Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes
The catalytic activity of two halometallate complexes based on imidazolium cations, (dimim)[FeCl4] (1) and (dimim)2[Fe2Cl6(μ-O)] (2), was evaluated in the glycolysis of polyethylene terephthalate (PET), either under conventional heating or microwave-assisted conditions. The two procedures led to the...
| Autores: | , , , , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2019 |
| País: | España |
| Institución: | Universidad de Cantabria (UC) |
| Repositorio: | UCrea Repositorio Abierto de la Universidad de Cantabria |
| Idioma: | inglés |
| OAI Identifier: | oai:repositorio.unican.es:10902/18452 |
| Acceso en línea: | http://hdl.handle.net/10902/18452 |
| Access Level: | acceso abierto |
| Palabra clave: | Imidazolium-based halometallate complex Iron-containing ionic liquid Poly(ethylene terephthalate) Bis(2-hydroxyethyl)terephthalate Glycolysis |
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Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexesSce, FabioCano, IsraelMartín, CarmenBeobide Pacheco, GarikoitzCastillo, ÓscarPedro del Valle, Imanol de|||0000-0002-5581-2220Imidazolium-based halometallate complexIron-containing ionic liquidPoly(ethylene terephthalate)Bis(2-hydroxyethyl)terephthalateGlycolysisThe catalytic activity of two halometallate complexes based on imidazolium cations, (dimim)[FeCl4] (1) and (dimim)2[Fe2Cl6(μ-O)] (2), was evaluated in the glycolysis of polyethylene terephthalate (PET), either under conventional heating or microwave-assisted conditions. The two procedures led to the formation of bis(2-hydroxyethyl)terephthalate (BHET) as the major product with high yields, also allowing the isolation and structural characterization of a new polymorph. The influence of the halometallate structure on the catalytic activity was investigated, and additional experimental studies proved the involvement of both the imidazolium cation and metal anion in the reaction mechanism. The comparison of both approaches showed the advantages of the microwave methodology in terms of efficiency and time saving. Indeed, the use of ground PET and microwave heating provided quantitative yields of BHET. Under conventional heating conditions, the dinuclear iron complex gave a slightly lower yield than (dimim)[FeCl4] (74% vs. 77% for post-consumer PET) after 24 h of reaction. However, the microwave-assisted process led to comparable results in remarkably shorter reaction times (2 h). Interestingly, complex 2, containing the dipolar [Fe2Cl6(μ-O)]2− moiety, provided higher yields than 1 with the non-dipolar [FeCl4]− anion (77% vs. 69%). This behaviour has been rationalized on the basis of dielectric heating mechanisms (polarization and conduction), and it suggests a new approach towards obtaining more efficient catalysts by tailoring the catalytic species to be active in both heating mechanisms.Financial support from the Spanish Ministerio de Ciencia e Innovación (Projects MAT2014-55049-C2-R and MAT2016-75883-C2-1-P), Universidad del País Vasco/EuskalHerrikoUnibertsitatea (GIU17/50 and PPG17/37). Universidad de Cantabria (Proyecto Puente convocatoria 2018 financed by SODERCAN-FEDER).Royal Society of ChemistryUniversidad de Cantabria20192019-06-22journal articlehttp://purl.org/coar/resource_type/c_6501NAhttp://purl.org/coar/version/c_be7fb7dd8ff6fe43info:eu-repo/semantics/articlehttp://hdl.handle.net/10902/18452New J. Chem., 2019,43, 3476-3485reponame:UCrea Repositorio Abierto de la Universidad de Cantabriainstname:Universidad de Cantabria (UC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:repositorio.unican.es:10902/184522026-06-02T12:39:31Z |
| dc.title.none.fl_str_mv |
Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes |
| title |
Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes |
| spellingShingle |
Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes Sce, Fabio Imidazolium-based halometallate complex Iron-containing ionic liquid Poly(ethylene terephthalate) Bis(2-hydroxyethyl)terephthalate Glycolysis |
| title_short |
Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes |
| title_full |
Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes |
| title_fullStr |
Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes |
| title_full_unstemmed |
Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes |
| title_sort |
Comparing conventional and microwave-assisted heating in PET degradation mediated by imidazolium-based halometallate complexes |
| dc.creator.none.fl_str_mv |
Sce, Fabio Cano, Israel Martín, Carmen Beobide Pacheco, Garikoitz Castillo, Óscar Pedro del Valle, Imanol de|||0000-0002-5581-2220 |
| author |
Sce, Fabio |
| author_facet |
Sce, Fabio Cano, Israel Martín, Carmen Beobide Pacheco, Garikoitz Castillo, Óscar Pedro del Valle, Imanol de|||0000-0002-5581-2220 |
| author_role |
author |
| author2 |
Cano, Israel Martín, Carmen Beobide Pacheco, Garikoitz Castillo, Óscar Pedro del Valle, Imanol de|||0000-0002-5581-2220 |
| author2_role |
author author author author author |
| dc.contributor.none.fl_str_mv |
Universidad de Cantabria |
| dc.subject.none.fl_str_mv |
Imidazolium-based halometallate complex Iron-containing ionic liquid Poly(ethylene terephthalate) Bis(2-hydroxyethyl)terephthalate Glycolysis |
| topic |
Imidazolium-based halometallate complex Iron-containing ionic liquid Poly(ethylene terephthalate) Bis(2-hydroxyethyl)terephthalate Glycolysis |
| description |
The catalytic activity of two halometallate complexes based on imidazolium cations, (dimim)[FeCl4] (1) and (dimim)2[Fe2Cl6(μ-O)] (2), was evaluated in the glycolysis of polyethylene terephthalate (PET), either under conventional heating or microwave-assisted conditions. The two procedures led to the formation of bis(2-hydroxyethyl)terephthalate (BHET) as the major product with high yields, also allowing the isolation and structural characterization of a new polymorph. The influence of the halometallate structure on the catalytic activity was investigated, and additional experimental studies proved the involvement of both the imidazolium cation and metal anion in the reaction mechanism. The comparison of both approaches showed the advantages of the microwave methodology in terms of efficiency and time saving. Indeed, the use of ground PET and microwave heating provided quantitative yields of BHET. Under conventional heating conditions, the dinuclear iron complex gave a slightly lower yield than (dimim)[FeCl4] (74% vs. 77% for post-consumer PET) after 24 h of reaction. However, the microwave-assisted process led to comparable results in remarkably shorter reaction times (2 h). Interestingly, complex 2, containing the dipolar [Fe2Cl6(μ-O)]2− moiety, provided higher yields than 1 with the non-dipolar [FeCl4]− anion (77% vs. 69%). This behaviour has been rationalized on the basis of dielectric heating mechanisms (polarization and conduction), and it suggests a new approach towards obtaining more efficient catalysts by tailoring the catalytic species to be active in both heating mechanisms. |
| publishDate |
2019 |
| dc.date.none.fl_str_mv |
2019 2019-06-22 |
| dc.type.none.fl_str_mv |
journal article http://purl.org/coar/resource_type/c_6501 NA http://purl.org/coar/version/c_be7fb7dd8ff6fe43 |
| dc.type.openaire.fl_str_mv |
info:eu-repo/semantics/article |
| format |
article |
| dc.identifier.none.fl_str_mv |
http://hdl.handle.net/10902/18452 |
| url |
http://hdl.handle.net/10902/18452 |
| dc.language.none.fl_str_mv |
Inglés eng |
| language_invalid_str_mv |
Inglés |
| language |
eng |
| dc.rights.none.fl_str_mv |
open access http://purl.org/coar/access_right/c_abf2 |
| dc.rights.openaire.fl_str_mv |
info:eu-repo/semantics/openAccess |
| rights_invalid_str_mv |
open access http://purl.org/coar/access_right/c_abf2 |
| eu_rights_str_mv |
openAccess |
| dc.publisher.none.fl_str_mv |
Royal Society of Chemistry |
| publisher.none.fl_str_mv |
Royal Society of Chemistry |
| dc.source.none.fl_str_mv |
New J. Chem., 2019,43, 3476-3485 reponame:UCrea Repositorio Abierto de la Universidad de Cantabria instname:Universidad de Cantabria (UC) |
| instname_str |
Universidad de Cantabria (UC) |
| reponame_str |
UCrea Repositorio Abierto de la Universidad de Cantabria |
| collection |
UCrea Repositorio Abierto de la Universidad de Cantabria |
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|
| repository.mail.fl_str_mv |
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1869407428260397056 |
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15,300719 |