A-M HarrisJ Robin Fulton
Feb 29, 2020·Chemical Science·Sofia M SmithLiviu M Mirica
Apr 13, 2021·Angewandte Chemie·Anirban ChandraKallol Ray
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Jun 19, 2012·Inorganic Chemistry·Tapash DebMichael P Jensen
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Aug 31, 2011·Accounts of Chemical Research·Shenglai Yao, Matthias Driess
Sep 13, 2014·Journal of the American Chemical Society·Kallol RayWonwoo Nam

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