期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 131, 期 24, 页码 8340-+出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja9004656
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资金
- National Science Foundation (NSF) [CHE-055664]
In order to determine the origin of the NO photolability of the active site of Fe-containing nitrite hydratase (Fe-NHase), a model complex of the NO-bound active site (dark form) has been isolated and structurally characterized. The model, NEt4[(Cl(2)PhPepS)Fe(NO)(DMAP)] (2), is derived from a tetradentate ligand comprising carboxamido N and thiolato S donor centers much like the donors present in the active site of Fe-NHase. This [{Fe-NO}(6) nitrosyl effectively mimics the NO-bound active site in terms of structural and spectroscopic parameters. However, this model lacks the key property of NO photolability. Interestingly, S-oxygenation of the model complex results in formation of Na[(Cl(2)PhPep{SO2}(2))Fe(NO)(DMAP)] (3), in which the -S donors are oxygenated to -SO2 moieties, and this species exhibits NO photolability. These results indicate that S-oxygenation could be the key reason for the observed NO photolability of the active site of the dark form of Fe-NHase.
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