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Organic Lewis Pairs Based on Phosphine and Electrophilic Silane for the Direct and Controlled Polymerization of Methyl Methacrylate: Experimental and Theoretical Investigations

dc.rights.licenseopen
hal.structure.identifierTeam 1 LCPO : Polymerization Catalyses & Engineering
dc.contributor.authorNZAHOU OTTOU, W.
dc.contributor.authorCONDE-MENDIZABAL, E.
hal.structure.identifierLaboratoire de Chimie des Polymères Organiques [LCPO]
dc.contributor.authorPASCUAL, A.
hal.structure.identifierLaboratoire de Chimie des Polymères Organiques [LCPO]
dc.contributor.authorWIROTIUS, A.-L.
dc.contributor.authorBOURICHON, D.
hal.structure.identifierLaboratoire de Chimie des Polymères Organiques [LCPO]
dc.contributor.authorVIGNOLLE, Joan
hal.structure.identifierLaboratoire de Caractérisation Physique Off-line [LCPO]
dc.contributor.authorROBERT, F.
hal.structure.identifierInstitut des Sciences Moléculaires [ISM]
dc.contributor.authorLANDAIS, Y.
hal.structure.identifierInstitut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux [IPREM]
dc.contributor.authorSOTIROPOULOS, Jean-Marc
hal.structure.identifierInstitut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux [IPREM]
dc.contributor.authorMIQUEU, Karinne
hal.structure.identifierLaboratoire de Chimie des Polymères Organiques [LCPO]
dc.contributor.authorTATON, Daniel
dc.date.accessioned2020
dc.date.available2020
dc.date.issued2017
dc.identifier.issn0024-9297
dc.identifier.urihttps://oskar-bordeaux.fr/handle/20.500.12278/20127
dc.description.abstractEnFully organic Lewis pairs, combining a phosphine such as tri-n-butylphosphine (PnBu3), tritert-butylphosphine (PtBu3) or tris(2,4,6-trimethoxyphenyl) phosphine (TTMPP) as a Lewis base, and N-(trimethylsilyl)bis(trifluoromethane sulfonyl)imide (Me3SiNTf2) as a Lewis acid, are shown to directly initiate the polymerization of methyl methacrylate (MMA) at room temperature in toluene. A dual reaction mechanism involving an optimal TTMPP:Me3SiNTf2 ratio of 1:2 accounts for the control of the polymerization. Molar masses of poly(methyl methacrylate)’s (PMMA’s) can be varied by the initial [MMA]0/[TTMPP]0 molar ratio. Chain extension experiments confirm that a majority of chains of a TTMPP/Me3SiNTf2-derived PMMA can be reactivated. Both density functional theory (DFT) calculations and stoichiometric studies reveal that TTMPP and Me3SiNTf2 form a P-silyl phosphonium intermediate that is in equilibrium with the corresponding frustrated Lewis pair (FLP). This FLP could correspond to the active form of the initiation step. Both computational and experimental data support the existence of a cooperative mechanism during the TTMPP/Me3SiNTf2 Lewis pair-mediated polymerization of MMA.
dc.description.sponsorshipPOLYMERISATIONS ORGANOCATALYSEES PAR LES CARBENES : VERS UNE PLATEFORME CATALYTIQUE MULTI-TACHE - ANR-11-BS08-0011
dc.language.isoen
dc.publisherAmerican Chemical Society
dc.title.enOrganic Lewis Pairs Based on Phosphine and Electrophilic Silane for the Direct and Controlled Polymerization of Methyl Methacrylate: Experimental and Theoretical Investigations
dc.typeArticle de revue
dc.identifier.doi10.1021/acs.macromol.6b02205
dc.subject.halChimie
dc.subject.halChimie/Chimie organique
dc.subject.halChimie/Chimie théorique et/ou physique
bordeaux.journalMacromolecules
bordeaux.page762-774
bordeaux.volume50
bordeaux.hal.laboratoriesLaboratoire de Chimie des Polymères Organiques (LCPO) - UMR 5629*
bordeaux.issue3
bordeaux.institutionBordeaux INP
bordeaux.institutionUniversité de Bordeaux
bordeaux.peerReviewedoui
hal.identifierhal-01499136
hal.version1
hal.origin.linkhttps://hal.archives-ouvertes.fr//hal-01499136v1
bordeaux.COinSctx_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.jtitle=Macromolecules&rft.date=2017&rft.volume=50&rft.issue=3&rft.spage=762-774&rft.epage=762-774&rft.eissn=0024-9297&rft.issn=0024-9297&rft.au=NZAHOU%20OTTOU,%20W.&CONDE-MENDIZABAL,%20E.&PASCUAL,%20A.&WIROTIUS,%20A.-L.&BOURICHON,%20D.&rft.genre=article


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