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http://hdl.handle.net/10261/154801
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dc.contributor.author | Betoré, M. Pilar | - |
dc.contributor.author | García-Orduña, Pilar | - |
dc.contributor.author | Lahoz, Fernando J. | - |
dc.contributor.author | Casado, Miguel A. | - |
dc.contributor.author | Polo, Víctor | - |
dc.contributor.author | Oro, Luis A. | - |
dc.date.accessioned | 2017-09-06T09:31:28Z | - |
dc.date.available | 2017-09-06T09:31:28Z | - |
dc.date.issued | 2016 | - |
dc.identifier | doi: 10.1002/ejic.201600925 | - |
dc.identifier | e-issn: 1099-0682 | - |
dc.identifier | issn: 1434-1948 | - |
dc.identifier.citation | European Journal of Inorganic Chemistry 2016(34): 5347-5355 (2016) | - |
dc.identifier.uri | http://hdl.handle.net/10261/154801 | - |
dc.description.abstract | Treatment of acetone solutions of the known chlorido-bridged complexes [{M(µ-Cl)(cod)}2] (M = Ir, Rh; cod = 1,5-cyclooctadiene) under an ammonia atmosphere afforded the cationic complexes {M(cod)[κN,κN-NH2–C(CH3)2–CH2–C(CH3)=NH]}Cl [M = Ir (3), Rh (4)]. The molecular structures of 3 and 4 showed the formation of six-membered metallacycles due to the presence of a 4-imino-2-methylpentan-2-amine-κN,κN-chelated ligand. Alternatively, the cations [M(cod)(NCCH3)2]BF4 (M = Ir, Rh) reacted with gaseous ammonia at atmospheric pressure affording bis(ammine) complexes [M(cod)(NH3)2]BF4 [M = Ir (5), Rh (6)], which were found to react with acetone, forming cations [M(cod)(κN,κN-NH2–C(CH3)2–CH2–C(CH3)=NH)]BF4 [M = Ir (7), Rh (8)]. DFT studies reveal that the transformation of 6 into 8 is mediated by NH3 molecules acting as an external base. The reaction is triggered by deprotonation of an ammonia ligand forming a amido–metal intermediate, which further transforms into an acetimino ligand through aldol condensation. The terminal methyl group of one acetimino ligand is deprotonated by NH3 yielding an enamine ligand, which can react with the imine ligand through concerted nucleophilic addition to afford the metallacycle, which is stabilized by protonation. | - |
dc.description.sponsorship | The authors express their appreciation for the financial support by the Spanish Ministerio de Economía y Competitividad/Fondo Europeo de Desarrollo Regional (MINECO/FEDER) (projectCTQ2015-67366-P) and the Diputación General de Aragón (group E07) (DGA/FSE-E07). Support from the KFUPM – University of Zaragoza and the Centre of Research Excellence in Petroleum Refining & Petrochemicals (KFUPM) is gratefully acknowledged. | - |
dc.publisher | Wiley-VCH | - |
dc.relation | info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2015-67366-P | - |
dc.rights | closedAccess | - |
dc.subject | C-C coupling | - |
dc.subject | C-N coupling | - |
dc.subject | Ammonia | - |
dc.subject | Rhodium | - |
dc.subject | Iridium | - |
dc.title | C–N bond coupling reactions of ammonia with acetone promoted by iridium and rhodium complexes: Experimental and DFT studies | - |
dc.type | artículo | - |
dc.identifier.doi | 10.1002/ejic.201600925 | - |
dc.date.updated | 2017-09-06T09:31:28Z | - |
dc.description.version | Peer Reviewed | - |
dc.language.rfc3066 | eng | - |
dc.contributor.funder | King Fahd University of Petroleum and Minerals | - |
dc.contributor.funder | Diputación General de Aragón | - |
dc.contributor.funder | European Commission | - |
dc.contributor.funder | Ministerio de Economía y Competitividad (España) | - |
dc.contributor.funder | Universidad de Zaragoza | - |
dc.relation.csic | Sí | - |
dc.identifier.funder | http://dx.doi.org/10.13039/501100004055 | es_ES |
dc.identifier.funder | http://dx.doi.org/10.13039/501100000780 | es_ES |
dc.identifier.funder | http://dx.doi.org/10.13039/501100003329 | es_ES |
dc.identifier.funder | http://dx.doi.org/10.13039/501100007041 | es_ES |
dc.type.coar | http://purl.org/coar/resource_type/c_6501 | es_ES |
item.cerifentitytype | Publications | - |
item.grantfulltext | none | - |
item.openairecristype | http://purl.org/coar/resource_type/c_18cf | - |
item.fulltext | No Fulltext | - |
item.openairetype | artículo | - |
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