Publication:
Reductive Elimination Reactions in Gold(III) Complexes Leading to C(sp3)–X (X = C, N, P, O, Halogen) Bond Formation: Inner-Sphere vs SN2 Pathways

dc.contributor.authorPortugués Rodríguez, Alejandro
dc.contributor.authorMartínez-Nortes, Miguel Ángel
dc.contributor.authorBautista, Delia
dc.contributor.authorGonzález Herrero, Pablo
dc.contributor.authorGil Rubio, Juan
dc.contributor.departmentQuímica Inorgánica
dc.date.accessioned2024-01-25T11:37:56Z
dc.date.available2024-01-25T11:37:56Z
dc.date.copyright © 2023 The Authors
dc.date.issued2023-01-19
dc.description.abstractThe reactions leading to the formation of C–heteroatom bonds in the coordination sphere of Au(III) complexes are uncommon, and their mechanisms are not well known. This work reports on the synthesis and reductive elimination reactions of a series of Au(III) methyl complexes containing different Au–heteroatom bonds. Complexes [Au(CF3)(Me)(X)(PR3)] (R = Ph, X = OTf, OClO3, ONO2, OC(O)CF3, F, Cl, Br; R = Cy, X = Me, OTf, Br) were obtained by the reaction of trans-[Au(CF3)(Me)2(PR3)] (R = Ph, Cy) with HX. The cationic complex cis-[Au(CF3)(Me)(PPh3)2]OTf was obtained by the reaction of [Au(CF3)(Me)(OTf)(PPh3)] with PPh3. Heating these complexes led to the reductive elimination of MeX (X = Me, Ph3P+, OTf, OClO3, ONO2, OC(O)CF3, F, Cl, Br). Mechanistic studies indicate that these reductive elimination reactions occur either through (a) the formation of tricoordinate intermediates by phosphine dissociation, followed by reductive elimination of MeX, or (b) the attack of weakly coordinating anionic (TfO– or ClO4–) or neutral nucleophiles (PPh3 or NEt3) to the Au-bound methyl carbon. The obtained results show for the first time that the nucleophilic substitution should be considered as a likely reductive elimination pathway in Au(III) alkyl complexes.es
dc.formatapplication/pdfes
dc.format.extent35es
dc.identifier.citationInorganic Chemistry, 2023, vol. 62, issue 4, pag. 1708-1718
dc.identifier.doihttps://doi.org/10.1021/acs.inorgchem.2c04166
dc.identifier.issnElectronic: 1520-510X
dc.identifier.issnPrint: 0947-6539
dc.identifier.urihttp://hdl.handle.net/10201/137770
dc.languageenges
dc.publisherAmerican Chemical Societyes
dc.relationPROYECTO 1) Ministerio de Ciencia e Innovación/FEDER (Proyectos de I+D de Generación de Conocimiento 2018; nombre del proyecto: "Ampliando la aplicabilidad de los complejos organometálicos de metales de transición en catálisis y fotoquímica"; referencia PGC2018-100719-B-100). PROYECTO 2) Agencia de Ciencia y Tecnología de la Región de Murcia, Fundación Séneca (Ayudas a Grupos de Excelencia 2014; nombre del proyecto: "Síntesis, estructura y reactividad de nuevos tipos de complejos organometálicos. Aplicaciones como intermedios en síntesis y materiales fotoactivos", referencia 19890/GERM/15) . es
dc.relationFinancial support from the following grants is gratefully acknowledged: grant PGC2018-100719-B-I00 funded by MCIN/AEI/10.13039/501100011033 and by ERDF A way of making Europe; grant 19890/GERM/15 funded by the Séneca Foundation of the Region of Murcia (Ayudas a Grupos de Excelencia).
dc.relation.publisherversionhttps://pubs.acs.org/doi/10.1021/acs.inorgchem.2c04166es
dc.rightsinfo:eu-repo/semantics/openAccesses
dc.rightsAtribución 4.0 Internacional*
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/*
dc.subjectGoldes
dc.subjectAlkylses
dc.subjectDissociationes
dc.subjectReductive eliminationes
dc.subjectNucleophilic Substitutiones
dc.subject.otherCDU::5 - Ciencias puras y naturales::54 - Química::546 - Química inorgánicaes
dc.titleReductive Elimination Reactions in Gold(III) Complexes Leading to C(sp3)–X (X = C, N, P, O, Halogen) Bond Formation: Inner-Sphere vs SN2 Pathwayses
dc.typeinfo:eu-repo/semantics/articlees
dc.type.versioninfo:eu-repo/semantics/acceptedVersion
dspace.entity.typePublicationes
relation.isAuthorOfPublication244828c8-5381-49a7-9972-c550880196e5
relation.isAuthorOfPublication940323e4-526b-4ee9-b4f9-728b2b9a5da7
relation.isAuthorOfPublication2f3d3cfa-1196-4adc-8012-a11c570cafc4
relation.isAuthorOfPublication.latestForDiscovery244828c8-5381-49a7-9972-c550880196e5
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