Site-selective formation of an iron(iv)-oxo species at the more electron-rich iron atom of heteroleptic μ-nitrido diiron phthalocyanines

Chemical Science
Ümit İşciSam P de Visser

Abstract

Iron(iv)-oxo species have been identified as the active intermediates in key enzymatic processes, and their catalytic properties are strongly affected by the equatorial and axial ligands bound to the metal, but details of these effects are still unresolved. In our aim to create better and more efficient oxidants of H-atom abstraction reactions, we have investigated a unique heteroleptic diiron phthalocyanine complex. We propose a novel intramolecular approach to determine the structural features that govern the catalytic activity of iron(iv)-oxo sites. Heteroleptic μ-nitrido diiron phthalocyanine complexes having an unsubstituted phthalocyanine (Pc1) and a phthalocyanine ligand substituted with electron-withdrawing alkylsulfonyl groups (PcSO2R) were prepared and characterized. A reaction with terminal oxidants gives two isomeric iron(iv)-oxo and iron(iii)-hydroperoxo species with abundances dependent on the equatorial ligand. Cryospray ionization mass spectrometry (CSI-MS) characterized both hydroperoxo and diiron oxo species in the presence of H2O2. When m-CPBA was used as the oxidant, the formation of diiron oxo species (PcSO2R)FeNFe(Pc1)[double bond, length as m-dash]O was also evidenced. Sufficient amounts of these transien...Continue Reading

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Citations

Sep 28, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Gourab MukherjeeSam P de Visser
Nov 21, 2018·Chemistry : a European Journal·Taniyuki FuruyamaMasahito Segi
Jun 13, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Fabián G Cantú ReinhardSam P de Visser
Sep 29, 2019·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·M Qadri E MubarakSam P de Visser
Apr 22, 2016·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Abayomi S FaponleSam P de Visser
Nov 1, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Andrey P KroitorAlexander B Sorokin
Apr 14, 2016·International Journal of Molecular Sciences·Sam P de Visser, Martin J Stillman
Jun 13, 2018·Nature Communications·Keiko KawauchiDaisuke Miyoshi
Oct 2, 2015·International Journal of Molecular Sciences·Mala A Sainna, Sam P de Visser
Apr 30, 2019·Frontiers in Chemistry·Matthew G QuesneC Richard A Catlow
Dec 24, 2015·Chemistry : a European Journal·Matthew G QuesneSam P de Visser
Jul 11, 2018·International Journal of Molecular Sciences·Verònica PostilsSam P de Visser
Jan 15, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Lucie P CaillerAlexander B Sorokin
Apr 29, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Yasuyuki YamadaKentaro Tanaka
Mar 12, 2016·Accounts of Chemical Research·Pavel Afanasiev, Alexander B Sorokin
Dec 30, 2017·Chemical Reviews·Xiongyi Huang, John T Groves
May 14, 2019·Inorganic Chemistry·Sk Asif IkbalAlexandre Martinez
Jan 19, 2022·Journal of the American Chemical Society·Jeonguk KweonSukbok Chang

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