Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals

Abstract: Utilization of reversible non-covalent interactions is a versatile design strategy for the development of stimuli responsive soft materials. In this study, hydrophobic interactions were harnessed to assemble water-soluble macromolecules and nanoparticles into a transient hybrid network for...

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Autores: Nigmatullin, Rinat, Gabrielli, Valeria, Muñoz-García, Juan C., Lewandowska, Anna E., Harniman, Robert, Khimyak, Yaroslav Z., Angulo, Jesús, Eichhorn, Stephen J.
Formato: artículo
Estado:Versión publicada
Fecha de publicación:2019
País:España
Recursos:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/387166
Acesso em linha:http://hdl.handle.net/10261/387166
https://api.elsevier.com/content/abstract/scopus_id/85059692823
Access Level:acceso abierto
Palavra-chave:Thermoresponsive
Cellulose nanocrystals
Hydrogel
Hydroxypropyl methylcellulose
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spelling Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystalsNigmatullin, RinatGabrielli, ValeriaMuñoz-García, Juan C.Lewandowska, Anna E.Harniman, RobertKhimyak, Yaroslav Z.Angulo, JesúsEichhorn, Stephen J.ThermoresponsiveCellulose nanocrystalsHydrogelHydroxypropyl methylcelluloseAbstract: Utilization of reversible non-covalent interactions is a versatile design strategy for the development of stimuli responsive soft materials. In this study, hydrophobic interactions were harnessed to assemble water-soluble macromolecules and nanoparticles into a transient hybrid network forming thermosensitive hydrogels with tunable rheological properties. Hybrid hydrogels were built of biopolymer derived components: cellulose nanocrystals (CNCs), nanoparticles of high aspect ratio, and hydroxypropyl methylcellulose (HPMC). To enable polymer/CNC assembly via hydrophobic interactions, the surface of highly hydrophilic CNCs was modified by binding octyl moieties (octyl-CNCs). The amphiphilicity of octyl-CNCs was confirmed by surface tension measurements. The molecular and particulate amphiphiles assemble into hybrid networks, which result in stiffer and stronger hydrogels compared to HPMC hydrogels and hydrogels reinforced with hydrophilic CNCs. Hybrid hydrogels retain the ability of HPMC hydrogels to flow under applied shear stress. However, significantly higher viscosity was achieved for HPMC/octyl-CNCs compared with HPMC/CNCs hydrogels. The inherent thermal response of rheological properties of HPMC hydrogels was further amplified in combination with octyl-CNCs due to temperature-induced polymer/nanoparticle association via hydrophobic interactions. Saturation transfer difference NMR spectroscopy demonstrated the growth of network-bound water with an increase in temperature, which correlates with the increase of stiffness and viscosity of hydrogels upon heating. Rheological properties of these hybrid hydrogels are defined by the content of the soluble polymer and the CNCs, and it is shown that they can be finely adjusted for a required application. Graphical abstract: [Figure not available: see fulltext.].The Engineering and Physical Sciences Research Council (EPSRC) is acknowledged for provision of financial support (EP/N03340X/2, EP/N033337/1). We are grateful for the use of the University of East Anglia (UEA) Faculty of Science NMR facility and the Wolfson Bioimaging Facility of the University of Bristol. We would like to thank Mrs Judith Mantell for the cryo-SEM micrographs of the hydrogels.Peer reviewedSpringerEngineering and Physical Sciences Research Council (UK)University of East AngliaUniversity of BristolNigmatullin, Rinat [0000-0003-3517-1208]Gabrielli, Valeria [0000-0003-0475-5032]Muñoz-García, Juan C. [0000-0003-2246-3236]Lewandowska, Anna E. [0000-0001-7768-7216]Harniman, Robert [0000-0002-3452-1213]Khimyak, Yaroslav Z. [0000-0003-0424-4128]Angulo, Jesús [0000-0001-7250-5639]Eichhorn, Stephen J. [0000-0003-4101-273X]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252019info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionaplication/pdfhttp://hdl.handle.net/10261/387166https://api.elsevier.com/content/abstract/scopus_id/85059692823reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE#1777178https://doi.org/10.1007/s10570-018-02225-8Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3871662026-05-22T06:33:51Z
dc.title.none.fl_str_mv Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals
title Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals
spellingShingle Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals
Nigmatullin, Rinat
Thermoresponsive
Cellulose nanocrystals
Hydrogel
Hydroxypropyl methylcellulose
title_short Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals
title_full Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals
title_fullStr Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals
title_full_unstemmed Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals
title_sort Thermosensitive supramolecular and colloidal hydrogels via self-assembly modulated by hydrophobized cellulose nanocrystals
dc.creator.none.fl_str_mv Nigmatullin, Rinat
Gabrielli, Valeria
Muñoz-García, Juan C.
Lewandowska, Anna E.
Harniman, Robert
Khimyak, Yaroslav Z.
Angulo, Jesús
Eichhorn, Stephen J.
author Nigmatullin, Rinat
author_facet Nigmatullin, Rinat
Gabrielli, Valeria
Muñoz-García, Juan C.
Lewandowska, Anna E.
Harniman, Robert
Khimyak, Yaroslav Z.
Angulo, Jesús
Eichhorn, Stephen J.
author_role author
author2 Gabrielli, Valeria
Muñoz-García, Juan C.
Lewandowska, Anna E.
Harniman, Robert
Khimyak, Yaroslav Z.
Angulo, Jesús
Eichhorn, Stephen J.
author2_role author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Engineering and Physical Sciences Research Council (UK)
University of East Anglia
University of Bristol
Nigmatullin, Rinat [0000-0003-3517-1208]
Gabrielli, Valeria [0000-0003-0475-5032]
Muñoz-García, Juan C. [0000-0003-2246-3236]
Lewandowska, Anna E. [0000-0001-7768-7216]
Harniman, Robert [0000-0002-3452-1213]
Khimyak, Yaroslav Z. [0000-0003-0424-4128]
Angulo, Jesús [0000-0001-7250-5639]
Eichhorn, Stephen J. [0000-0003-4101-273X]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Thermoresponsive
Cellulose nanocrystals
Hydrogel
Hydroxypropyl methylcellulose
topic Thermoresponsive
Cellulose nanocrystals
Hydrogel
Hydroxypropyl methylcellulose
description Abstract: Utilization of reversible non-covalent interactions is a versatile design strategy for the development of stimuli responsive soft materials. In this study, hydrophobic interactions were harnessed to assemble water-soluble macromolecules and nanoparticles into a transient hybrid network forming thermosensitive hydrogels with tunable rheological properties. Hybrid hydrogels were built of biopolymer derived components: cellulose nanocrystals (CNCs), nanoparticles of high aspect ratio, and hydroxypropyl methylcellulose (HPMC). To enable polymer/CNC assembly via hydrophobic interactions, the surface of highly hydrophilic CNCs was modified by binding octyl moieties (octyl-CNCs). The amphiphilicity of octyl-CNCs was confirmed by surface tension measurements. The molecular and particulate amphiphiles assemble into hybrid networks, which result in stiffer and stronger hydrogels compared to HPMC hydrogels and hydrogels reinforced with hydrophilic CNCs. Hybrid hydrogels retain the ability of HPMC hydrogels to flow under applied shear stress. However, significantly higher viscosity was achieved for HPMC/octyl-CNCs compared with HPMC/CNCs hydrogels. The inherent thermal response of rheological properties of HPMC hydrogels was further amplified in combination with octyl-CNCs due to temperature-induced polymer/nanoparticle association via hydrophobic interactions. Saturation transfer difference NMR spectroscopy demonstrated the growth of network-bound water with an increase in temperature, which correlates with the increase of stiffness and viscosity of hydrogels upon heating. Rheological properties of these hybrid hydrogels are defined by the content of the soluble polymer and the CNCs, and it is shown that they can be finely adjusted for a required application. Graphical abstract: [Figure not available: see fulltext.].
publishDate 2019
dc.date.none.fl_str_mv 2019
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/10261/387166
https://api.elsevier.com/content/abstract/scopus_id/85059692823
url http://hdl.handle.net/10261/387166
https://api.elsevier.com/content/abstract/scopus_id/85059692823
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
1777178
https://doi.org/10.1007/s10570-018-02225-8
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv aplication/pdf
dc.publisher.none.fl_str_mv Springer
publisher.none.fl_str_mv Springer
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
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,81155

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