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The role of undecenoic acid on the preparation of cecorated MCM-41/Polyethylene hybrids by In situ polymerization: Catalytic aspects and properties of the resultant materials

2023-08-02 Open access
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dc.contributor.authorCerrada, María L.
dc.contributor.authorBento, Artur
dc.contributor.authorPérez, Ernesto
dc.contributor.authorLourenço, João P.
dc.contributor.authorRibeiro, M. Rosário
dc.date.accessioned2023-09-04T16:53:07Z
dc.date.available2023-09-04T16:53:07Z
dc.date.issued2023-08-02
dc.date.updated2023-08-25T12:37:51Z
dc.description.abstractFunctionalized polyethylene-based nanocomposites were prepared by in situ polymerization of ethylene with modified or neat MCM-41 nanoparticles (NMCM-41). Two different synthetic approaches were investigated to improve the compatibility between the hydrophobic HDPE matrix and the hydrophilic NMCM-41: (i) incorporation of UA into the polymeric matrix by copolymerization with ethylene, promoted by the zirconocene catalyst under homogeneous conditions, in the presence of pristine NMCM-41; (ii) use of undecenoic acid (UA) as an interfacial agent to obtain decorated NMCM-41 to be used as nanofiller for the in situ ethylene polymerization, catalyzed by Cp2ZrCl2/MAO under supported conditions. The strong polar character of the carboxylic group is expected to either increase the hydrophilicity of the HDPE chains (strategy i) or interact with the NMCM-41 surface and provide an additional link to the polymeric chains via copolymerization of the vinyl group under supported conditions (strategy ii). Although metallocene catalysts have been shown to copolymerize olefins with functional monomers, the presence of oxygen-containing compounds in the reaction media strongly affects the polymerization activity as a result of the interaction of functional groups with the electrophilic active center of the catalyst. Thus, UA was pre-contacted with tri(isobutyl)aluminum (TIBA) prior to its use in the polymerization to reduce the deactivating character of the carboxylic acid groups towards the zirconocene catalyst. The influence of the UA presence on the polymerization behavior of the protection step is discussed, and the polymerization activities observed for the different approaches are compared. In addition, the thermal behavior and structural details of the resulting materials have been characterized. The impact of using neat or functionalized NMCM-41 on the final dispersion within the polymeric matrix is also analyzed, which is correlated with the mechanical performance exhibited by these HDPE_UA_NMCM-41 nanocomposites.
dc.description.sponsorshipMCIN/AEI/10.13039/501100011033, LA/P/0056/2020
dc.identifier.citationCatalysts 13 (8): 1182 (2023)
dc.identifier.doi10.3390/catal13081182
dc.identifier.eissn2073-4344
dc.identifier.urihttp://hdl.handle.net/10400.1/19946
dc.publisherMDPI
dc.relationCentro de Química Estrutural
dc.relationCentro de Química Estrutural
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/
dc.subjectPolyethylene
dc.subjectUndecenoic acid
dc.subjectMCM-41
dc.subjectNanocomposites
dc.subjectDispersion
dc.subjectCrystallinity
dc.subjectStiffness
dc.titleThe role of undecenoic acid on the preparation of cecorated MCM-41/Polyethylene hybrids by In situ polymerization: Catalytic aspects and properties of the resultant materials
dspace.entity.typePublication
oaire.awardTitleCentro de Química Estrutural
oaire.awardTitleCentro de Química Estrutural
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/6817 - DCRRNI ID/UIDB%2F00100%2F2020/PT
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/6817 - DCRRNI ID/UIDP%2F00100%2F2020/PT
oaire.citation.issue13
oaire.citation.startPage1182
oaire.citation.volume8
oaire.fundingStream6817 - DCRRNI ID
oaire.fundingStream6817 - DCRRNI ID
person.familyNameLourenço
person.givenNameJoão P.
person.identifier634248
person.identifier.ciencia-idF81F-A1F0-2A7C
person.identifier.orcid0000-0002-0501-6672
person.identifier.ridA-7758-2008
person.identifier.scopus-author-id57195730600
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.nameFundação para a Ciência e a Tecnologia
project.funder.nameFundação para a Ciência e a Tecnologia
rcaap.rightsopenAccess
relation.isAuthorOfPublicationf66ab886-d989-4c1d-9550-527507723c26
relation.isAuthorOfPublication.latestForDiscoveryf66ab886-d989-4c1d-9550-527507723c26
relation.isProjectOfPublicationdf39fd72-bd68-4aaf-8b89-25d17b8c5ebd
relation.isProjectOfPublication36364d2a-b4fe-4b0f-a8c8-ca575b121cf4
relation.isProjectOfPublication.latestForDiscoverydf39fd72-bd68-4aaf-8b89-25d17b8c5ebd

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