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High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide

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Resumo:This study investigates the low-temperature depolymerization of polyethylene terephthalate (PET) using near-stoichiometric choline hydroxide (ChOH) in methanol, assisted by dichloromethane (DCM) or dimethoxymethane (DMM) as co-solvents. The DCM-assisted system enables rapid apparent PET depolymerization within 30 min under mild conditions, whereas the DMM-assisted system achieves hydrolysis within 20 h at room temperature, yielding choline terephthalate and ethylene glycol. Although slower, the DMM-assisted process proceeds more smoothly, as supported by spectroscopic and microscopic analyses, while the DCM-assisted route leads to accumulation of partially hydrolysed intermediates and transient micro/nanoplastic residues during the early stages of hydrolysis. The studied processes exhibit high atom economy due to the near-stoichiometric use of choline hydroxide and simplified product isolation without acid neutralization or extensive purification steps. In addition, benchmarking based on energy and environmental metrics was extended to account for multistage operations such as solvent removal, drying, and metathesis processes, enabling more comprehensive comparison with previously reported PET depolymerization methods. The results highlight the importance of balanced benchmarking when evaluating sustainability claims in chemical plastic recycling and demonstrate the potential of choline hydroxide-mediated PET hydrolysis as a low-temperature and resource-efficient depolymerization strategy.
Autores principais:Araujo, Hugo Q.
Outros Autores:Martins, Diogo; Goncalves, Joao; Matos, Ines; Ventura, Marcia; Diniz, Mario; Tomazio, Diana; Branco, Luis C.; Lapa, Nuno; Petrovski, Zeljko
Assunto:Analytical Chemistry Chemistry (miscellaneous) Organic Chemistry Electrochemistry
Ano:2026
País:Portugal
Tipo de documento:artigo
Tipo de acesso:acesso aberto
Instituição associada:Universidade Nova de Lisboa
Idioma:inglês
Origem:Repositório Institucional da UNL
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author Araujo, Hugo Q.
author2 Martins, Diogo
Goncalves, Joao
Matos, Ines
Ventura, Marcia
Diniz, Mario
Tomazio, Diana
Branco, Luis C.
Lapa, Nuno
Petrovski, Zeljko
author2_role author
author
author
author
author
author
author
author
author
author_facet Araujo, Hugo Q.
Martins, Diogo
Goncalves, Joao
Matos, Ines
Ventura, Marcia
Diniz, Mario
Tomazio, Diana
Branco, Luis C.
Lapa, Nuno
Petrovski, Zeljko
author_role author
contributor_name_str_mv LAQV@REQUIMTE
UCIBIO - Applied Molecular Biosciences Unit
RSC - Royal Society of Chemistry
RUN
country_str PT
creators_json_txt [{\"Person.name\":\"Araujo, Hugo Q.\"},{\"Person.name\":\"Martins, Diogo\"},{\"Person.name\":\"Goncalves, Joao\"},{\"Person.name\":\"Matos, Ines\"},{\"Person.name\":\"Ventura, Marcia\"},{\"Person.name\":\"Diniz, Mario\"},{\"Person.name\":\"Tomazio, Diana\"},{\"Person.name\":\"Branco, Luis C.\"},{\"Person.name\":\"Lapa, Nuno\"},{\"Person.name\":\"Petrovski, Zeljko\"}]
datacite.contributors.contributor.contributorName.fl_str_mv LAQV@REQUIMTE
UCIBIO - Applied Molecular Biosciences Unit
RSC - Royal Society of Chemistry
RUN
datacite.creators.creator.creatorName.fl_str_mv Araujo, Hugo Q.
Martins, Diogo
Goncalves, Joao
Matos, Ines
Ventura, Marcia
Diniz, Mario
Tomazio, Diana
Branco, Luis C.
Lapa, Nuno
Petrovski, Zeljko
datacite.date.Accepted.fl_str_mv 2026-09-01T00:00:00Z
datacite.date.available.fl_str_mv 2026-09-07T14:07:01Z
datacite.date.embargoed.fl_str_mv 2026-09-07T14:07:01Z
datacite.rights.fl_str_mv http://purl.org/coar/access_right/c_abf2
datacite.subjects.subject.fl_str_mv Analytical Chemistry
Chemistry (miscellaneous)
Organic Chemistry
Electrochemistry
datacite.titles.title.fl_str_mv High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
dc.contributor.none.fl_str_mv LAQV@REQUIMTE
UCIBIO - Applied Molecular Biosciences Unit
RSC - Royal Society of Chemistry
RUN
dc.creator.none.fl_str_mv Araujo, Hugo Q.
Martins, Diogo
Goncalves, Joao
Matos, Ines
Ventura, Marcia
Diniz, Mario
Tomazio, Diana
Branco, Luis C.
Lapa, Nuno
Petrovski, Zeljko
dc.date.Accepted.fl_str_mv 2026-09-01T00:00:00Z
dc.date.available.fl_str_mv 2026-09-07T14:07:01Z
dc.date.embargoed.fl_str_mv 2026-09-07T14:07:01Z
dc.format.none.fl_str_mv application/pdf
dc.identifier.none.fl_str_mv http://hdl.handle.net/10362/206132
dc.language.none.fl_str_mv eng
dc.rights.none.fl_str_mv http://purl.org/coar/access_right/c_abf2
dc.subject.none.fl_str_mv Analytical Chemistry
Chemistry (miscellaneous)
Organic Chemistry
Electrochemistry
dc.title.fl_str_mv High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
dc.type.none.fl_str_mv http://purl.org/coar/resource_type/c_6501
description This study investigates the low-temperature depolymerization of polyethylene terephthalate (PET) using near-stoichiometric choline hydroxide (ChOH) in methanol, assisted by dichloromethane (DCM) or dimethoxymethane (DMM) as co-solvents. The DCM-assisted system enables rapid apparent PET depolymerization within 30 min under mild conditions, whereas the DMM-assisted system achieves hydrolysis within 20 h at room temperature, yielding choline terephthalate and ethylene glycol. Although slower, the DMM-assisted process proceeds more smoothly, as supported by spectroscopic and microscopic analyses, while the DCM-assisted route leads to accumulation of partially hydrolysed intermediates and transient micro/nanoplastic residues during the early stages of hydrolysis. The studied processes exhibit high atom economy due to the near-stoichiometric use of choline hydroxide and simplified product isolation without acid neutralization or extensive purification steps. In addition, benchmarking based on energy and environmental metrics was extended to account for multistage operations such as solvent removal, drying, and metathesis processes, enabling more comprehensive comparison with previously reported PET depolymerization methods. The results highlight the importance of balanced benchmarking when evaluating sustainability claims in chemical plastic recycling and demonstrate the potential of choline hydroxide-mediated PET hydrolysis as a low-temperature and resource-efficient depolymerization strategy.
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eu_rights_str_mv openAccess
format article
fulltext.url.fl_str_mv https://run.unl.pt/bitstreams/78a5f228-b406-47cb-b19f-1cfed3a212ae/download
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identifier.url.fl_str_mv http://hdl.handle.net/10362/206132
inst_facet_str urn:organizationAcronym:unl{{{_:::_}}}Universidade Nova de Lisboa
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institution Universidade Nova de Lisboa
instname_str Universidade Nova de Lisboa
language eng
network_acronym_str run
network_name_str Repositório Institucional da UNL
oai_identifier_str oai:run.unl.pt:10362/206132
organization_str_mv urn:organizationAcronym:unl
person_str_mv Araujo, Hugo Q.
Martins, Diogo
Goncalves, Joao
Matos, Ines
Ventura, Marcia
Diniz, Mario
Tomazio, Diana
Branco, Luis C.
Lapa, Nuno
Petrovski, Zeljko
publishDate 2026
repo_facet_str urn:repositoryAcronym:run{{{_:::_}}}Repositório Institucional da UNL
reponame_str Repositório Institucional da UNL
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service_str_mv urn:repositoryAcronym:run
spelling engenThis study investigates the low-temperature depolymerization of polyethylene terephthalate (PET) using near-stoichiometric choline hydroxide (ChOH) in methanol, assisted by dichloromethane (DCM) or dimethoxymethane (DMM) as co-solvents. The DCM-assisted system enables rapid apparent PET depolymerization within 30 min under mild conditions, whereas the DMM-assisted system achieves hydrolysis within 20 h at room temperature, yielding choline terephthalate and ethylene glycol. Although slower, the DMM-assisted process proceeds more smoothly, as supported by spectroscopic and microscopic analyses, while the DCM-assisted route leads to accumulation of partially hydrolysed intermediates and transient micro/nanoplastic residues during the early stages of hydrolysis. The studied processes exhibit high atom economy due to the near-stoichiometric use of choline hydroxide and simplified product isolation without acid neutralization or extensive purification steps. In addition, benchmarking based on energy and environmental metrics was extended to account for multistage operations such as solvent removal, drying, and metathesis processes, enabling more comprehensive comparison with previously reported PET depolymerization methods. The results highlight the importance of balanced benchmarking when evaluating sustainability claims in chemical plastic recycling and demonstrate the potential of choline hydroxide-mediated PET hydrolysis as a low-temperature and resource-efficient depolymerization strategy.application/pdfenHigh atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxideAraujo, Hugo Q.Martins, DiogoGoncalves, JoaoMatos, InesVentura, MarciaDiniz, MarioTomazio, DianaBranco, Luis C.Lapa, NunoPetrovski, ZeljkoLAQV@REQUIMTEUCIBIO - Applied Molecular Biosciences UnitRSC - Royal Society of ChemistryHostingInstitutionOrganizationalRUNe-mailmailto:run@unl.ptrun@unl.ptISSNIsPartOf2753-8125URNIsPartOfPURE: 171486430URNIsPartOfPURE UUID: 6495b0a3-aef5-4a98-884d-995ac5de5f19URNIsPartOfWOS: 001824690000001URNIsPartOfScopus: 105045422179URNIsPartOfORCID: /0000-0002-8104-7008/work/226046369URNIsPartOfORCID: /0000-0001-7862-7477/work/226047114DOIIsPartOf10.1039/d6su00314a2026-09-07T14:07:01Z2026-09-012026-09-01T00:00:00ZHandlehttp://hdl.handle.net/10362/206132http://purl.org/coar/access_right/c_abf2open accessAnalytical ChemistryChemistry (miscellaneous)Organic ChemistryElectrochemistry1115794 bytesliteraturehttp://purl.org/coar/resource_type/c_6501journal articlehttp://purl.org/coar/access_right/c_abf2application/pdffulltexthttps://run.unl.pt/bitstreams/78a5f228-b406-47cb-b19f-1cfed3a212ae/download
spellingShingle High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
Araujo, Hugo Q.
Analytical Chemistry
Chemistry (miscellaneous)
Organic Chemistry
Electrochemistry
status SINGLETON
subject.fl_str_mv Analytical Chemistry
Chemistry (miscellaneous)
Organic Chemistry
Electrochemistry
title High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
title_full High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
title_fullStr High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
title_full_unstemmed High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
title_short High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
title_sort High atom-economy low-temperature depolymerization of polyethylene terephthalate using choline hydroxide
topic Analytical Chemistry
Chemistry (miscellaneous)
Organic Chemistry
Electrochemistry
topic_facet Analytical Chemistry
Chemistry (miscellaneous)
Organic Chemistry
Electrochemistry
url http://hdl.handle.net/10362/206132
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