Living with Oxygen

Accounts of Chemical Research
Harry B Gray, Jay R Winkler

Abstract

Work on the electronic structures of metal-oxo complexes began in Copenhagen over 50 years ago. This work led to the prediction that tetragonal multiply bonded transition metal-oxos would not be stable beyond the iron-ruthenium-osmium oxo wall in the periodic table and that triply bonded metal-oxos could not be protonated, even in the strongest Brønsted acids. In this theory, only double bonded metal-oxos could attract protons, with basicities being a function of the electron donating ability of ancillary ligands. Such correlations of electronic structure with reactivity have gained importance in recent years, most notably owing to the widespread recognition that high-valent iron-oxos are intermediates in biological reactions critical to life on Earth. In this Account, we focus attention on the oxygenations of inert organic substrates by cytochromes P450, as these reactions involve multiply bonded iron-oxos. We emphasize that P450 iron-oxos are strong oxidants, so strong that they would destroy nearby amino acids if substrates are not oxygenated rapidly; it is our view that these high-valent iron-oxos are such dangerous reactive oxygen species that Nature surely found ways to disable them. Looking more deeply into this matter, ...Continue Reading

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Citations

May 16, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Sachidulal BiswasAchintesh N Biswas
Mar 15, 2020·Angewandte Chemie·Hunter B VibbertMichael D Hopkins
Dec 1, 2020·Trends in Biochemical Sciences·Bernd Moosmann
Feb 18, 2021·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Melanie PaulSonja Herres-Pawlis
Feb 27, 2021·Nature Ecology & Evolution·Jagoda Jabłońska, Dan S Tawfik
Apr 24, 2021·Physical Chemistry Chemical Physics : PCCP·C André Ohlin
Jun 8, 2021·The Journal of Biological Chemistry·Anthony J PastoreAlexander Angerhofer
Jul 9, 2021·Langmuir : the ACS Journal of Surfaces and Colloids·Valery V Belousov, Sergey V Fedorov
Mar 12, 2019·The Journal of Physical Chemistry Letters·Laura Zanetti-PolziStefano Corni
Jun 2, 2020·Journal of the American Chemical Society·Astrid Nilsen-MoeCecilia Tommos
Jan 30, 2019·ACS Central Science·Kana TakematsuJay R Winkler
Oct 12, 2019·Journal of the American Chemical Society·Estella F YeeBrian R Crane
Aug 21, 2021·ACS Catalysis·Daniel Bím, Anastassia N Alexandrova
Jul 16, 2019·Inorganic Chemistry·Yoshihiro Shimoyama, Takahiko Kojima
Dec 24, 2020·Journal of the American Chemical Society·Chang CuiDaniel G Nocera
Jan 8, 2020·Inorganic Chemistry·Julian D RolfesFrank Neese
Dec 31, 2020·The Journal of Physical Chemistry. B·Clorice R ReinhardtSharon Hammes-Schiffer
Jan 14, 2021·Journal of the American Chemical Society·Namita SharmaWonwoo Nam
Oct 20, 2018·Journal of the American Chemical Society·Erik AndrisJana Roithová
Sep 8, 2021·Inorganic Chemistry·Justin L LeeA S Borovik
Dec 18, 2021·Environmental Science & Technology·Virender K SharmaChing-Hua Huang

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Methods Mentioned

BETA
X-ray
cross-linking studies

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