Tuning Catalytic Bias of Hydrogen Gas Producing Hydrogenases.
Identifieur interne : 000007 ( Main/Exploration ); précédent : 000006; suivant : 000008Tuning Catalytic Bias of Hydrogen Gas Producing Hydrogenases.
Auteurs : Jacob H. Artz [États-Unis] ; Oleg A. Zadvornyy [États-Unis] ; David W. Mulder [États-Unis] ; Stephen M. Keable [États-Unis] ; Aina E. Cohen [États-Unis] ; Michael W. Ratzloff [États-Unis] ; S Garrett Williams [États-Unis] ; Bojana Ginovska [États-Unis] ; Neeraj Kumar [États-Unis] ; Jinhu Song [États-Unis] ; Scott E. Mcphillips [États-Unis] ; Catherine M. Davidson [États-Unis] ; Artem Y. Lyubimov [États-Unis] ; Natasha Pence [États-Unis] ; Gerrit J. Schut [États-Unis] ; Anne K. Jones [États-Unis] ; S Michael Soltis [États-Unis] ; Michael W W. Adams [États-Unis] ; Simone Raugei [États-Unis] ; Paul W. King [États-Unis] ; John W. Peters [États-Unis]Source :
- Journal of the American Chemical Society [ 1520-5126 ] ; 2020.
Abstract
Hydrogenases display a wide range of catalytic rates and biases in reversible hydrogen gas oxidation catalysis. The interactions of the iron-sulfur-containing catalytic site with the local protein environment are thought to contribute to differences in catalytic reactivity, but this has not been demonstrated. The microbe Clostridium pasteurianum produces three [FeFe]-hydrogenases that differ in "catalytic bias" by exerting a disproportionate rate acceleration in one direction or the other that spans a remarkable 6 orders of magnitude. The combination of high-resolution structural work, biochemical analyses, and computational modeling indicates that protein secondary interactions directly influence the relative stabilization/destabilization of different oxidation states of the active site metal cluster. This selective stabilization or destabilization of oxidation states can preferentially promote hydrogen oxidation or proton reduction and represents a simple yet elegant model by which a protein catalytic site can confer catalytic bias.
DOI: 10.1021/jacs.9b08756
PubMed: 31816235
Affiliations:
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<sourceDesc><biblStruct><analytic><title xml:lang="en">Tuning Catalytic Bias of Hydrogen Gas Producing Hydrogenases.</title>
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<author><name sortKey="Lyubimov, Artem Y" sort="Lyubimov, Artem Y" uniqKey="Lyubimov A" first="Artem Y" last="Lyubimov">Artem Y. Lyubimov</name>
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<author><name sortKey="Jones, Anne K" sort="Jones, Anne K" uniqKey="Jones A" first="Anne K" last="Jones">Anne K. Jones</name>
<affiliation wicri:level="1"><nlm:affiliation>School of Molecular Sciences , Arizona State University , Tempe , Arizona 85287 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>School of Molecular Sciences , Arizona State University , Tempe , Arizona 85287 </wicri:regionArea>
<wicri:noRegion>Arizona 85287 </wicri:noRegion>
</affiliation>
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<author><name sortKey="Soltis, S Michael" sort="Soltis, S Michael" uniqKey="Soltis S" first="S Michael" last="Soltis">S Michael Soltis</name>
<affiliation wicri:level="1"><nlm:affiliation>Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 </wicri:regionArea>
<wicri:noRegion>California 94025 </wicri:noRegion>
</affiliation>
</author>
<author><name sortKey="Adams, Michael W W" sort="Adams, Michael W W" uniqKey="Adams M" first="Michael W W" last="Adams">Michael W W. Adams</name>
<affiliation wicri:level="1"><nlm:affiliation>Department of Biochemistry and Molecular Biology , University of Georgia , Athens , Georgia 30602 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>Department of Biochemistry and Molecular Biology , University of Georgia , Athens , Georgia 30602 </wicri:regionArea>
<wicri:noRegion>Georgia 30602 </wicri:noRegion>
</affiliation>
</author>
<author><name sortKey="Raugei, Simone" sort="Raugei, Simone" uniqKey="Raugei S" first="Simone" last="Raugei">Simone Raugei</name>
<affiliation wicri:level="1"><nlm:affiliation>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 </wicri:regionArea>
<wicri:noRegion>Washington 99164 </wicri:noRegion>
</affiliation>
<affiliation wicri:level="1"><nlm:affiliation>Pacific Northwest National Laboratory , Richland , Washington 99352 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>Pacific Northwest National Laboratory , Richland , Washington 99352 </wicri:regionArea>
<wicri:noRegion>Washington 99352 </wicri:noRegion>
</affiliation>
</author>
<author><name sortKey="King, Paul W" sort="King, Paul W" uniqKey="King P" first="Paul W" last="King">Paul W. King</name>
<affiliation wicri:level="1"><nlm:affiliation>Biosciences Center , National Renewable Energy Laboratory , Golden , Colorado 80401 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>Biosciences Center , National Renewable Energy Laboratory , Golden , Colorado 80401 </wicri:regionArea>
<wicri:noRegion>Colorado 80401 </wicri:noRegion>
</affiliation>
</author>
<author><name sortKey="Peters, John W" sort="Peters, John W" uniqKey="Peters J" first="John W" last="Peters">John W. Peters</name>
<affiliation wicri:level="1"><nlm:affiliation>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 </wicri:regionArea>
<wicri:noRegion>Washington 99164 </wicri:noRegion>
</affiliation>
<affiliation wicri:level="1"><nlm:affiliation>Department of Chemistry and Biochemistry , Montana State University , Bozeman , Montana 59717 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>Department of Chemistry and Biochemistry , Montana State University , Bozeman , Montana 59717 </wicri:regionArea>
<wicri:noRegion>Montana 59717 </wicri:noRegion>
</affiliation>
<affiliation wicri:level="1"><nlm:affiliation>Pacific Northwest National Laboratory , Richland , Washington 99352 , United States.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<wicri:regionArea>Pacific Northwest National Laboratory , Richland , Washington 99352 </wicri:regionArea>
<wicri:noRegion>Washington 99352 </wicri:noRegion>
</affiliation>
</author>
</analytic>
<series><title level="j">Journal of the American Chemical Society</title>
<idno type="eISSN">1520-5126</idno>
<imprint><date when="2020" type="published">2020</date>
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<front><div type="abstract" xml:lang="en">Hydrogenases display a wide range of catalytic rates and biases in reversible hydrogen gas oxidation catalysis. The interactions of the iron-sulfur-containing catalytic site with the local protein environment are thought to contribute to differences in catalytic reactivity, but this has not been demonstrated. The microbe <i>Clostridium pasteurianum</i>
produces three [FeFe]-hydrogenases that differ in "catalytic bias" by exerting a disproportionate rate acceleration in one direction or the other that spans a remarkable 6 orders of magnitude. The combination of high-resolution structural work, biochemical analyses, and computational modeling indicates that protein secondary interactions directly influence the relative stabilization/destabilization of different oxidation states of the active site metal cluster. This selective stabilization or destabilization of oxidation states can preferentially promote hydrogen oxidation or proton reduction and represents a simple yet elegant model by which a protein catalytic site can confer catalytic bias.</div>
</front>
</TEI>
<pubmed><MedlineCitation Status="In-Process" Owner="NLM"><PMID Version="1">31816235</PMID>
<DateRevised><Year>2020</Year>
<Month>06</Month>
<Day>16</Day>
</DateRevised>
<Article PubModel="Print-Electronic"><Journal><ISSN IssnType="Electronic">1520-5126</ISSN>
<JournalIssue CitedMedium="Internet"><Volume>142</Volume>
<Issue>3</Issue>
<PubDate><Year>2020</Year>
<Month>01</Month>
<Day>22</Day>
</PubDate>
</JournalIssue>
<Title>Journal of the American Chemical Society</Title>
<ISOAbbreviation>J Am Chem Soc</ISOAbbreviation>
</Journal>
<ArticleTitle>Tuning Catalytic Bias of Hydrogen Gas Producing Hydrogenases.</ArticleTitle>
<Pagination><MedlinePgn>1227-1235</MedlinePgn>
</Pagination>
<ELocationID EIdType="doi" ValidYN="Y">10.1021/jacs.9b08756</ELocationID>
<Abstract><AbstractText>Hydrogenases display a wide range of catalytic rates and biases in reversible hydrogen gas oxidation catalysis. The interactions of the iron-sulfur-containing catalytic site with the local protein environment are thought to contribute to differences in catalytic reactivity, but this has not been demonstrated. The microbe <i>Clostridium pasteurianum</i>
produces three [FeFe]-hydrogenases that differ in "catalytic bias" by exerting a disproportionate rate acceleration in one direction or the other that spans a remarkable 6 orders of magnitude. The combination of high-resolution structural work, biochemical analyses, and computational modeling indicates that protein secondary interactions directly influence the relative stabilization/destabilization of different oxidation states of the active site metal cluster. This selective stabilization or destabilization of oxidation states can preferentially promote hydrogen oxidation or proton reduction and represents a simple yet elegant model by which a protein catalytic site can confer catalytic bias.</AbstractText>
</Abstract>
<AuthorList CompleteYN="Y"><Author ValidYN="Y"><LastName>Artz</LastName>
<ForeName>Jacob H</ForeName>
<Initials>JH</Initials>
<Identifier Source="ORCID">0000-0001-7661-2538</Identifier>
<AffiliationInfo><Affiliation>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 , United States.</Affiliation>
</AffiliationInfo>
<AffiliationInfo><Affiliation>Biosciences Center , National Renewable Energy Laboratory , Golden , Colorado 80401 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Zadvornyy</LastName>
<ForeName>Oleg A</ForeName>
<Initials>OA</Initials>
<Identifier Source="ORCID">0000-0002-5374-6856</Identifier>
<AffiliationInfo><Affiliation>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Mulder</LastName>
<ForeName>David W</ForeName>
<Initials>DW</Initials>
<AffiliationInfo><Affiliation>Biosciences Center , National Renewable Energy Laboratory , Golden , Colorado 80401 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Keable</LastName>
<ForeName>Stephen M</ForeName>
<Initials>SM</Initials>
<AffiliationInfo><Affiliation>Department of Chemistry and Biochemistry , Montana State University , Bozeman , Montana 59717 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Cohen</LastName>
<ForeName>Aina E</ForeName>
<Initials>AE</Initials>
<AffiliationInfo><Affiliation>Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Ratzloff</LastName>
<ForeName>Michael W</ForeName>
<Initials>MW</Initials>
<AffiliationInfo><Affiliation>Biosciences Center , National Renewable Energy Laboratory , Golden , Colorado 80401 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Williams</LastName>
<ForeName>S Garrett</ForeName>
<Initials>SG</Initials>
<Identifier Source="ORCID">0000-0003-4027-4770</Identifier>
<AffiliationInfo><Affiliation>School of Molecular Sciences , Arizona State University , Tempe , Arizona 85287 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Ginovska</LastName>
<ForeName>Bojana</ForeName>
<Initials>B</Initials>
<Identifier Source="ORCID">0000-0003-0165-8202</Identifier>
<AffiliationInfo><Affiliation>Pacific Northwest National Laboratory , Richland , Washington 99352 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Kumar</LastName>
<ForeName>Neeraj</ForeName>
<Initials>N</Initials>
<Identifier Source="ORCID">0000-0001-6713-2129</Identifier>
<AffiliationInfo><Affiliation>Pacific Northwest National Laboratory , Richland , Washington 99352 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Song</LastName>
<ForeName>Jinhu</ForeName>
<Initials>J</Initials>
<AffiliationInfo><Affiliation>Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>McPhillips</LastName>
<ForeName>Scott E</ForeName>
<Initials>SE</Initials>
<AffiliationInfo><Affiliation>Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Davidson</LastName>
<ForeName>Catherine M</ForeName>
<Initials>CM</Initials>
<Identifier Source="ORCID">0000-0002-2523-4319</Identifier>
<AffiliationInfo><Affiliation>Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Lyubimov</LastName>
<ForeName>Artem Y</ForeName>
<Initials>AY</Initials>
<AffiliationInfo><Affiliation>Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Pence</LastName>
<ForeName>Natasha</ForeName>
<Initials>N</Initials>
<Identifier Source="ORCID">0000-0002-6096-4894</Identifier>
<AffiliationInfo><Affiliation>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Schut</LastName>
<ForeName>Gerrit J</ForeName>
<Initials>GJ</Initials>
<AffiliationInfo><Affiliation>Department of Biochemistry and Molecular Biology , University of Georgia , Athens , Georgia 30602 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Jones</LastName>
<ForeName>Anne K</ForeName>
<Initials>AK</Initials>
<Identifier Source="ORCID">0000-0003-4025-4809</Identifier>
<AffiliationInfo><Affiliation>School of Molecular Sciences , Arizona State University , Tempe , Arizona 85287 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Soltis</LastName>
<ForeName>S Michael</ForeName>
<Initials>SM</Initials>
<AffiliationInfo><Affiliation>Stanford Synchrotron Radiation Lightsource , SLAC National Accelerator Laboratory , Menlo Park , California 94025 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Adams</LastName>
<ForeName>Michael W W</ForeName>
<Initials>MWW</Initials>
<Identifier Source="ORCID">0000-0002-9796-5014</Identifier>
<AffiliationInfo><Affiliation>Department of Biochemistry and Molecular Biology , University of Georgia , Athens , Georgia 30602 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Raugei</LastName>
<ForeName>Simone</ForeName>
<Initials>S</Initials>
<Identifier Source="ORCID">0000-0001-9118-8480</Identifier>
<AffiliationInfo><Affiliation>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 , United States.</Affiliation>
</AffiliationInfo>
<AffiliationInfo><Affiliation>Pacific Northwest National Laboratory , Richland , Washington 99352 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>King</LastName>
<ForeName>Paul W</ForeName>
<Initials>PW</Initials>
<Identifier Source="ORCID">0000-0001-5039-654X</Identifier>
<AffiliationInfo><Affiliation>Biosciences Center , National Renewable Energy Laboratory , Golden , Colorado 80401 , United States.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y"><LastName>Peters</LastName>
<ForeName>John W</ForeName>
<Initials>JW</Initials>
<Identifier Source="ORCID">0000-0001-9117-9568</Identifier>
<AffiliationInfo><Affiliation>Institute of Biological Chemistry , Washington State University , Pullman , Washington 99164 , United States.</Affiliation>
</AffiliationInfo>
<AffiliationInfo><Affiliation>Department of Chemistry and Biochemistry , Montana State University , Bozeman , Montana 59717 , United States.</Affiliation>
</AffiliationInfo>
<AffiliationInfo><Affiliation>Pacific Northwest National Laboratory , Richland , Washington 99352 , United States.</Affiliation>
</AffiliationInfo>
</Author>
</AuthorList>
<Language>eng</Language>
<GrantList CompleteYN="Y"><Grant><GrantID>P41 GM103393</GrantID>
<Acronym>GM</Acronym>
<Agency>NIGMS NIH HHS</Agency>
<Country>United States</Country>
</Grant>
</GrantList>
<PublicationTypeList><PublicationType UI="D016428">Journal Article</PublicationType>
<PublicationType UI="D013486">Research Support, U.S. Gov't, Non-P.H.S.</PublicationType>
<PublicationType UI="D052061">Research Support, N.I.H., Extramural</PublicationType>
</PublicationTypeList>
<ArticleDate DateType="Electronic"><Year>2020</Year>
<Month>01</Month>
<Day>10</Day>
</ArticleDate>
</Article>
<MedlineJournalInfo><Country>United States</Country>
<MedlineTA>J Am Chem Soc</MedlineTA>
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<ISSNLinking>0002-7863</ISSNLinking>
</MedlineJournalInfo>
<CitationSubset>IM</CitationSubset>
</MedlineCitation>
<PubmedData><History><PubMedPubDate PubStatus="pubmed"><Year>2019</Year>
<Month>12</Month>
<Day>10</Day>
<Hour>6</Hour>
<Minute>0</Minute>
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<PubMedPubDate PubStatus="medline"><Year>2019</Year>
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<affiliations><list><country><li>États-Unis</li>
</country>
</list>
<tree><country name="États-Unis"><noRegion><name sortKey="Artz, Jacob H" sort="Artz, Jacob H" uniqKey="Artz J" first="Jacob H" last="Artz">Jacob H. Artz</name>
</noRegion>
<name sortKey="Adams, Michael W W" sort="Adams, Michael W W" uniqKey="Adams M" first="Michael W W" last="Adams">Michael W W. Adams</name>
<name sortKey="Artz, Jacob H" sort="Artz, Jacob H" uniqKey="Artz J" first="Jacob H" last="Artz">Jacob H. Artz</name>
<name sortKey="Cohen, Aina E" sort="Cohen, Aina E" uniqKey="Cohen A" first="Aina E" last="Cohen">Aina E. Cohen</name>
<name sortKey="Davidson, Catherine M" sort="Davidson, Catherine M" uniqKey="Davidson C" first="Catherine M" last="Davidson">Catherine M. Davidson</name>
<name sortKey="Ginovska, Bojana" sort="Ginovska, Bojana" uniqKey="Ginovska B" first="Bojana" last="Ginovska">Bojana Ginovska</name>
<name sortKey="Jones, Anne K" sort="Jones, Anne K" uniqKey="Jones A" first="Anne K" last="Jones">Anne K. Jones</name>
<name sortKey="Keable, Stephen M" sort="Keable, Stephen M" uniqKey="Keable S" first="Stephen M" last="Keable">Stephen M. Keable</name>
<name sortKey="King, Paul W" sort="King, Paul W" uniqKey="King P" first="Paul W" last="King">Paul W. King</name>
<name sortKey="Kumar, Neeraj" sort="Kumar, Neeraj" uniqKey="Kumar N" first="Neeraj" last="Kumar">Neeraj Kumar</name>
<name sortKey="Lyubimov, Artem Y" sort="Lyubimov, Artem Y" uniqKey="Lyubimov A" first="Artem Y" last="Lyubimov">Artem Y. Lyubimov</name>
<name sortKey="Mcphillips, Scott E" sort="Mcphillips, Scott E" uniqKey="Mcphillips S" first="Scott E" last="Mcphillips">Scott E. Mcphillips</name>
<name sortKey="Mulder, David W" sort="Mulder, David W" uniqKey="Mulder D" first="David W" last="Mulder">David W. Mulder</name>
<name sortKey="Pence, Natasha" sort="Pence, Natasha" uniqKey="Pence N" first="Natasha" last="Pence">Natasha Pence</name>
<name sortKey="Peters, John W" sort="Peters, John W" uniqKey="Peters J" first="John W" last="Peters">John W. Peters</name>
<name sortKey="Peters, John W" sort="Peters, John W" uniqKey="Peters J" first="John W" last="Peters">John W. Peters</name>
<name sortKey="Peters, John W" sort="Peters, John W" uniqKey="Peters J" first="John W" last="Peters">John W. Peters</name>
<name sortKey="Ratzloff, Michael W" sort="Ratzloff, Michael W" uniqKey="Ratzloff M" first="Michael W" last="Ratzloff">Michael W. Ratzloff</name>
<name sortKey="Raugei, Simone" sort="Raugei, Simone" uniqKey="Raugei S" first="Simone" last="Raugei">Simone Raugei</name>
<name sortKey="Raugei, Simone" sort="Raugei, Simone" uniqKey="Raugei S" first="Simone" last="Raugei">Simone Raugei</name>
<name sortKey="Schut, Gerrit J" sort="Schut, Gerrit J" uniqKey="Schut G" first="Gerrit J" last="Schut">Gerrit J. Schut</name>
<name sortKey="Soltis, S Michael" sort="Soltis, S Michael" uniqKey="Soltis S" first="S Michael" last="Soltis">S Michael Soltis</name>
<name sortKey="Song, Jinhu" sort="Song, Jinhu" uniqKey="Song J" first="Jinhu" last="Song">Jinhu Song</name>
<name sortKey="Williams, S Garrett" sort="Williams, S Garrett" uniqKey="Williams S" first="S Garrett" last="Williams">S Garrett Williams</name>
<name sortKey="Zadvornyy, Oleg A" sort="Zadvornyy, Oleg A" uniqKey="Zadvornyy O" first="Oleg A" last="Zadvornyy">Oleg A. Zadvornyy</name>
</country>
</tree>
</affiliations>
</record>
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