Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers

Achieving a unique combination of stiffness, strength, extensibility, and toughness in sol-cast poly(urethane–urea) (PU) copolymer films is a challenge since these properties are—in general—mutually exclusive. Here we demonstrate that geometric confinement of the basic building blocks controls stiff...

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Autores: Oguz, Oguzhan, Candau, Nicolas|||0000-0002-1559-8696, Stoclet, Grégory, Simsek, Erem, Kosak Soz, Cagla, Yilgor, Emel, Yilgor, Iskender, Menceloglu, Yusuf Z.
Formato: artículo
Fecha de publicación:2021
País:España
Recursos:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/377852
Acesso em linha:https://hdl.handle.net/2117/377852
https://dx.doi.org/10.1021/acs.macromol.1c00596
Access Level:acceso abierto
Palavra-chave:Copolymers
Crystallization
Crystals
Organic polymers
Urea
Copolímers
Cristal·lització
Àrees temàtiques de la UPC::Enginyeria dels materials
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spelling Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymersOguz, OguzhanCandau, Nicolas|||0000-0002-1559-8696Stoclet, GrégorySimsek, EremKosak Soz, CaglaYilgor, EmelYilgor, IskenderMenceloglu, Yusuf Z.CopolymersCrystallizationCopolymersCrystallizationCrystalsOrganic polymersUreaCopolímersCristal·litzacióÀrees temàtiques de la UPC::Enginyeria dels materialsAchieving a unique combination of stiffness, strength, extensibility, and toughness in sol-cast poly(urethane–urea) (PU) copolymer films is a challenge since these properties are—in general—mutually exclusive. Here we demonstrate that geometric confinement of the basic building blocks controls stiffness, strength, extensibility, and toughness in PU films. Our results suggest that the severity of geometric confinement can be tuned by adjusting (i) soft segment molecular weight (SSMW) and (ii) drying temperature (DT) thanks to their effects on the structure formation via microphase separation and/or (confined and/or bulk) crystallization. It is therefore possible to produce (i) soft (no notable confinement) and (ii) stiff, strong, extensible, and tough (severe confinement) materials without changing any other parameter except SSMW and DT. The former has a typical physically cross-linked network and shows a well-defined elastomeric behavior with an elastic modulus (E) of 5–20 MPa, a tensile strength (smax) of 30–35 MPa, an extensibility (e) of 1000–1300%, and a toughness (W) of 90–180 MJ m–3. The latter, on the other hand, possesses an elegant hierarchical structure containing tightly packed secondary structures (72-helix, 41-helix, and antiparallel ß-sheets) and displays an elastoplastic behavior with an E of 400–700 MPa, a smax of 45–55 MPa, an e of 650–850%, and a W of 200–250 MJ m–3. Hence, our findings may be of interest in designing advanced materials containing synthetic replica of the secondary structures found in protein-based materials. The structure formation in the materials with this structural hierarchy is driven by the confined crystallization of helical poly(ethylene oxide) (PEO) chains in subnanometer urea channels, which—to the best of our knowledge—is a phenomenon well-known in host–guest systems but has not yet demonstrated in PU copolymers, and complemented by the “bulk” crystallization of PEO and/or the microphase separation.Peer ReviewedAmerican Chemical Society (ACS)20212021-05-2520222022-12-12journal articlehttp://purl.org/coar/resource_type/c_6501AMhttp://purl.org/coar/version/c_ab4af688f83e57aainfo:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/2117/377852https://dx.doi.org/10.1021/acs.macromol.1c00596reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/3778522026-05-27T15:37:01Z
dc.title.none.fl_str_mv Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers
title Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers
spellingShingle Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers
Oguz, Oguzhan
Copolymers
Crystallization
Copolymers
Crystallization
Crystals
Organic polymers
Urea
Copolímers
Cristal·lització
Àrees temàtiques de la UPC::Enginyeria dels materials
title_short Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers
title_full Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers
title_fullStr Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers
title_full_unstemmed Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers
title_sort Geometric confinement controls stiffness, strength, extensibility, and toughness in poly(urethane–urea) copolymers
dc.creator.none.fl_str_mv Oguz, Oguzhan
Candau, Nicolas|||0000-0002-1559-8696
Stoclet, Grégory
Simsek, Erem
Kosak Soz, Cagla
Yilgor, Emel
Yilgor, Iskender
Menceloglu, Yusuf Z.
author Oguz, Oguzhan
author_facet Oguz, Oguzhan
Candau, Nicolas|||0000-0002-1559-8696
Stoclet, Grégory
Simsek, Erem
Kosak Soz, Cagla
Yilgor, Emel
Yilgor, Iskender
Menceloglu, Yusuf Z.
author_role author
author2 Candau, Nicolas|||0000-0002-1559-8696
Stoclet, Grégory
Simsek, Erem
Kosak Soz, Cagla
Yilgor, Emel
Yilgor, Iskender
Menceloglu, Yusuf Z.
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Copolymers
Crystallization
Copolymers
Crystallization
Crystals
Organic polymers
Urea
Copolímers
Cristal·lització
Àrees temàtiques de la UPC::Enginyeria dels materials
topic Copolymers
Crystallization
Copolymers
Crystallization
Crystals
Organic polymers
Urea
Copolímers
Cristal·lització
Àrees temàtiques de la UPC::Enginyeria dels materials
description Achieving a unique combination of stiffness, strength, extensibility, and toughness in sol-cast poly(urethane–urea) (PU) copolymer films is a challenge since these properties are—in general—mutually exclusive. Here we demonstrate that geometric confinement of the basic building blocks controls stiffness, strength, extensibility, and toughness in PU films. Our results suggest that the severity of geometric confinement can be tuned by adjusting (i) soft segment molecular weight (SSMW) and (ii) drying temperature (DT) thanks to their effects on the structure formation via microphase separation and/or (confined and/or bulk) crystallization. It is therefore possible to produce (i) soft (no notable confinement) and (ii) stiff, strong, extensible, and tough (severe confinement) materials without changing any other parameter except SSMW and DT. The former has a typical physically cross-linked network and shows a well-defined elastomeric behavior with an elastic modulus (E) of 5–20 MPa, a tensile strength (smax) of 30–35 MPa, an extensibility (e) of 1000–1300%, and a toughness (W) of 90–180 MJ m–3. The latter, on the other hand, possesses an elegant hierarchical structure containing tightly packed secondary structures (72-helix, 41-helix, and antiparallel ß-sheets) and displays an elastoplastic behavior with an E of 400–700 MPa, a smax of 45–55 MPa, an e of 650–850%, and a W of 200–250 MJ m–3. Hence, our findings may be of interest in designing advanced materials containing synthetic replica of the secondary structures found in protein-based materials. The structure formation in the materials with this structural hierarchy is driven by the confined crystallization of helical poly(ethylene oxide) (PEO) chains in subnanometer urea channels, which—to the best of our knowledge—is a phenomenon well-known in host–guest systems but has not yet demonstrated in PU copolymers, and complemented by the “bulk” crystallization of PEO and/or the microphase separation.
publishDate 2021
dc.date.none.fl_str_mv 2021
2021-05-25
2022
2022-12-12
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/2117/377852
https://dx.doi.org/10.1021/acs.macromol.1c00596
url https://hdl.handle.net/2117/377852
https://dx.doi.org/10.1021/acs.macromol.1c00596
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-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
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-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society (ACS)
publisher.none.fl_str_mv American Chemical Society (ACS)
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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