Guanidine functionalized porous SiO2 as heterogeneous catalysts for microwave depolymerization of PET and PLA

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dc.contributor.authorCasey, Éadaoinen
dc.contributor.authorBreen, Rachelen
dc.contributor.authorPareras, Gerarden
dc.contributor.authorRimola, Alberten
dc.contributor.authorHolmes, Justin D.en
dc.contributor.authorCollins, Gillianen
dc.contributor.funderScience Foundation Irelanden
dc.date.accessioned2024-05-15T13:24:14Z
dc.date.available2024-05-15T13:24:14Z
dc.date.issued2024-03-06en
dc.description.abstractChemical recycling is an important strategy to tackle the growing global problem of plastic waste pollution. The development of metal-free catalysts for depolymerization of plastics is attractive as it avoids the use of metal salts, which are potentially damaging to the environment. Here we report a metal-free heterogeneous catalyst for the glycolysis of polyethylene terephthalate (PET) and methanolysis of polylactic acid (PLA). The catalysts are synthesized by covalent surface modification of mesoporous silica (SiO2) with guanidine ligands and evaluated under conventional thermal and microwave-assisted heating. A surface bound cyanoguanidine ligand was found to be the best catalyst leading to 100% PET conversion with 80% BHET yield. The nature of the catalyst support material influenced the catalytic performance of the guanidine ligands with porous SiO2 supports outperforming activated carbon in conventional thermal glycolysis, while the opposite trend was observed with microwave assisted glycolysis. Dedicated density functional theory (DFT) computations were performed to simulate the depolymerization processes, obtain the free energy profiles of the reaction mechanisms, and identify the important role of hydrogen bonding in the reaction mechanism.en
dc.description.sponsorshipScience Foundation Ireland (AMBER Grant No. 12/RC2278_P2)en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationCasey, É., Breen, R., Pareras, G., Rimola, A., Holmes, J. D. and Collins, G. (2024) 'Guanidine functionalized porous SiO 2 as heterogeneous catalysts for microwave depolymerization of PET and PLA', RSC Sustainability, 2(4), pp.1040-1051. Available at: https://doi.org/10.1039/D3SU00425Ben
dc.identifier.doihttps://doi.org/10.1039/D3SU00425Ben
dc.identifier.eissn2753-8125en
dc.identifier.endpage1051en
dc.identifier.issued4en
dc.identifier.journaltitleRSC Sustainabilityen
dc.identifier.startpage1040en
dc.identifier.urihttps://hdl.handle.net/10468/15872
dc.identifier.volume2en
dc.language.isoenen
dc.publisherRoyal Society of Chemistryen
dc.rights© 2024, the Authors. Published by the Royal Society of Chemistry. This open access article is made available under the CC BY-NC license (https://creativecommons.org/licenses/by-nc/4.0/)en
dc.rights.urihttps://creativecommons.org/licenses/by-nc/4.0/en
dc.subjectChemical recyclingen
dc.subjectPlastic waste pollutionen
dc.subjectMetal-free catalysts for depolymerization of plasticsen
dc.subjectMetal-free heterogeneous catalysten
dc.subjectGlycolysisen
dc.subjectPolyethylene terephthalate (PET)en
dc.subjectMethanolysisen
dc.subjectPolylactic acid (PLA)en
dc.subjectMesoporous silica (SiO2)en
dc.subjectGuanidine ligandsen
dc.titleGuanidine functionalized porous SiO2 as heterogeneous catalysts for microwave depolymerization of PET and PLAen
dc.typeArticle (peer-reviewed)en
oaire.citation.issue4en
oaire.citation.volume2en
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