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PMID: 8460163 Published · ppublish English Comparative Study Journal Article Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S. Research Support, U.S. Gov't, P.H.S.

Stearoyl-acyl carrier protein delta 9 desaturase from Ricinus communis is a diiron-oxo protein.

Fox BG, Shanklin J, Somerville C, Münck E

Abstract

A gene encoding stearoyl-acyl carrier protein delta 9 desaturase (EC 1.14.99.6) from castor was expressed in Escherichia coli. The purified catalytically active enzyme contained four atoms of iron per homodimer. The desaturase was studied in two oxidation states with Mössbauer spectroscopy in applied fields up to 6.0 T. These studies show conclusively that the oxidized enzyme contains two (identical) clusters consisting of a pair of antiferromagnetically coupled (J > 60 cm-1, H = JS1.S2) Fe3+ sites. The diferric cluster exhibited absorption bands from 300 to 355 nm; addition of azide elicited a charge transfer band at 450 nm. In the presence of dithionite, the clusters were reduced to the diferrous state. Addition of stearoyl-CoA and O2 returned the clusters to the diferric state. These properties are consistent with assigning the desaturase to the class of O2-activating proteins containing diiron-oxo clusters, most notably ribonucleotide reductase and methane monooxygenase hydroxylase. Comparison of the primary structures for these three catalytically diverse proteins revealed a conserved pair of the amino acid sequence -(Asp/Glu)-Glu-Xaa-Arg-His- separated by approximately 100 amino acids. Since each of these proteins can catalyze O2-dependent cleavage of unactivated C--H bonds, we propose that these amino acid sequences represent a biological motif used for the creation of reactive catalytic intermediates. Thus, eukaryotic fatty acid desaturation may proceed via enzymatic generation of a high-valent iron-oxo species derived from the diiron cluster.

MeSH Terms
Amino Acid Sequence Cloning, Molecular Dithionite Escherichia coli/genetics Genes, Plant Iron/analysis Mixed Function Oxygenases/chemistry,genetics Molecular Sequence Data Oligodeoxyribonucleotides Open Reading Frames Oxidation-Reduction Plants, Toxic Polymerase Chain Reaction/methods Recombinant Proteins/chemistry Ricinus/enzymology,genetics Sequence Homology, Amino Acid Spectrophotometry Spectrum Analysis
Chemicals
Oligodeoxyribonucleotides Recombinant Proteins Dithionite Iron Mixed Function Oxygenases acyl-(acyl-carrier-protein)desaturase
Authors & Affiliations
4 authors, click to expand affiliations / ORCID
Fox B G
Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA 15213.
Shanklin J
Somerville C
Münck E
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22 references, click to expand
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Article Info
Journal
Proceedings of the National Academy of Sciences of the United States of America
Abbr.
Proc Natl Acad Sci U S A
ISSN
0027-8424
Published
1993-03-15
Pages
2486-90
Language
English
Region
United States
NLM ID
7505876
PMCID
PMC46112
Subset
IM
Grants
NIGMS NIH HHS · GM-22701 · United States
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