Heidinger, Lorenz and Kneuttinger, Andrea C. and Kashiwazaki, Gengo and Weber, Stefan and Carell, Thomas and Schleicher, Erik (2016) Direct observation of a deoxyadenosyl radical in an active enzyme environment. FEBS LETTERS, 590 (24). pp. 4489-4494. ISSN 0014-5793, 1873-3468
Full text not available from this repository. (Request a copy)Abstract
5'-deoxyadenosyl radicals have been proposed as the first common intermediate in the molecular reaction mechanism of the family of radical S-adenosyl-L-methionine (SAM) enzymes. However, this radical species has not yet been directly observed in a catalytically active enzyme environment. In a reduced and SAM-containing C140A mutant of the spore photoproduct lyase from Geobacillus thermodenitrificans, a mutant with altered catalytic activity, we were able to identify an organic radical with pronounced hyperfine structure using electron paramagnetic resonance spectroscopy. Guided by quantum-chemical computations at the density functional theory level of theory, this radical could be tentatively assigned to a deoxyadenosyl radical, which provides first experimental evidence for this intermediate in the reaction mechanism of radical SAM enzymes.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | SPORE-PHOTOPRODUCT-LYASE; DNA-REPAIR ENZYME; S-ADENOSYLMETHIONINE; LYSINE 2,3-AMINOMUTASE; ALLYLIC ANALOG; SAM ENZYMES; INTERMEDIATE; MECHANISM; CATALYSIS; SUPERFAMILY; deoxyadenosyl radical; EPR spectroscopy; radical intermediate; radical SAM enzymes; spore photoproduct lyase |
| Subjects: | 500 Science > 570 Life sciences |
| Divisions: | Biology, Preclinical Medicine > Institut für Biophysik und physikalische Biochemie |
| Depositing User: | Dr. Gernot Deinzer |
| Date Deposited: | 04 Apr 2019 11:13 |
| Last Modified: | 04 Apr 2019 11:13 |
| URI: | https://pred.uni-regensburg.de/id/eprint/3849 |
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