Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites

Hydrolytic degradation of poly(4-hydroxybutyrate) (P4HB) films has been studied considering media of different pH values (i.e., 3, 7 and 10) and temperatures (i.e., 37 and 55 °C). Enzymatic degradation has also been evaluated at physiological conditions using two different lipases: Pseudomonas cepac...

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Autores: Keridou, Ina, Franco García, María Lourdes|||0000-0001-5968-285X, Valle Mendoza, Luis Javier del|||0000-0001-9916-1741, Martínez, Juan Carlos, Funk, Lutz, Turon Dols, Pau, Puiggalí Bellalta, Jordi|||0000-0002-0640-4474
Tipo de recurso: artículo
Fecha de publicación:2021
País:España
Institución:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/356575
Acceso en línea:https://hdl.handle.net/2117/356575
https://dx.doi.org/10.1016/j.polymdegradstab.2020.109451
Access Level:acceso abierto
Palabra clave:Polymers--Biodegradation
Enzymatic analysis
Poly(4-hydroxybutyrate)
Biodegradable polymers
Hydrolytic degradation
Enzymatic degradation
Films
Thermal properties
Microstructure
Polímers--Biodegradació
Anàlisi enzimàtica
Àrees temàtiques de la UPC::Enginyeria química
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spelling Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulitesKeridou, InaFranco García, María Lourdes|||0000-0001-5968-285XValle Mendoza, Luis Javier del|||0000-0001-9916-1741Martínez, Juan CarlosFunk, LutzTuron Dols, PauPuiggalí Bellalta, Jordi|||0000-0002-0640-4474Polymers--BiodegradationEnzymatic analysisPoly(4-hydroxybutyrate)Biodegradable polymersHydrolytic degradationEnzymatic degradationFilmsThermal propertiesMicrostructurePolímers--BiodegradacióAnàlisi enzimàticaÀrees temàtiques de la UPC::Enginyeria químicaHydrolytic degradation of poly(4-hydroxybutyrate) (P4HB) films has been studied considering media of different pH values (i.e., 3, 7 and 10) and temperatures (i.e., 37 and 55 °C). Enzymatic degradation has also been evaluated at physiological conditions using two different lipases: Pseudomonas cepacia and Rhizopus oryzae. Different bulk and surface erosion mechanisms with random chain scissions and successive removal of monomer units have been supported through weight loss measurements, molecular weight determinations by GPC and NMR spectroscopy and changes on thermal properties by DSC. Thermal annealing during exposure to different media and even degradation influenced on the melting temperature and crystallinity of samples, as well as on the lamellar geometrical parameters as evaluated by SAXS. Enzymatic degradation was ideal to selectively eliminate the amorphous regions and highlight the spherulitic morphology. Presence of ringed textures were therefore evident in bright field optical micrographs in addition to SEM images, namely observations under polarized light was not necessary to distinguish the presence of banded spherulites. Rhizopus oryzae was revealed to be the most suitable enzyme to crop out the P4HB spherulites that form part of the initial smooth surfaces of solvent casting films. After determining the appropriate activity and exposure time, the presence of rings constituted by cooperative C-shaped edge-on lamellae and flat-on lamellae was highlighted.Peer Reviewed20212021-01-0120212021-11-17journal articlehttp://purl.org/coar/resource_type/c_6501AMhttp://purl.org/coar/version/c_ab4af688f83e57aainfo:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/2117/356575https://dx.doi.org/10.1016/j.polymdegradstab.2020.109451reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivs 3.0 Spainhttp://creativecommons.org/licenses/by-nc-nd/3.0/es/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/3565752026-05-27T15:37:01Z
dc.title.none.fl_str_mv Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites
title Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites
spellingShingle Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites
Keridou, Ina
Polymers--Biodegradation
Enzymatic analysis
Poly(4-hydroxybutyrate)
Biodegradable polymers
Hydrolytic degradation
Enzymatic degradation
Films
Thermal properties
Microstructure
Polímers--Biodegradació
Anàlisi enzimàtica
Àrees temàtiques de la UPC::Enginyeria química
title_short Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites
title_full Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites
title_fullStr Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites
title_full_unstemmed Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites
title_sort Hydrolytic and enzymatic degradation of biobased poly(4-hydroxybutyrate) films. Selective etching of spherulites
dc.creator.none.fl_str_mv Keridou, Ina
Franco García, María Lourdes|||0000-0001-5968-285X
Valle Mendoza, Luis Javier del|||0000-0001-9916-1741
Martínez, Juan Carlos
Funk, Lutz
Turon Dols, Pau
Puiggalí Bellalta, Jordi|||0000-0002-0640-4474
author Keridou, Ina
author_facet Keridou, Ina
Franco García, María Lourdes|||0000-0001-5968-285X
Valle Mendoza, Luis Javier del|||0000-0001-9916-1741
Martínez, Juan Carlos
Funk, Lutz
Turon Dols, Pau
Puiggalí Bellalta, Jordi|||0000-0002-0640-4474
author_role author
author2 Franco García, María Lourdes|||0000-0001-5968-285X
Valle Mendoza, Luis Javier del|||0000-0001-9916-1741
Martínez, Juan Carlos
Funk, Lutz
Turon Dols, Pau
Puiggalí Bellalta, Jordi|||0000-0002-0640-4474
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv Polymers--Biodegradation
Enzymatic analysis
Poly(4-hydroxybutyrate)
Biodegradable polymers
Hydrolytic degradation
Enzymatic degradation
Films
Thermal properties
Microstructure
Polímers--Biodegradació
Anàlisi enzimàtica
Àrees temàtiques de la UPC::Enginyeria química
topic Polymers--Biodegradation
Enzymatic analysis
Poly(4-hydroxybutyrate)
Biodegradable polymers
Hydrolytic degradation
Enzymatic degradation
Films
Thermal properties
Microstructure
Polímers--Biodegradació
Anàlisi enzimàtica
Àrees temàtiques de la UPC::Enginyeria química
description Hydrolytic degradation of poly(4-hydroxybutyrate) (P4HB) films has been studied considering media of different pH values (i.e., 3, 7 and 10) and temperatures (i.e., 37 and 55 °C). Enzymatic degradation has also been evaluated at physiological conditions using two different lipases: Pseudomonas cepacia and Rhizopus oryzae. Different bulk and surface erosion mechanisms with random chain scissions and successive removal of monomer units have been supported through weight loss measurements, molecular weight determinations by GPC and NMR spectroscopy and changes on thermal properties by DSC. Thermal annealing during exposure to different media and even degradation influenced on the melting temperature and crystallinity of samples, as well as on the lamellar geometrical parameters as evaluated by SAXS. Enzymatic degradation was ideal to selectively eliminate the amorphous regions and highlight the spherulitic morphology. Presence of ringed textures were therefore evident in bright field optical micrographs in addition to SEM images, namely observations under polarized light was not necessary to distinguish the presence of banded spherulites. Rhizopus oryzae was revealed to be the most suitable enzyme to crop out the P4HB spherulites that form part of the initial smooth surfaces of solvent casting films. After determining the appropriate activity and exposure time, the presence of rings constituted by cooperative C-shaped edge-on lamellae and flat-on lamellae was highlighted.
publishDate 2021
dc.date.none.fl_str_mv 2021
2021-01-01
2021
2021-11-17
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
AM
http://purl.org/coar/version/c_ab4af688f83e57aa
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/2117/356575
https://dx.doi.org/10.1016/j.polymdegradstab.2020.109451
url https://hdl.handle.net/2117/356575
https://dx.doi.org/10.1016/j.polymdegradstab.2020.109451
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
Attribution-NonCommercial-NoDerivs 3.0 Spain
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
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
Attribution-NonCommercial-NoDerivs 3.0 Spain
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:UPCommons. Portal del coneixement obert de la UPC
instname:Universitat Politècnica de Catalunya (UPC)
instname_str Universitat Politècnica de Catalunya (UPC)
reponame_str UPCommons. Portal del coneixement obert de la UPC
collection UPCommons. Portal del coneixement obert de la UPC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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