期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 129, 期 44, 页码 13408-+出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja076454e
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资金
- NCRR NIH HHS [P20 RR 016461] Funding Source: Medline
- NIGMS NIH HHS [GM 20011, R01 GM058833, GM 49338, R01 GM069657, GM 69657] Funding Source: Medline
The complex of the mononuclear non-heme halogenase CytC3 from Streptomyces, Fe(II), alpha-ketoglutarate, bromide, and the substrate L-2-aminobutyryl-S -CytC2 reacts with 02 to form a reaction intermediate. Variable-field, freeze-quench Mossbauer spectroscopy reveals this intermediate to be a mixture of two high-spin Fe(IV) complexes in an approximate 3.7/1 ratio. Freeze-quench Fe K-edge X-ray absorption spectroscopy provides further insight into the structure of this intermediate. A short 1.62-angstrom interaction between the Fe and one of its ligands is attributed to the Fe(IV)-oxo group, and a 2.43-angstrom interaction is assigned to the Fe-Br interaction. A significantly longer Fe-Br separation (2.53 angstrom) is observed in the reactant complex, consistent with lower valency of the Fe in the reactant complex. This intermediate is the first example for a Br-Fe(IV)-oxo complex in a protein and provides evidence for a unifying mechanism for Fe(II) and a-ketoglutarate-dependent dioxygenases and halogenases.
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