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dc.contributor.author
Zipse, Hendrik
dc.contributor.author
Artin, Erin
dc.contributor.author
Wnuk, Stanislaw
dc.contributor.author
Lohman, Gregory J. S.
dc.contributor.author
Martino, Debora Marcela
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dc.contributor.author
Griffin, Robert G.
dc.contributor.author
Kacprzak, Sylwia
dc.contributor.author
Kaupp, Martin
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Hoffman, Brian
dc.contributor.author
Bennati, Marina
dc.contributor.author
Stubbe, JoAnne
dc.contributor.author
Lees, Nicholas
dc.date.available
2017-05-30T19:19:19Z
dc.date.issued
2009-12
dc.identifier.citation
Zipse, Hendrik; Artin, Erin; Wnuk, Stanislaw; Lohman, Gregory J. S.; Martino, Debora Marcela; et al.; Structure of the nucleotide radical formed during reaction of CDP/TTP with the E441Q-a2b2 of E. coli ribonucleotide reductase; American Chemical Society; Journal Of The American Chemical Society; 131; 1; 12-2009; 200-211
dc.identifier.issn
0002-7863
dc.identifier.uri
http://hdl.handle.net/11336/17116
dc.description.abstract
The Escherichia coli ribonucleotide reductase (RNR) catalyzes the conversion of nucleoside diphosphates to deoxynucleotides and requires a diferric-tyrosyl radical cofactor for catalysis. RNR is composed of a 1:1 complex of two homodimeric subunits: alpha and beta. Incubation of the E441Q-R mutant RNR with substrate CDP and allosteric effector TTP results in loss of the tyrosyl radical and formation of two new radicals on the 200 ms to min time scale. The first radical was previously established by stopped flow UV/vis spectroscopy and pulsed high field EPR spectroscopy to be a disulfide radical anion. The second radical was proposed to be a 4'-radical of a 3'-keto-2'-deoxycytidine 5'-diphosphate. To identify the structure of the nucleotide radical [1'-2H], [2'-2H], [4'-2H], [5'-2H], [U-13C, 15N], [U-15N], and [5,6 -2H] CDP and [beta-2H] cysteine-R were synthesized and incubated with E441Q-alpha2beta2 and TTP. The nucleotide radical was examined by 9 GHz and 140 GHz pulsed EPR spectroscopy and 35 GHz ENDOR spectroscopy. Substitution of 2H at C4' and C1' altered the observed hyperfine interactions of the nucleotide radical and established that the observed structure was not that predicted. DFT calculations (B3LYP/IGLO-III/B3LYP/ TZVP) were carried out in an effort to recapitulate the spectroscopic observations and lead to a new structure consistent with all of the experimental data. The results indicate, unexpectedly, that the radical is a semidione nucleotide radical of cytidine 5'-diphosphate. The relationship of this radical to the disulfide radical anion is discussed.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
American Chemical Society
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dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
Epr
dc.subject
High Field
dc.subject
Tyrosine
dc.subject.classification
Físico-Química, Ciencia de los Polímeros, Electroquímica
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dc.subject.classification
Ciencias Químicas
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dc.subject.classification
CIENCIAS NATURALES Y EXACTAS
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dc.title
Structure of the nucleotide radical formed during reaction of CDP/TTP with the E441Q-a2b2 of E. coli ribonucleotide reductase
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2017-05-22T14:03:26Z
dc.journal.volume
131
dc.journal.number
1
dc.journal.pagination
200-211
dc.journal.pais
Estados Unidos
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dc.description.fil
Fil: Zipse, Hendrik. Ludwig-Maximilians Universitaet Muenchen; Alemania
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Fil: Artin, Erin. Massachusetts Institute of Technology; Estados Unidos
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Fil: Wnuk, Stanislaw. Florida International University; Estados Unidos
dc.description.fil
Fil: Lohman, Gregory J. S.. Massachusetts Institute of Technology; Estados Unidos
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Fil: Martino, Debora Marcela. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina
dc.description.fil
Fil: Griffin, Robert G.. Massachusetts Institute of Technology; Estados Unidos
dc.description.fil
Fil: Kacprzak, Sylwia. Florida International University; Estados Unidos
dc.description.fil
Fil: Kaupp, Martin. Institute fu¨r Physikalische Chemie; Alemania
dc.description.fil
Fil: Hoffman, Brian. Northwestern University; Estados Unidos
dc.description.fil
Fil: Bennati, Marina. Florida International University; Estados Unidos
dc.description.fil
Fil: Stubbe, JoAnne. Massachusetts Institute of Technology; Estados Unidos
dc.description.fil
Fil: Lees, Nicholas. Northwestern University; Estados Unidos
dc.journal.title
Journal Of The American Chemical Society
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dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1021/ja806693s
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/ja806693s
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