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A Nonheme Iron(III) Superoxide Complex Leads to Sulfur Oxygenation.
Yadav, Sudha; Yadav, Vishal; Siegler, Maxime A; Moënne-Loccoz, Pierre; Jameson, Guy N L; Goldberg, David P.
Affiliation
  • Yadav S; Department of Chemistry, The Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218, United States.
  • Yadav V; Department of Chemistry, The Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218, United States.
  • Siegler MA; Department of Chemistry, The Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218, United States.
  • Moënne-Loccoz P; Department of Chemical Physiology and Biochemistry, Oregon Health & Science University, Portland, Oregon 97239, United States.
  • Jameson GNL; School of Chemistry, Bio21 Molecular Science and Biotechnology Institute, The University of Melbourne, 30 Flemington Road,Parkville, Victoria 3010, Australia.
  • Goldberg DP; Department of Chemistry, The Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218, United States.
J Am Chem Soc ; 146(12): 7915-7921, 2024 03 27.
Article in En | MEDLINE | ID: mdl-38488295
ABSTRACT
A new alkylthiolate-ligated nonheme iron complex, FeII(BNPAMe2S)Br (1), is reported. Reaction of 1 with O2 at -40 °C, or reaction of the ferric form with O2•- at -80 °C, gives a rare iron(III)-superoxide intermediate, [FeIII(O2)(BNPAMe2S)]+ (2), characterized by UV-vis, 57Fe Mössbauer, ATR-FTIR, EPR, and CSIMS. Metastable 2 then converts to an S-oxygenated FeII(sulfinate) product via a sequential O atom transfer mechanism involving an iron-sulfenate intermediate. These results provide evidence for the feasibility of proposed intermediates in thiol dioxygenases.
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Full text: 1 Collection: 01-internacional Database: MEDLINE Main subject: Superoxides / Iron Language: En Journal: J Am Chem Soc Year: 2024 Type: Article Affiliation country: United States
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Full text: 1 Collection: 01-internacional Database: MEDLINE Main subject: Superoxides / Iron Language: En Journal: J Am Chem Soc Year: 2024 Type: Article Affiliation country: United States