Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse

In this work, amphiphilic block copolymers (BCs) consisting of a hydrophilic poly(ethylene glycol) methyl ether (PEG) and a degradable polycarbonate block derived from 2,2-bis(hydroxymethyl)propionic acid (bis-MPA) with pendant ureido units, along with corresponding homopolycarbonates are described....

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Autores: Martín-Martín, Javier, Abad, Miriam, Lopez de Pariza, Xabier, Ezquerra, Tiberio A., Nogales, Aurora, Sardon, Haritz, Sebastián, Víctor, Oriol, Luis, Piñol, Milagros
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/387218
Acceso en línea:http://hdl.handle.net/10261/387218
https://api.elsevier.com/content/abstract/scopus_id/105000465809
Access Level:acceso abierto
Palabra clave:UCST behavior
Amphiphilic block copolymers
Degradable polymers
Polymer self‐assembly
Thermoresponsive polymers
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dc.title.none.fl_str_mv Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse
title Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse
spellingShingle Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse
Martín-Martín, Javier
UCST behavior
Amphiphilic block copolymers
Degradable polymers
Polymer self‐assembly
Thermoresponsive polymers
title_short Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse
title_full Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse
title_fullStr Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse
title_full_unstemmed Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse
title_sort Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponse
dc.creator.none.fl_str_mv Martín-Martín, Javier
Abad, Miriam
Lopez de Pariza, Xabier
Ezquerra, Tiberio A.
Nogales, Aurora
Sardon, Haritz
Sebastián, Víctor
Oriol, Luis
Piñol, Milagros
author Martín-Martín, Javier
author_facet Martín-Martín, Javier
Abad, Miriam
Lopez de Pariza, Xabier
Ezquerra, Tiberio A.
Nogales, Aurora
Sardon, Haritz
Sebastián, Víctor
Oriol, Luis
Piñol, Milagros
author_role author
author2 Abad, Miriam
Lopez de Pariza, Xabier
Ezquerra, Tiberio A.
Nogales, Aurora
Sardon, Haritz
Sebastián, Víctor
Oriol, Luis
Piñol, Milagros
author2_role author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Ministerio de Ciencia e Innovación (España)
Gobierno de Aragón
Universidad de Zaragoza
Consejo Superior de Investigaciones Científicas (España)
Agencia Estatal de Investigación (España)
Ministerio de Ciencia, Innovación y Universidades (España)
Martin-Martin, Javier [0000-0002-4833-5796]
Abad, Miriam [0000-0002-8677-3316]
Lopez de Pariza, Xabier [0000-0002-0758-1712]
Ezquerra, Tiberio A. [0000-0001-9966-519X]
Nogales, Aurora [0000-0002-2494-3551]
Sardon, Haritz [0000-0002-6268-0916]
Sebastián, Víctor [0000-0002-6873-5244]
Oriol, Luis [0000-0002-0922-5615]
Piñol, Milagros [0000-0001-5556-2172]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv UCST behavior
Amphiphilic block copolymers
Degradable polymers
Polymer self‐assembly
Thermoresponsive polymers
topic UCST behavior
Amphiphilic block copolymers
Degradable polymers
Polymer self‐assembly
Thermoresponsive polymers
description In this work, amphiphilic block copolymers (BCs) consisting of a hydrophilic poly(ethylene glycol) methyl ether (PEG) and a degradable polycarbonate block derived from 2,2-bis(hydroxymethyl)propionic acid (bis-MPA) with pendant ureido units, along with corresponding homopolycarbonates are described. Polymers are synthesized by combining ring opening polymerization (ROP) and thiol-ene/yne functionalization to incorporate UCST-promoting ureido groups. For homopolycarbonates, increasing the ureido groups density along the polymer chain facilitates the upper critical solution temperature (UCST)-type thermoresponse in water. Because of their amphiphilic character, BCs form stable self-assemblies either by direct dispersion in water, co-solvent method or microfluidics. Upon heating, these self-assemblies swell, and collapse due to extensive hydration of the polycarbonate block, rather than becoming solubilized. Thermoresponsiveness is analyzed in terms of the number of ureido groups in the polycarbonate for a given polycarbonate block length as well as the length of polycarbonate block. As a proof of concept, the potential of these self-assemblies as thermoresponsive drug nanocarriers is evaluated, using curcumin as a hydrophobic model drug.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/387218
https://api.elsevier.com/content/abstract/scopus_id/105000465809
url http://hdl.handle.net/10261/387218
https://api.elsevier.com/content/abstract/scopus_id/105000465809
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
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info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-127847OB-I00
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/CEX2023-001286-S
The underlying dataset has been published as supplementary material of the article in the publisher platform at DOI 10.1002/marc.202500029
https://doi.org/10.1002/marc.202500029
Sí
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dc.publisher.none.fl_str_mv Wiley-VCH
publisher.none.fl_str_mv Wiley-VCH
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
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spelling Degradable ureido-polycarbonate block copolymers with a complex UCST thermoresponseMartín-Martín, JavierAbad, MiriamLopez de Pariza, XabierEzquerra, Tiberio A.Nogales, AuroraSardon, HaritzSebastián, VíctorOriol, LuisPiñol, MilagrosUCST behaviorAmphiphilic block copolymersDegradable polymersPolymer self‐assemblyThermoresponsive polymersIn this work, amphiphilic block copolymers (BCs) consisting of a hydrophilic poly(ethylene glycol) methyl ether (PEG) and a degradable polycarbonate block derived from 2,2-bis(hydroxymethyl)propionic acid (bis-MPA) with pendant ureido units, along with corresponding homopolycarbonates are described. Polymers are synthesized by combining ring opening polymerization (ROP) and thiol-ene/yne functionalization to incorporate UCST-promoting ureido groups. For homopolycarbonates, increasing the ureido groups density along the polymer chain facilitates the upper critical solution temperature (UCST)-type thermoresponse in water. Because of their amphiphilic character, BCs form stable self-assemblies either by direct dispersion in water, co-solvent method or microfluidics. Upon heating, these self-assemblies swell, and collapse due to extensive hydration of the polycarbonate block, rather than becoming solubilized. Thermoresponsiveness is analyzed in terms of the number of ureido groups in the polycarbonate for a given polycarbonate block length as well as the length of polycarbonate block. As a proof of concept, the potential of these self-assemblies as thermoresponsive drug nanocarriers is evaluated, using curcumin as a hydrophobic model drug.This work was financially supported by MICIN/AEI (PDI2021-1261132NB-100 and PID2021-127847OB-I00) and Gobierno de Aragón-FSE(LMP93_21 and E47_23R). INMA authors acknowledge grant CEX2023-001286-S funded by MICIU/AEI/10.13039/501100011033. JMM acknowl-edges MICIN/AEI his FPI PhD grant. Authors would like to acknowledgethe use of Servicio General de Apoyo a la Investigación-SAI, Universidad de Zaragoza, NAMBIOSIS and ELECMI-Laboratorio de Microscopías Avanzadas-LMA (INMA-Unizar) and Servicios Científicos Técnicos ofCEQMA (CSIC-Unizar). The authors would also like to thank Dr. P.Romero for her invaluable guidance in the NMR studies. CSIC-ConexiónNanomedicina is also acknowledged.With funding from the Spanish government through the "Severo Ochoa Centre of Excellence" accreditation (CEX2023-001286-S).Peer reviewedWiley-VCHMinisterio de Ciencia e Innovación (España)Gobierno de AragónUniversidad de ZaragozaConsejo Superior de Investigaciones Científicas (España)Agencia Estatal de Investigación (España)Ministerio de Ciencia, Innovación y Universidades (España)Martin-Martin, Javier [0000-0002-4833-5796]Abad, Miriam [0000-0002-8677-3316]Lopez de Pariza, Xabier [0000-0002-0758-1712]Ezquerra, Tiberio A. [0000-0001-9966-519X]Nogales, Aurora [0000-0002-2494-3551]Sardon, Haritz [0000-0002-6268-0916]Sebastián, Víctor [0000-0002-6873-5244]Oriol, Luis [0000-0002-0922-5615]Piñol, Milagros [0000-0001-5556-2172]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252025info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10261/387218https://api.elsevier.com/content/abstract/scopus_id/105000465809reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/AEI//PID2021-1261132NB-100info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-127847OB-I00info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/CEX2023-001286-SThe underlying dataset has been published as supplementary material of the article in the publisher platform at DOI 10.1002/marc.202500029https://doi.org/10.1002/marc.202500029Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3872182026-05-22T06:33:51Z
score 15,811543

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