EXAFS spectroscopic evidence for an Fe=O unit in the Fe(IV) intermediate observed during oxygen activation by taurine:α-ketoglutarate dioxygenase

Journal of the American Chemical Society

Volumn 126, Issue 26, 2004, Pages 8108-8109

  Riggs Gelasco, Pamela J ^a   Price, John C ^b   Guyer, Robert B ^b   Brehm, Jessica H ^a   Barr, Eric W ^b   Bollinger Jr , J Martin ^b   Krebs, Carsten ^b  

^a School of Business   (United States)

^b PENNSYLVANIA STATE UNIVERSITY   (United States)

Author keywords

[No Author keywords available]

Indexed keywords

IRON; OXYGEN; OXYGENASE; TAURINE ALPHA KETOGLUTARATE DIOXYGENASE; UNCLASSIFIED DRUG;

ANALYTIC METHOD; ARTICLE; CHEMICAL BOND; DEGRADATION KINETICS; ENZYME ACTIVATION; EXTENDED X RAY ABSORPTION FINE STRUCTURE SPECTROSCOPY; MOSSBAUER SPECTROSCOPY; OSCILLATION; OXIDATION; SPECTROSCOPY; X RAY SPECTROMETRY;

ESCHERICHIA COLI; IRON; MIXED FUNCTION OXYGENASES; NONHEME IRON PROTEINS; OXYGEN; SPECTRUM ANALYSIS; X-RAYS;

EID: 3042770458     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja048255q     Document Type: Article

References (17)

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3. Abbreviations used: α-KG: α-ketoglutarate; TauD: taurine: α-ketoglutarate dioxygenase; XAS: X-ray absorption spectroscopy; XANES: X-ray absorption near edge spectrum; EXAFS: extended X-ray absorption fine structure; FT: Fourier transform.
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8. 2. 2 was prepared under identical conditions, except that the reaction time was 20 ms and oxygen was excluded. Samples were packed into a sample holder that can be used for Mössbauer and XAS spectroscopies. Mössbauer experiments were carried out as described in reference (5). XAS data were collected at the National Synchrotron Light Source on Beamline X9B. Samples were maintained at T = 14 K with a displex cryostat and the Fe Kα fluorescence was detected with a Canberra 13 element Ge detector. The general protocols for data reduction and curve fitting were described in Riggs-Gelasco et al., J. Am. Chem. Soc. 1996, 118, 2387-2399 and minor modifications are described in the Supporting Information.
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16. The spectrum of 1 shown is the average of 20 first and second scans of several replicate samples. Similar results are obtained if all scans, including scans after 10 h of collection, are averaged for a single sample. Also, if first and second scans are excluded from the average, the short Fe-O distance can still be detected, despite the apparent photoreduction in these scans.
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