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 : 003841 ( Ncbi/Checkpoint ); précédent : 003840; suivant : 003842Structural 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
Affiliations:
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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>
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<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>
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<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>
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</author>
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<biblStruct><analytic><author><name sortKey="Gong, W" uniqKey="Gong W">W. Gong</name>
</author>
<author><name sortKey="Hao, B" uniqKey="Hao B">B. Hao</name>
</author>
<author><name sortKey="Wei, Z" uniqKey="Wei Z">Z. Wei</name>
</author>
<author><name sortKey="Ferguson, D J" uniqKey="Ferguson D">D. J. Ferguson</name>
</author>
<author><name sortKey="Tallant, T" uniqKey="Tallant T">T. Tallant</name>
</author>
<author><name sortKey="Krzycki, J A" uniqKey="Krzycki J">J. A. Krzycki</name>
</author>
<author><name sortKey="Chan, M K" uniqKey="Chan M">M. K. Chan</name>
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</analytic>
</biblStruct>
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<author><name sortKey="Stowell, M H B" uniqKey="Stowell M">M. H. B. Stowell</name>
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<author><name sortKey="Soltis, S M" uniqKey="Soltis S">S. M. Soltis</name>
</author>
<author><name sortKey="Finnegan, M G" uniqKey="Finnegan M">M. G. Finnegan</name>
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<author><name sortKey="Johnson, M K" uniqKey="Johnson M">M. K. Johnson</name>
</author>
<author><name sortKey="Rees, D C" uniqKey="Rees D">D. C. Rees</name>
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</author>
<author><name sortKey="Peters, J C" uniqKey="Peters J">J. C. Peters</name>
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</analytic>
</biblStruct>
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Santen</name>
</author>
<author><name sortKey="Ciobica, I M" uniqKey="Ciobica I">I. M. Ciobica</name>
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<author><name sortKey="Van Steen, E" uniqKey="Van Steen E">E. van Steen</name>
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<author><name sortKey="Ghouri, M M" uniqKey="Ghouri M">M. M. Ghouri</name>
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<biblStruct><analytic><author><name sortKey="Pichler, H" uniqKey="Pichler H">H. Pichler</name>
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<author><name sortKey="Schulz, H" uniqKey="Schulz H">H. Schulz</name>
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</analytic>
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<affiliations><list><country><li>Allemagne</li>
<li>Japon</li>
<li>États-Unis</li>
</country>
</list>
<tree><country name="États-Unis"><noRegion><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>
</noRegion>
<name sortKey="Cramer, Stephen P" sort="Cramer, Stephen P" uniqKey="Cramer S" first="Stephen P." last="Cramer">Stephen P. Cramer</name>
<name sortKey="Cramer, Stephen P" sort="Cramer, Stephen P" uniqKey="Cramer S" first="Stephen P." last="Cramer">Stephen P. Cramer</name>
<name sortKey="Dapper, Christie H" sort="Dapper, Christie H" uniqKey="Dapper C" first="Christie H." last="Dapper">Christie H. Dapper</name>
<name sortKey="George, Simon J" sort="George, Simon J" uniqKey="George S" first="Simon J." last="George">Simon J. George</name>
<name sortKey="Guo, Yisong" sort="Guo, Yisong" uniqKey="Guo Y" first="Yisong" last="Guo">Yisong Guo</name>
<name sortKey="Newton, William E" sort="Newton, William E" uniqKey="Newton W" first="William E." last="Newton">William E. Newton</name>
<name sortKey="Wang, Hongxin" sort="Wang, Hongxin" uniqKey="Wang H" first="Hongxin" last="Wang">Hongxin Wang</name>
<name sortKey="Wang, Hongxin" sort="Wang, Hongxin" uniqKey="Wang H" first="Hongxin" last="Wang">Hongxin Wang</name>
<name sortKey="Yan, Lifen" sort="Yan, Lifen" uniqKey="Yan L" first="Lifen" last="Yan">Lifen Yan</name>
</country>
<country name="Allemagne"><noRegion><name sortKey="Pelmenschikov, Vladimir" sort="Pelmenschikov, Vladimir" uniqKey="Pelmenschikov V" first="Vladimir" last="Pelmenschikov">Vladimir Pelmenschikov</name>
</noRegion>
</country>
<country name="Japon"><noRegion><name sortKey="Yoda, Yoshitaka" sort="Yoda, Yoshitaka" uniqKey="Yoda Y" first="Yoshitaka" last="Yoda">Yoshitaka Yoda</name>
</noRegion>
<name sortKey="Tanaka, Yoshihito" sort="Tanaka, Yoshihito" uniqKey="Tanaka Y" first="Yoshihito" last="Tanaka">Yoshihito Tanaka</name>
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