Low valent and hydride complexes of NHC coordinated gallium and indium.
Identifieur interne : 000C28 ( Main/Exploration ); précédent : 000C27; suivant : 000C29Low valent and hydride complexes of NHC coordinated gallium and indium.
Auteurs : RBID : pubmed:22080333Abstract
The reactions of the N-heterocyclic carbene 1,3-dimesitylimidazol-2-ylidene (IMes) with Ga[GaCl(4)], "GaI", InCl(2) and GaBr(3) have been examined. All reactions using a low valent gallium or indium starting material led to species of the form [{MX(2)(IMes)}(2)], where M = Ga, X = Cl (1), I (2); M = In, X = Cl (3), with disproportionation and loss of gallium metal in the case of 2. Reaction of IMes with gallium tribromide yields the air and moisture stable complex [GaBr(3)(IMes)] (4), which has been used as a precursor to the mixed bromohydrides [GaBrH(2)(IMes)] (5) and [GaBr(2)H(IMes)] (6) by (i) ligand redistribution with [GaH(3)(IMes)], (ii) hydride-bromide exchange with triethylsilane, and (iii) alkylation with (n)butyllithium followed by β-hydride elimination (6 only). Attempts to prepare 1, or monovalent analogues such as [{GaCl(IMes)}(n)], by thermally induced reductive elimination of dihydrogen from the chlorohydride congeners of 5 and 6 resulted in isolation of the known compounds [IMesCl][Cl] (IMesCl = 1,3-dimesityl-2-chloroimidazolium), and/or 1,3-dimesityl-2-dihydroimidazole, and gallium metal. Preliminary photochemical NMR spectroscopy and catalytic studies of 5 and 6 aimed at reductive dehydrogenation under milder conditions are reported. Compounds 1 and 4 have been characterised by single crystal X-ray structure determination.
DOI: 10.1039/c1dt11202c
PubMed: 22080333
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<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en">Low valent and hydride complexes of NHC coordinated gallium and indium.</title><author><name sortKey="Ball, Graham E" uniqKey="Ball G">Graham E Ball</name><affiliation wicri:level="1"><nlm:affiliation>School of Chemistry, University of New South Wales, Sydney, NSW 2052, Australia.</nlm:affiliation><country xml:lang="fr">Australie</country><wicri:regionArea>School of Chemistry, University of New South Wales, Sydney, NSW 2052</wicri:regionArea></affiliation></author><author><name sortKey="Cole, Marcus L" uniqKey="Cole M">Marcus L Cole</name></author><author><name sortKey="Mckay, Alasdair I" uniqKey="Mckay A">Alasdair I McKay</name></author></titleStmt><publicationStmt><date when="2012">2012</date><idno type="doi">10.1039/c1dt11202c</idno><idno type="RBID">pubmed:22080333</idno><idno type="pmid">22080333</idno><idno type="wicri:Area/Main/Corpus">001071</idno><idno type="wicri:Area/Main/Curation">001071</idno><idno type="wicri:Area/Main/Exploration">000C28</idno></publicationStmt></fileDesc><profileDesc><textClass></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">The reactions of the N-heterocyclic carbene 1,3-dimesitylimidazol-2-ylidene (IMes) with Ga[GaCl(4)], "GaI", InCl(2) and GaBr(3) have been examined. All reactions using a low valent gallium or indium starting material led to species of the form [{MX(2)(IMes)}(2)], where M = Ga, X = Cl (1), I (2); M = In, X = Cl (3), with disproportionation and loss of gallium metal in the case of 2. Reaction of IMes with gallium tribromide yields the air and moisture stable complex [GaBr(3)(IMes)] (4), which has been used as a precursor to the mixed bromohydrides [GaBrH(2)(IMes)] (5) and [GaBr(2)H(IMes)] (6) by (i) ligand redistribution with [GaH(3)(IMes)], (ii) hydride-bromide exchange with triethylsilane, and (iii) alkylation with (n)butyllithium followed by β-hydride elimination (6 only). Attempts to prepare 1, or monovalent analogues such as [{GaCl(IMes)}(n)], by thermally induced reductive elimination of dihydrogen from the chlorohydride congeners of 5 and 6 resulted in isolation of the known compounds [IMesCl][Cl] (IMesCl = 1,3-dimesityl-2-chloroimidazolium), and/or 1,3-dimesityl-2-dihydroimidazole, and gallium metal. Preliminary photochemical NMR spectroscopy and catalytic studies of 5 and 6 aimed at reductive dehydrogenation under milder conditions are reported. Compounds 1 and 4 have been characterised by single crystal X-ray structure determination.</div></front></TEI><pubmed><MedlineCitation Owner="NLM" Status="PubMed-not-MEDLINE"><PMID Version="1">22080333</PMID><DateCreated><Year>2011</Year><Month>12</Month><Day>23</Day></DateCreated><DateCompleted><Year>2012</Year><Month>04</Month><Day>16</Day></DateCompleted><Article PubModel="Print-Electronic"><Journal><ISSN IssnType="Electronic">1477-9234</ISSN><JournalIssue CitedMedium="Internet"><Volume>41</Volume><Issue>3</Issue><PubDate><Year>2012</Year><Month>Jan</Month><Day>21</Day></PubDate></JournalIssue><Title>Dalton transactions (Cambridge, England : 2003)</Title><ISOAbbreviation>Dalton Trans</ISOAbbreviation></Journal><ArticleTitle>Low valent and hydride complexes of NHC coordinated gallium and indium.</ArticleTitle><Pagination><MedlinePgn>946-52</MedlinePgn></Pagination><ELocationID EIdType="doi" ValidYN="Y">10.1039/c1dt11202c</ELocationID><Abstract><AbstractText>The reactions of the N-heterocyclic carbene 1,3-dimesitylimidazol-2-ylidene (IMes) with Ga[GaCl(4)], "GaI", InCl(2) and GaBr(3) have been examined. All reactions using a low valent gallium or indium starting material led to species of the form [{MX(2)(IMes)}(2)], where M = Ga, X = Cl (1), I (2); M = In, X = Cl (3), with disproportionation and loss of gallium metal in the case of 2. Reaction of IMes with gallium tribromide yields the air and moisture stable complex [GaBr(3)(IMes)] (4), which has been used as a precursor to the mixed bromohydrides [GaBrH(2)(IMes)] (5) and [GaBr(2)H(IMes)] (6) by (i) ligand redistribution with [GaH(3)(IMes)], (ii) hydride-bromide exchange with triethylsilane, and (iii) alkylation with (n)butyllithium followed by β-hydride elimination (6 only). Attempts to prepare 1, or monovalent analogues such as [{GaCl(IMes)}(n)], by thermally induced reductive elimination of dihydrogen from the chlorohydride congeners of 5 and 6 resulted in isolation of the known compounds [IMesCl][Cl] (IMesCl = 1,3-dimesityl-2-chloroimidazolium), and/or 1,3-dimesityl-2-dihydroimidazole, and gallium metal. Preliminary photochemical NMR spectroscopy and catalytic studies of 5 and 6 aimed at reductive dehydrogenation under milder conditions are reported. Compounds 1 and 4 have been characterised by single crystal X-ray structure determination.</AbstractText></Abstract><AuthorList CompleteYN="Y"><Author ValidYN="Y"><LastName>Ball</LastName><ForeName>Graham E</ForeName><Initials>GE</Initials><Affiliation>School of Chemistry, University of New South Wales, Sydney, NSW 2052, Australia.</Affiliation></Author><Author ValidYN="Y"><LastName>Cole</LastName><ForeName>Marcus L</ForeName><Initials>ML</Initials></Author><Author ValidYN="Y"><LastName>McKay</LastName><ForeName>Alasdair I</ForeName><Initials>AI</Initials></Author></AuthorList><Language>eng</Language><PublicationTypeList><PublicationType>Journal Article</PublicationType></PublicationTypeList><ArticleDate DateType="Electronic"><Year>2011</Year><Month>11</Month><Day>14</Day></ArticleDate></Article><MedlineJournalInfo><Country>England</Country><MedlineTA>Dalton Trans</MedlineTA><NlmUniqueID>101176026</NlmUniqueID><ISSNLinking>1477-9226</ISSNLinking></MedlineJournalInfo></MedlineCitation><PubmedData><History><PubMedPubDate PubStatus="aheadofprint"><Year>2011</Year><Month>11</Month><Day>14</Day></PubMedPubDate><PubMedPubDate PubStatus="epublish"><Year>2011</Year><Month>12</Month><Day>22</Day></PubMedPubDate><PubMedPubDate PubStatus="entrez"><Year>2011</Year><Month>11</Month><Day>15</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="pubmed"><Year>2011</Year><Month>11</Month><Day>15</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="medline"><Year>2011</Year><Month>11</Month><Day>15</Day><Hour>6</Hour><Minute>1</Minute></PubMedPubDate></History><PublicationStatus>ppublish</PublicationStatus><ArticleIdList><ArticleId IdType="doi">10.1039/c1dt11202c</ArticleId><ArticleId IdType="pubmed">22080333</ArticleId></ArticleIdList></PubmedData></pubmed></record>Pour manipuler ce document sous Unix (Dilib)
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