A Nonheme Iron(III) Superoxide Complex Leads to Sulfur Oxygenation

被引：6

作者：

Yadav, Sudha ^{[1
]}

Yadav, Vishal ^{[1
]}

Siegler, Maxime A. ^{[1
]}

Moenne-Loccoz, Pierre ^{[2
]}

Jameson, Guy N. L. ^{[3
]}

Goldberg, David P. ^{[1
]}

机构：

[1] Johns Hopkins Univ, Dept Chem, Baltimore, MD 21218 USA

[2] Oregon Hlth & Sci Univ, Dept Chem Physiol & Biochem, Portland, OR 97239 USA

[3] Univ Melbourne, Sch Chem, Mol Sci & Biotechnol Inst Bio21, Parkville, Vic 3010, Australia

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2024年 / 146卷 / 12期

关键词：

2-HIS-1-CARBOXYLATE FACIAL TRIAD; CYSTEINE DIOXYGENASE HOMOLOG; SPECTROSCOPIC EVIDENCE; IRON; INTERMEDIATE; ACTIVATION; MECHANISM; OXIDATION; PARKINSONS; SULFINATE;

D O I：

10.1021/jacs.3c12337

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

A new alkylthiolate-ligated nonheme iron complex, Fe-II(BNPA(Me2)S)Br (<bold>1</bold>), is reported. Reaction of <bold>1</bold> with O-2 at -40 degrees C, or reaction of the ferric form with O-2(center dot-) at -80 degrees C, gives a rare iron(III)-superoxide intermediate, [Fe-III(O-2)(BNPA(Me2)S)](+) (<bold>2</bold>), characterized by UV-vis, Fe-57 M & ouml;ssbauer, ATR-FTIR, EPR, and CSIMS. Metastable <bold>2</bold> then converts to an S-oxygenated Fe-II(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.

引用

页码：7915 / 7921

页数：7

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