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Bis(N-Heterocyclic Carbene) Manganese(I) Complexes in Catalytic N-Formylation/N-Methylation of Amines Using Carbon Dioxide and Phenylsilane

2023-12-01Artigo científico Acesso aberto
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dc.contributor.authorMasaro, Chiara
dc.contributor.authorMeloni, Giammarco
dc.contributor.authorBaron, Marco
dc.contributor.authorGraiff, Claudia
dc.contributor.authorTubaro, Cristina
dc.contributor.authorRoyo, Beatriz
dc.contributor.institutionInstituto de Tecnologia Química e Biológica António Xavier (ITQB)
dc.contributor.pblWiley
dc.date.accessioned2024-04-02T23:51:34Z
dc.date.available2024-04-02T23:51:34Z
dc.date.issued2023-12-01
dc.description01BIRD2019‐UNIPD, PI: M. Baron] and by Fundação para a Ciência e Tecnologia (FCT) for Projects PTDC/QUI‐QIN/0359/2021, MOSTMICRO‐ITQB, UDIB/04612/2020, and UIPD/04612/2020. The National NMR Facility is supported by CERMAX through Project 022162. C. Almeida and UniMS facility at ITQB NOVA are acknowledged for HRMS. The authors would like to thank the Crystallography Service of the LAQV, Department of Chemistry, NOVA School of Science and Technology, Portugal, for the structural determination of the complexes and . 2 d 2 e Publisher Copyright: © 2023 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.
dc.description.abstractA series of six Mn(I) complexes with general formula [MnBr(bisNHC)(CO)3], having a bidentate bis(N-heterocyclic carbene) ligand (bisNHC), has been developed by varying the bridging group between the NHC donors, the nitrogen wingtip substituents and the heterocyclic ring. The synthesis of the complexes has been accomplished by in situ transmetalation of the bisNHC from the corresponding silver(I) complexes. Removal of the bromide anion affords the corresponding solvento complexes [Mn(bisNHC)(CO)3(CH3CN)](BF4). The influence of the bisNHC structure on its electron donor ability has been evaluated by FTIR and 13C NMR spectroscopy, both in the neutral and cationic complexes. Finally, the isolated Mn(I)-bisNHC complexes have been employed as homogeneous catalysts in the reductive N-formylation and N-methylation of amines with CO2 as C1 source and phenylsilane as reducing agent, showing a high selectivity for the N-methylated product. Preliminary mechanistic investigations suggest that, in the adopted reaction conditions, the formylated product can be formed via different reaction pathways, either metal-catalyzed or not, while the methylation reaction requires the use of the Mn(I) catalyst.en
dc.description.versionpublishersversion
dc.description.versionpublished
dc.format.extent2036587
dc.identifier.doi10.1002/chem.202302273
dc.identifier.issn0947-6539
dc.identifier.otherPURE: 83686450
dc.identifier.otherPURE UUID: 8f5e3834-6550-4aa0-b608-e93caa3b44b8
dc.identifier.otherScopus: 85174624997
dc.identifier.otherPubMed: 37695746
dc.identifier.otherORCID: /0000-0002-7909-9992/work/156734887
dc.identifier.urihttp://hdl.handle.net/10362/165735
dc.identifier.urlhttps://www.scopus.com/pages/publications/85174624997
dc.language.isoeng
dc.peerreviewedyes
dc.relationFunding Information: This work was supported by the Department of Chemical Sciences of the University of Padova [P-DiSC
dc.relation01BIRD2019-UNIPD, PI: M. Baron] and by Fundação para a Ciência e Tecnologia (FCT) for Projects PTDC/QUI-QIN/0359/2021, MOSTMICRO-ITQB, UDIB/04612/2020, and UIPD/04612/2020. The National NMR Facility is supported by CERMAX through Project 022162. C. Almeida and UniMS facility at ITQB NOVA are acknowledged for HRMS. The authors would like to thank the Crystallography Service of the LAQV, Department of Chemistry, NOVA School of Science and Technology, Portugal, for the structural determination of the complexes 2 d and 2 e. Funding Information: This work was supported by the Department of Chemical Sciences of the University of Padova [P‐DiSC
dc.subjectbidentate ligands
dc.subjectcarbon dioxide valorization
dc.subjectmanganese(I) complexes
dc.subjectmethylation of amines
dc.subjectN-heterocyclic carbene
dc.subjectCatalysis
dc.subjectGeneral Chemistry
dc.subjectOrganic Chemistry
dc.titleBis(N-Heterocyclic Carbene) Manganese(I) Complexes in Catalytic N-Formylation/N-Methylation of Amines Using Carbon Dioxide and Phenylsilaneen
dc.typejournal article
degois.publication.issue67
degois.publication.titleChemistry - A European Journal
degois.publication.volume29
dspace.entity.typePublication
rcaap.rightsopenAccess

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