Structural Characterization of CO-Inhibited Mo-Nitrogenase by Combined Application of Nuclear Resonance Vibrational Spectroscopy, Extended X-ray Absorption Fine Structure, and Density Functional Theory: New Insights into the Effects of CO Binding and the Role of the Interstitial Atom
Identifieur interne : 001145 ( Main/Curation ); précédent : 001144; suivant : 001146Structural Characterization of CO-Inhibited Mo-Nitrogenase by Combined Application of Nuclear Resonance Vibrational Spectroscopy, Extended X-ray Absorption Fine Structure, and Density Functional Theory: New Insights into the Effects of CO Binding and the Role of the Interstitial Atom
Auteurs : Aubrey X0a D. Scott [États-Unis] ; Vladimir Pelmenschikov [Allemagne] ; Yisong Guo [États-Unis] ; Lifen Yan [États-Unis] ; Hongxin Wang [États-Unis] ; Simon J. George [États-Unis] ; Christie H. Dapper [États-Unis] ; William E. Newton [États-Unis] ; Yoshitaka Yoda [Japon] ; Yoshihito Tanaka [Japon] ; Stephen P. Cramer [États-Unis]Source :
- Journal of the American Chemical Society [ 0002-7863 ] ; 2014.
Abstract
The properties of CO-inhibited
Url:
DOI: 10.1021/ja505720m
PubMed: 25275608
PubMed Central: 4235365
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PMC:4235365Le document en format XML
<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en">Structural
Characterization of CO-Inhibited Mo-Nitrogenase
by Combined Application of Nuclear Resonance Vibrational Spectroscopy,
Extended X-ray Absorption Fine Structure, and Density Functional
Theory: New Insights into the Effects of CO Binding and the Role of
the Interstitial Atom</title><author><name sortKey="Scott, Aubrey X0a D" sort="Scott, Aubrey X0a D" uniqKey="Scott A" first="Aubrey X0a D." last="Scott">Aubrey X0a D. Scott</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Pelmenschikov, Vladimir" sort="Pelmenschikov, Vladimir" uniqKey="Pelmenschikov V" first="Vladimir" last="Pelmenschikov">Vladimir Pelmenschikov</name><affiliation wicri:level="1"><nlm:aff id="aff1">Institut für Chemie,<institution>Technische Universität Berlin</institution>, 10623 Berlin,<country>Germany</country></nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Guo, Yisong" sort="Guo, Yisong" uniqKey="Guo Y" first="Yisong" last="Guo">Yisong Guo</name><affiliation wicri:level="1"><nlm:aff id="aff3">Department of Chemistry,<institution>Carnegie Mellon University</institution>, Pittsburgh, Pennsylvania 15213,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Yan, Lifen" sort="Yan, Lifen" uniqKey="Yan L" first="Lifen" last="Yan">Lifen Yan</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Wang, Hongxin" sort="Wang, Hongxin" uniqKey="Wang H" first="Hongxin" last="Wang">Hongxin Wang</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="aff4">Physical Biosciences Division,<institution>Lawrence Berkeley National Laboratory</institution>, Berkeley, California 94720,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="George, Simon J" sort="George, Simon J" uniqKey="George S" first="Simon J." last="George">Simon J. George</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Dapper, Christie H" sort="Dapper, Christie H" uniqKey="Dapper C" first="Christie H." last="Dapper">Christie H. Dapper</name><affiliation wicri:level="1"><nlm:aff id="aff5">Department of Biochemistry,<institution>Virginia Polytechnic Institute & State University</institution>, Blacksburg, Virginia 24061,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Newton, William E" sort="Newton, William E" uniqKey="Newton W" first="William E." last="Newton">William E. Newton</name><affiliation wicri:level="1"><nlm:aff id="aff5">Department of Biochemistry,<institution>Virginia Polytechnic Institute & State University</institution>, Blacksburg, Virginia 24061,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Yoda, Yoshitaka" sort="Yoda, Yoshitaka" uniqKey="Yoda Y" first="Yoshitaka" last="Yoda">Yoshitaka Yoda</name><affiliation wicri:level="1"><nlm:aff id="aff6">Research and Utilization Division,<institution>SPring-8/JASRI</institution>, 1-1-1 Kouto, Sayo, Hyogo 679-5198,<country>Japan</country></nlm:aff><country xml:lang="fr">Japon</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Tanaka, Yoshihito" sort="Tanaka, Yoshihito" uniqKey="Tanaka Y" first="Yoshihito" last="Tanaka">Yoshihito Tanaka</name><affiliation wicri:level="1"><nlm:aff id="aff7">SR Materials Science Instrumentation Unit,<institution>RIKEN SPring-8 Center</institution>, 1-1-1 Kouto, Sayo, Hyogo 679-5148,<country>Japan</country></nlm:aff><country xml:lang="fr">Japon</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Cramer, Stephen P" sort="Cramer, Stephen P" uniqKey="Cramer S" first="Stephen P." last="Cramer">Stephen P. Cramer</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="aff4">Physical Biosciences Division,<institution>Lawrence Berkeley National Laboratory</institution>, Berkeley, California 94720,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author></titleStmt><publicationStmt><idno type="wicri:source">PMC</idno><idno type="pmid">25275608</idno><idno type="pmc">4235365</idno><idno type="url">http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4235365</idno><idno type="RBID">PMC:4235365</idno><idno type="doi">10.1021/ja505720m</idno><date when="2014">2014</date><idno type="wicri:Area/Pmc/Corpus">000330</idno><idno type="wicri:explorRef" wicri:stream="Pmc" wicri:step="Corpus" wicri:corpus="PMC">000330</idno><idno type="wicri:Area/Pmc/Curation">000330</idno><idno type="wicri:explorRef" wicri:stream="Pmc" wicri:step="Curation">000330</idno><idno type="wicri:Area/Pmc/Checkpoint">000500</idno><idno type="wicri:explorRef" wicri:stream="Pmc" wicri:step="Checkpoint">000500</idno><idno type="wicri:Area/Ncbi/Merge">003841</idno><idno type="wicri:Area/Ncbi/Curation">003841</idno><idno type="wicri:Area/Ncbi/Checkpoint">003841</idno><idno type="wicri:doubleKey">0002-7863:2014:Scott A:structural:x:a</idno><idno type="wicri:Area/Main/Merge">001168</idno><idno type="wicri:Area/Main/Curation">001145</idno></publicationStmt><sourceDesc><biblStruct><analytic><title xml:lang="en" level="a" type="main">Structural
Characterization of CO-Inhibited Mo-Nitrogenase
by Combined Application of Nuclear Resonance Vibrational Spectroscopy,
Extended X-ray Absorption Fine Structure, and Density Functional
Theory: New Insights into the Effects of CO Binding and the Role of
the Interstitial Atom</title><author><name sortKey="Scott, Aubrey X0a D" sort="Scott, Aubrey X0a D" uniqKey="Scott A" first="Aubrey X0a D." last="Scott">Aubrey X0a D. Scott</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Pelmenschikov, Vladimir" sort="Pelmenschikov, Vladimir" uniqKey="Pelmenschikov V" first="Vladimir" last="Pelmenschikov">Vladimir Pelmenschikov</name><affiliation wicri:level="1"><nlm:aff id="aff1">Institut für Chemie,<institution>Technische Universität Berlin</institution>, 10623 Berlin,<country>Germany</country></nlm:aff><country xml:lang="fr">Allemagne</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Guo, Yisong" sort="Guo, Yisong" uniqKey="Guo Y" first="Yisong" last="Guo">Yisong Guo</name><affiliation wicri:level="1"><nlm:aff id="aff3">Department of Chemistry,<institution>Carnegie Mellon University</institution>, Pittsburgh, Pennsylvania 15213,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Yan, Lifen" sort="Yan, Lifen" uniqKey="Yan L" first="Lifen" last="Yan">Lifen Yan</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Wang, Hongxin" sort="Wang, Hongxin" uniqKey="Wang H" first="Hongxin" last="Wang">Hongxin Wang</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="aff4">Physical Biosciences Division,<institution>Lawrence Berkeley National Laboratory</institution>, Berkeley, California 94720,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="George, Simon J" sort="George, Simon J" uniqKey="George S" first="Simon J." last="George">Simon J. George</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Dapper, Christie H" sort="Dapper, Christie H" uniqKey="Dapper C" first="Christie H." last="Dapper">Christie H. Dapper</name><affiliation wicri:level="1"><nlm:aff id="aff5">Department of Biochemistry,<institution>Virginia Polytechnic Institute & State University</institution>, Blacksburg, Virginia 24061,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Newton, William E" sort="Newton, William E" uniqKey="Newton W" first="William E." last="Newton">William E. Newton</name><affiliation wicri:level="1"><nlm:aff id="aff5">Department of Biochemistry,<institution>Virginia Polytechnic Institute & State University</institution>, Blacksburg, Virginia 24061,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Yoda, Yoshitaka" sort="Yoda, Yoshitaka" uniqKey="Yoda Y" first="Yoshitaka" last="Yoda">Yoshitaka Yoda</name><affiliation wicri:level="1"><nlm:aff id="aff6">Research and Utilization Division,<institution>SPring-8/JASRI</institution>, 1-1-1 Kouto, Sayo, Hyogo 679-5198,<country>Japan</country></nlm:aff><country xml:lang="fr">Japon</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Tanaka, Yoshihito" sort="Tanaka, Yoshihito" uniqKey="Tanaka Y" first="Yoshihito" last="Tanaka">Yoshihito Tanaka</name><affiliation wicri:level="1"><nlm:aff id="aff7">SR Materials Science Instrumentation Unit,<institution>RIKEN SPring-8 Center</institution>, 1-1-1 Kouto, Sayo, Hyogo 679-5148,<country>Japan</country></nlm:aff><country xml:lang="fr">Japon</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author><author><name sortKey="Cramer, Stephen P" sort="Cramer, Stephen P" uniqKey="Cramer S" first="Stephen P." last="Cramer">Stephen P. Cramer</name><affiliation wicri:level="1"><nlm:aff id="aff2">Department of Chemistry,<institution>University of California</institution>, Davis, California 95616,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation><affiliation wicri:level="1"><nlm:aff id="aff4">Physical Biosciences Division,<institution>Lawrence Berkeley National Laboratory</institution>, Berkeley, California 94720,<country>United States</country></nlm:aff><country xml:lang="fr">États-Unis</country><wicri:regionArea># see nlm:aff country strict</wicri:regionArea></affiliation></author></analytic><series><title level="j">Journal of the American Chemical Society</title><idno type="ISSN">0002-7863</idno><idno type="eISSN">1520-5126</idno><imprint><date when="2014">2014</date></imprint></series></biblStruct></sourceDesc></fileDesc><profileDesc><textClass></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en"><p content-type="toc-graphic"><graphic xlink:href="ja-2014-05720m_0010" id="ab-tgr1"></graphic></p><p>The properties of CO-inhibited <italic><italic>Azotobacter
vinelandii</italic></italic> (<italic>Av</italic>) Mo-nitrogenase
(N<sub>2</sub>ase) have been examined by the combined application
of nuclear resonance vibrational spectroscopy (NRVS), extended X-ray
absorption fine structure (EXAFS), and density functional theory (DFT).
Dramatic changes in the NRVS are seen under high-CO conditions, especially
in a 188 cm<sup>–1</sup> mode associated with symmetric breathing
of the central cage of the FeMo-cofactor. Similar changes are reproduced
with the α-H195Q N<sub>2</sub>ase variant. In the frequency
region above 450 cm<sup>–1</sup>, additional features are seen
that are assigned to Fe-CO bending and stretching modes (confirmed
by <sup>13</sup>CO isotope shifts). The EXAFS for wild-type N<sub>2</sub>ase shows evidence for a significant cluster distortion under
high-CO conditions, most dramatically in the splitting of the interaction
between Mo and the shell of Fe atoms originally at 5.08 Å in
the resting enzyme. A DFT model with both a terminal −CO and
a partially reduced −CHO ligand bound to adjacent Fe sites
is consistent with both earlier FT-IR experiments, and the present
EXAFS and NRVS observations for the wild-type enzyme. Another DFT
model with two terminal CO ligands on the adjacent Fe atoms yields
Fe-CO bands consistent with the α-H195Q variant NRVS. The calculations
also shed light on the vibrational “shake” modes of
the interstitial atom inside the central cage, and their interaction
with the Fe-CO modes. Implications for the CO and N<sub>2</sub> reactivity
of N<sub>2</sub>ase are discussed.</p></div></front><back><div1 type="bibliography"><listBibl><biblStruct><analytic><author><name sortKey="Hoffman, B M" uniqKey="Hoffman B">B. M. Hoffman</name></author><author><name sortKey="Dean, D R" uniqKey="Dean D">D. R. Dean</name></author><author><name sortKey="Seefeldt, L C" uniqKey="Seefeldt L">L. C. Seefeldt</name></author></analytic></biblStruct><biblStruct><analytic><author><name sortKey="Burgess, B X0a K" uniqKey="Burgess B">B.
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|texte= Structural
Characterization of CO-Inhibited Mo-Nitrogenase
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Extended X-ray Absorption Fine Structure, and Density Functional
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