A Zeolite‐Supported Molecular Ruthenium Complex with η6‐C6H6 Ligands: Chemistry Elucidated by Using Spectroscopy and Density Functional Theory
Identifieur interne : 002E76 ( Istex/Corpus ); précédent : 002E75; suivant : 002E77A Zeolite‐Supported Molecular Ruthenium Complex with η6‐C6H6 Ligands: Chemistry Elucidated by Using Spectroscopy and Density Functional Theory
Auteurs : Isao Ogino ; Mingyang Chen ; Jason Dyer ; Philip Kletnieks ; James Haw ; David Dixon ; Bruce GatesSource :
- Chemistry – A European Journal [ 0947-6539 ] ; 2010-07-05.
English descriptors
Abstract
An essentially molecular ruthenium–benzene complex anchored at the aluminum sites of dealuminated zeolite Y was formed by treating a zeolite‐supported mononuclear ruthenium complex, [Ru(acac)(η2‐C2H4)2]+ (acac=acetylacetonate, C5H7O2−), with 13C6H6 at 413 K. IR, 13C NMR, and extended X‐ray absorption fine structure (EXAFS) spectra of the sample reveal the replacement of two ethene ligands and one acac ligand in the original complex with one 13C6H6 ligand and the formation of adsorbed protonated acac (Hacac). The EXAFS results indicate that the supported [Ru(η6‐C6H6)]2+ incorporates an oxygen atom of the support to balance the charge, being bonded to the zeolite through three RuO bonds. The supported ruthenium–benzene complex is analogous to complexes with polyoxometalate ligands, consistent with the high structural uniformity of the zeolite‐supported species, which led to good agreement between the spectra and calculations at the density functional theory level. The calculations show that the interaction of the zeolite with the Hacac formed on treatment of the original complex with 13C6H6 drives the reaction to form the ruthenium–benzene complex.
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DOI: 10.1002/chem.201000303
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(USA), Fax: (+1) 205‐348‐4704</mods:affiliation></affiliation><affiliation><mods:affiliation>E-mail: dadixon@bama.ua.edu</mods:affiliation></affiliation></author><author><name sortKey="Gates, Bruce" sort="Gates, Bruce" uniqKey="Gates B" first="Bruce" last="Gates">Bruce Gates</name><affiliation><mods:affiliation>Department of Chemical Engineering and Materials Science, University of California, Davis, Davis, CA, 95616 (USA), Fax: (+1) 530‐752‐1031</mods:affiliation></affiliation><affiliation><mods:affiliation>E-mail: bcgates@ucdavis.edu</mods:affiliation></affiliation></author></analytic><monogr></monogr><series><title level="j">Chemistry – A European Journal</title><title level="j" type="abbrev">Chem. 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IR, 13C NMR, and extended X‐ray absorption fine structure (EXAFS) spectra of the sample reveal the replacement of two ethene ligands and one acac ligand in the original complex with one 13C6H6 ligand and the formation of adsorbed protonated acac (Hacac). The EXAFS results indicate that the supported [Ru(η6‐C6H6)]2+ incorporates an oxygen atom of the support to balance the charge, being bonded to the zeolite through three RuO bonds. The supported ruthenium–benzene complex is analogous to complexes with polyoxometalate ligands, consistent with the high structural uniformity of the zeolite‐supported species, which led to good agreement between the spectra and calculations at the density functional theory level. The calculations show that the interaction of the zeolite with the Hacac formed on treatment of the original complex with 13C6H6 drives the reaction to form the ruthenium–benzene complex.</div></front></TEI><istex><corpusName>wiley</corpusName><author><json:item><name>Isao Ogino</name><affiliations><json:string>Department of Chemical Engineering and Materials Science, University of California, Davis, Davis, CA, 95616 (USA), Fax: (+1) 530‐752‐1031</json:string></affiliations></json:item><json:item><name>Mingyang Chen</name><affiliations><json:string>Department of Chemistry, University of Alabama, Tuscaloosa, AL, 35487 (USA), Fax: (+1) 205‐348‐4704</json:string></affiliations></json:item><json:item><name>Jason Dyer</name><affiliations><json:string>Department of Chemistry, University of Alabama, Tuscaloosa, AL, 35487 (USA), Fax: (+1) 205‐348‐4704</json:string></affiliations></json:item><json:item><name>Philip W. 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Eur. J.</title><idno type="pISSN">0947-6539</idno><idno type="eISSN">1521-3765</idno><idno type="DOI">10.1002/(ISSN)1521-3765</idno><imprint><publisher>WILEY‐VCH Verlag</publisher><pubPlace>Weinheim</pubPlace><date type="published" when="2010-07-05"></date><biblScope unit="volume">16</biblScope><biblScope unit="issue">25</biblScope><biblScope unit="page" from="7427">7427</biblScope><biblScope unit="page" to="7436">7436</biblScope></imprint></monogr><idno type="istex">72FEB7BFF30A01321E7CCB623A070704BBEF8D76</idno><idno type="DOI">10.1002/chem.201000303</idno><idno type="ArticleID">CHEM201000303</idno></biblStruct></sourceDesc></fileDesc><profileDesc><creation><date>2010</date></creation><langUsage><language ident="en">en</language></langUsage><abstract xml:lang="en"><p>An essentially molecular ruthenium–benzene complex anchored at the aluminum sites of dealuminated zeolite Y was formed by treating a zeolite‐supported mononuclear ruthenium complex, [Ru(acac)(η2‐C2H4)2]+ (acac=acetylacetonate, C5H7O2−), with 13C6H6 at 413 K. IR, 13C NMR, and extended X‐ray absorption fine structure (EXAFS) spectra of the sample reveal the replacement of two ethene ligands and one acac ligand in the original complex with one 13C6H6 ligand and the formation of adsorbed protonated acac (Hacac). The EXAFS results indicate that the supported [Ru(η6‐C6H6)]2+ incorporates an oxygen atom of the support to balance the charge, being bonded to the zeolite through three RuO bonds. The supported ruthenium–benzene complex is analogous to complexes with polyoxometalate ligands, consistent with the high structural uniformity of the zeolite‐supported species, which led to good agreement between the spectra and calculations at the density functional theory level. The calculations show that the interaction of the zeolite with the Hacac formed on treatment of the original complex with 13C6H6 drives the reaction to form the ruthenium–benzene complex.</p></abstract><abstract xml:lang="en" style="graphical"><p>Look below the surface: A highly uniform mononuclear ruthenium–benzene complex supported on zeolite (see figure) has been synthesized and characterized by using IR, 13C NMR, and EXAFS spectroscopies complemented by density functional theory calculations.</p></abstract><textClass xml:lang="en"><keywords scheme="keyword"><list><head>keywords</head><item><term>density functional calculations</term></item><item><term>EXAFS spectroscopy</term></item><item><term>NMR spectroscopy</term></item><item><term>ruthenium</term></item><item><term>zeolites</term></item></list></keywords></textClass><textClass><keywords scheme="Journal Subject"><list><head>article-category</head><item><term>Full Paper</term></item></list></keywords></textClass></profileDesc><revisionDesc><change when="2010-02-04">Received</change><change when="2010-07-05">Published</change></revisionDesc></teiHeader></istex:fulltextTEI><json:item><original>false</original><mimetype>text/plain</mimetype><extension>txt</extension><uri>https://api.istex.fr/document/72FEB7BFF30A01321E7CCB623A070704BBEF8D76/fulltext/txt</uri></json:item></fulltext><metadata><istex:metadataXml wicri:clean="Wiley, elements deleted: body"><istex:xmlDeclaration>version="1.0" encoding="UTF-8" standalone="yes"</istex:xmlDeclaration><istex:document><component version="2.0" type="serialArticle" xml:lang="en"><header><publicationMeta level="product"><publisherInfo><publisherName>WILEY‐VCH Verlag</publisherName><publisherLoc>Weinheim</publisherLoc></publisherInfo><doi registered="yes">10.1002/(ISSN)1521-3765</doi><issn type="print">0947-6539</issn><issn type="electronic">1521-3765</issn><idGroup><id type="product" value="CHEM"></id></idGroup><titleGroup><title type="main" xml:lang="en" sort="CHEMISTRY - A EUROPEAN JOURNAL">Chemistry – A European Journal</title><title type="short">Chem. 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KGaA, Weinheim</copyright><eventGroup><event type="manuscriptReceived" date="2010-02-04"></event><event type="firstOnline" date="2010-06-10"></event><event type="publishedOnlineFinalForm" date="2010-06-25"></event><event type="publishedOnlineAcceptedOrEarlyUnpaginated" date="2010-06-10"></event><event type="xmlConverted" agent="Converter:JWSART34_TO_WML3G version:2.4.8 mode:FullText mathml2tex" date="2011-03-29"></event><event type="xmlConverted" agent="Converter:WILEY_ML3G_TO_WILEY_ML3GV2 version:3.8.8" date="2014-01-09"></event><event type="xmlConverted" agent="Converter:WML3G_To_WML3G version:4.1.7 mode:FullText,remove_FC" date="2014-10-15"></event></eventGroup><numberingGroup><numbering type="pageFirst">7427</numbering><numbering type="pageLast">7436</numbering></numberingGroup><objectNameGroup><objectName elementName="figure">Scheme</objectName></objectNameGroup><linkGroup><link type="toTypesetVersion" href="file:CHEM.CHEM201000303.pdf"></link></linkGroup></publicationMeta><contentMeta><countGroup><count type="figureTotal" number="9"></count><count type="tableTotal" number="2"></count><count type="referenceTotal" number="66"></count></countGroup><titleGroup><title type="main" xml:lang="en">A Zeolite‐Supported Molecular Ruthenium Complex with η<sup>6</sup>‐C<sub>6</sub>H<sub>6</sub> Ligands: Chemistry Elucidated by Using Spectroscopy and Density Functional Theory</title></titleGroup><creators><creator xml:id="au1" creatorRole="author" affiliationRef="#aa"><personName><givenNames>Isao</givenNames><familyName>Ogino</familyName></personName></creator><creator xml:id="au2" creatorRole="author" affiliationRef="#ab"><personName><givenNames>Mingyang</givenNames><familyName>Chen</familyName></personName></creator><creator xml:id="au3" creatorRole="author" affiliationRef="#ab"><personName><givenNames>Jason</givenNames><familyName>Dyer</familyName></personName></creator><creator xml:id="au4" creatorRole="author" affiliationRef="#ac"><personName><givenNames>Philip W.</givenNames><familyName>Kletnieks</familyName></personName></creator><creator xml:id="au5" creatorRole="author" affiliationRef="#ac"><personName><givenNames>James F.</givenNames><familyName>Haw</familyName><degrees>Prof.</degrees></personName></creator><creator xml:id="au6" creatorRole="author" affiliationRef="#ab"><personName><givenNames>David A.</givenNames><familyName>Dixon</familyName><degrees>Prof.</degrees></personName><contactDetails><email>dadixon@bama.ua.edu</email></contactDetails></creator><creator xml:id="au7" creatorRole="author" affiliationRef="#aa"><personName><givenNames>Bruce C.</givenNames><familyName>Gates</familyName><degrees>Prof.</degrees></personName><contactDetails><email>bcgates@ucdavis.edu</email></contactDetails></creator></creators><affiliationGroup><affiliation xml:id="aa" countryCode="US" type="organization"><unparsedAffiliation>Department of Chemical Engineering and Materials Science, University of California, Davis, Davis, CA, 95616 (USA), Fax: (+1) 530‐752‐1031</unparsedAffiliation></affiliation><affiliation xml:id="ab" countryCode="US" type="organization"><unparsedAffiliation>Department of Chemistry, University of Alabama, Tuscaloosa, AL, 35487 (USA), Fax: (+1) 205‐348‐4704</unparsedAffiliation></affiliation><affiliation xml:id="ac" countryCode="US" type="organization"><unparsedAffiliation>Department of Chemistry, University of Southern California, Los Angeles, CA 90089 (USA)</unparsedAffiliation></affiliation></affiliationGroup><keywordGroup xml:lang="en" type="author"><keyword xml:id="kwd1">density functional calculations</keyword><keyword xml:id="kwd2">EXAFS spectroscopy</keyword><keyword xml:id="kwd3">NMR spectroscopy</keyword><keyword xml:id="kwd4">ruthenium</keyword><keyword xml:id="kwd5">zeolites</keyword></keywordGroup><fundingInfo><fundingAgency>Department of Energy</fundingAgency></fundingInfo><fundingInfo><fundingAgency>Office of Science, Basic Energy Sciences</fundingAgency><fundingNumber>DE‐FG02‐04ER15513</fundingNumber><fundingNumber>DE‐FG02‐03ER15481</fundingNumber><fundingNumber>DE‐FG02‐04ER15598</fundingNumber></fundingInfo><supportingInformation><p>Detailed facts of importance to specialist readers are published as ”Supporting Information”. Such documents are peer‐reviewed, but not copy‐edited or typeset. They are made available as submitted by the authors. </p><supportingInfoItem><mediaResource alt="supporting information" href="urn-x:wiley:09476539:media:chem201000303:chem_201000303_sm_miscellaneous_information"></mediaResource><caption>miscellaneous_information</caption></supportingInfoItem></supportingInformation><abstractGroup><abstract type="main" xml:lang="en"><title type="main">Abstract</title><p>An essentially molecular ruthenium–benzene complex anchored at the aluminum sites of dealuminated zeolite Y was formed by treating a zeolite‐supported mononuclear ruthenium complex, [Ru(acac)(η<sup>2</sup>‐C<sub>2</sub>H<sub>4</sub>)<sub>2</sub>]<sup>+</sup> (acac=acetylacetonate, C<sub>5</sub>H<sub>7</sub>O<sub>2</sub><sup>−</sup>), with <sup>13</sup>C<sub>6</sub>H<sub>6</sub> at 413 K. IR, <sup>13</sup>C NMR, and extended X‐ray absorption fine structure (EXAFS) spectra of the sample reveal the replacement of two ethene ligands and one acac ligand in the original complex with one <sup>13</sup>C<sub>6</sub>H<sub>6</sub> ligand and the formation of adsorbed protonated acac (Hacac). The EXAFS results indicate that the supported [Ru(η<sup>6</sup>‐C<sub>6</sub>H<sub>6</sub>)]<sup>2+</sup> incorporates an oxygen atom of the support to balance the charge, being bonded to the zeolite through three RuO bonds. The supported ruthenium–benzene complex is analogous to complexes with polyoxometalate ligands, consistent with the high structural uniformity of the zeolite‐supported species, which led to good agreement between the spectra and calculations at the density functional theory level. The calculations show that the interaction of the zeolite with the Hacac formed on treatment of the original complex with <sup>13</sup>C<sub>6</sub>H<sub>6</sub> drives the reaction to form the ruthenium–benzene complex.</p></abstract><abstract type="graphical" xml:lang="en"><p><b>Look below the surface</b>: A highly uniform mononuclear ruthenium–benzene complex supported on zeolite (see figure) has been synthesized and characterized by using IR, <sup>13</sup>C NMR, and EXAFS spectroscopies complemented by density functional theory calculations.<blockFixed type="graphic"><mediaResourceGroup><mediaResource alt="image" eRights="yes" copyright="WILEY-VCH" href="urn:x-wiley:09476539:media:CHEM201000303:content"></mediaResource><mediaResource alt="thumbnail image" rendition="webLoRes" mimeType="image/gif" href=""></mediaResource><mediaResource alt="original image" rendition="webOriginal" mimeType="image/gif" href=""></mediaResource><mediaResource alt="magnified image" rendition="webHiRes" mimeType="image/gif" href=""></mediaResource></mediaResourceGroup></blockFixed></p></abstract></abstractGroup></contentMeta></header></component></istex:document></istex:metadataXml><mods version="3.6"><titleInfo lang="en"><title>A Zeolite‐Supported Molecular Ruthenium Complex with η6‐C6H6 Ligands: Chemistry Elucidated by Using Spectroscopy and Density Functional Theory</title></titleInfo><titleInfo type="alternative" contentType="CDATA" lang="en"><title>A Zeolite‐Supported Molecular Ruthenium Complex with η</title></titleInfo><name type="personal"><namePart type="given">Isao</namePart><namePart type="family">Ogino</namePart><affiliation>Department of Chemical Engineering and Materials Science, University of California, Davis, Davis, CA, 95616 (USA), Fax: (+1) 530‐752‐1031</affiliation><role><roleTerm type="text">author</roleTerm></role></name><name type="personal"><namePart type="given">Mingyang</namePart><namePart type="family">Chen</namePart><affiliation>Department of Chemistry, University of Alabama, Tuscaloosa, AL, 35487 (USA), Fax: (+1) 205‐348‐4704</affiliation><role><roleTerm type="text">author</roleTerm></role></name><name type="personal"><namePart type="given">Jason</namePart><namePart type="family">Dyer</namePart><affiliation>Department of Chemistry, University of Alabama, Tuscaloosa, AL, 35487 (USA), Fax: (+1) 205‐348‐4704</affiliation><role><roleTerm type="text">author</roleTerm></role></name><name type="personal"><namePart type="given">Philip W.</namePart><namePart type="family">Kletnieks</namePart><affiliation>Department of Chemistry, University of Southern California, Los Angeles, CA 90089 (USA)</affiliation><role><roleTerm type="text">author</roleTerm></role></name><name type="personal"><namePart type="given">James F.</namePart><namePart type="family">Haw</namePart><namePart type="termsOfAddress">Prof.</namePart><affiliation>Department of Chemistry, University of Southern California, Los Angeles, CA 90089 (USA)</affiliation><role><roleTerm type="text">author</roleTerm></role></name><name type="personal"><namePart type="given">David A.</namePart><namePart type="family">Dixon</namePart><namePart type="termsOfAddress">Prof.</namePart><affiliation>Department of Chemistry, University of Alabama, Tuscaloosa, AL, 35487 (USA), Fax: (+1) 205‐348‐4704</affiliation><affiliation>E-mail: dadixon@bama.ua.edu</affiliation><role><roleTerm type="text">author</roleTerm></role></name><name type="personal"><namePart type="given">Bruce C.</namePart><namePart type="family">Gates</namePart><namePart type="termsOfAddress">Prof.</namePart><affiliation>Department of Chemical Engineering and Materials Science, University of California, Davis, Davis, CA, 95616 (USA), Fax: (+1) 530‐752‐1031</affiliation><affiliation>E-mail: bcgates@ucdavis.edu</affiliation><role><roleTerm type="text">author</roleTerm></role></name><typeOfResource>text</typeOfResource><genre type="article" displayLabel="article"></genre><originInfo><publisher>WILEY‐VCH Verlag</publisher><place><placeTerm type="text">Weinheim</placeTerm></place><dateIssued encoding="w3cdtf">2010-07-05</dateIssued><dateCaptured encoding="w3cdtf">2010-02-04</dateCaptured><copyrightDate encoding="w3cdtf">2010</copyrightDate></originInfo><language><languageTerm type="code" authority="rfc3066">en</languageTerm><languageTerm type="code" authority="iso639-2b">eng</languageTerm></language><physicalDescription><internetMediaType>text/html</internetMediaType><extent unit="figures">9</extent><extent unit="tables">2</extent><extent unit="references">66</extent></physicalDescription><abstract lang="en">An essentially molecular ruthenium–benzene complex anchored at the aluminum sites of dealuminated zeolite Y was formed by treating a zeolite‐supported mononuclear ruthenium complex, [Ru(acac)(η2‐C2H4)2]+ (acac=acetylacetonate, C5H7O2−), with 13C6H6 at 413 K. IR, 13C NMR, and extended X‐ray absorption fine structure (EXAFS) spectra of the sample reveal the replacement of two ethene ligands and one acac ligand in the original complex with one 13C6H6 ligand and the formation of adsorbed protonated acac (Hacac). The EXAFS results indicate that the supported [Ru(η6‐C6H6)]2+ incorporates an oxygen atom of the support to balance the charge, being bonded to the zeolite through three RuO bonds. The supported ruthenium–benzene complex is analogous to complexes with polyoxometalate ligands, consistent with the high structural uniformity of the zeolite‐supported species, which led to good agreement between the spectra and calculations at the density functional theory level. The calculations show that the interaction of the zeolite with the Hacac formed on treatment of the original complex with 13C6H6 drives the reaction to form the ruthenium–benzene complex.</abstract><abstract type="graphical" lang="en">Look below the surface: A highly uniform mononuclear ruthenium–benzene complex supported on zeolite (see figure) has been synthesized and characterized by using IR, 13C NMR, and EXAFS spectroscopies complemented by density functional theory calculations.</abstract><note type="funding">Department of Energy</note><note type="funding">Office of Science, Basic Energy Sciences - No. DE‐FG02‐04ER15513; No. DE‐FG02‐03ER15481; No. DE‐FG02‐04ER15598; </note><subject lang="en"><genre>keywords</genre><topic>density functional calculations</topic><topic>EXAFS spectroscopy</topic><topic>NMR spectroscopy</topic><topic>ruthenium</topic><topic>zeolites</topic></subject><relatedItem type="host"><titleInfo><title>Chemistry – A European Journal</title></titleInfo><titleInfo type="abbreviated"><title>Chem. Eur. J.</title></titleInfo><genre type="journal">journal</genre><note type="content"> Detailed facts of importance to specialist readers are published as ”Supporting Information”. Such documents are peer‐reviewed, but not copy‐edited or typeset. They are made available as submitted by the authors.Supporting Info Item: miscellaneous_information - </note><subject><genre>article-category</genre><topic>Full Paper</topic></subject><identifier type="ISSN">0947-6539</identifier><identifier type="eISSN">1521-3765</identifier><identifier type="DOI">10.1002/(ISSN)1521-3765</identifier><identifier type="PublisherID">CHEM</identifier><part><date>2010</date><detail type="volume"><caption>vol.</caption><number>16</number></detail><detail type="issue"><caption>no.</caption><number>25</number></detail><extent unit="pages"><start>7427</start><end>7436</end><total>10</total></extent></part></relatedItem><identifier type="istex">72FEB7BFF30A01321E7CCB623A070704BBEF8D76</identifier><identifier type="DOI">10.1002/chem.201000303</identifier><identifier type="ArticleID">CHEM201000303</identifier><accessCondition type="use and reproduction" contentType="copyright">Copyright © 2010 WILEY‐VCH Verlag GmbH & Co. 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