Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performance

Abstract The plastic waste crisis is among humanity’s most urgent challenges. However, widespread adoption of sustainable plastics is hindered by their often inadequate processing characteristics and performance. Here, we introduce a bio-inspired strategy for the modification of a representative hig...

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Main Authors: Daniel Görl, Shuichi Haraguchi, Yevhen Hryshunin, Sophia Thiele, Giorgia Scetta, Alexandre Simula, Matthieu Wendling, Oguzhan Oguz, Nicolas Candau, Torne Tänzer, Marianne Liebi, Christopher J. G. Plummer, Holger Frauenrath
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-55166-1
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author Daniel Görl
Shuichi Haraguchi
Yevhen Hryshunin
Sophia Thiele
Giorgia Scetta
Alexandre Simula
Matthieu Wendling
Oguzhan Oguz
Nicolas Candau
Torne Tänzer
Marianne Liebi
Christopher J. G. Plummer
Holger Frauenrath
author_facet Daniel Görl
Shuichi Haraguchi
Yevhen Hryshunin
Sophia Thiele
Giorgia Scetta
Alexandre Simula
Matthieu Wendling
Oguzhan Oguz
Nicolas Candau
Torne Tänzer
Marianne Liebi
Christopher J. G. Plummer
Holger Frauenrath
author_sort Daniel Görl
collection DOAJ
description Abstract The plastic waste crisis is among humanity’s most urgent challenges. However, widespread adoption of sustainable plastics is hindered by their often inadequate processing characteristics and performance. Here, we introduce a bio-inspired strategy for the modification of a representative high molar mass, biodegradable aliphatic polyester that helps overcome these limitations and remains effective at molar masses far greater than the entanglement molar mass. We use co-assembly of oligopeptide-based polymer end groups and a low molar mass additive to create a hierarchical structure characterized by regularly spaced nanofibrils interconnected by entangled polymer segments. The modified materials show a rubbery plateau at temperatures above their melting point, associated with strongly increased melt strength, extraordinary melt extensibility, improved dimensional stability, and accelerated crystallization. These thermomechanical property changes open up otherwise inaccessible processing routes and offer considerable scope for improving solid-state properties, thereby addressing typical shortcomings of sustainable alternatives to conventional plastics.
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institution Kabale University
issn 2041-1723
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series Nature Communications
spelling doaj-art-94fc8e6f469c40879a5fbf7dc12f69302025-01-05T12:39:38ZengNature PortfolioNature Communications2041-17232025-01-0116111310.1038/s41467-024-55166-1Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performanceDaniel Görl0Shuichi Haraguchi1Yevhen Hryshunin2Sophia Thiele3Giorgia Scetta4Alexandre Simula5Matthieu Wendling6Oguzhan Oguz7Nicolas Candau8Torne Tänzer9Marianne Liebi10Christopher J. G. Plummer11Holger Frauenrath12Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsPaul Scherrer Institute Photon Science Division 5232 Villigen PSIPaul Scherrer Institute Photon Science Division 5232 Villigen PSIEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsEcole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic MaterialsAbstract The plastic waste crisis is among humanity’s most urgent challenges. However, widespread adoption of sustainable plastics is hindered by their often inadequate processing characteristics and performance. Here, we introduce a bio-inspired strategy for the modification of a representative high molar mass, biodegradable aliphatic polyester that helps overcome these limitations and remains effective at molar masses far greater than the entanglement molar mass. We use co-assembly of oligopeptide-based polymer end groups and a low molar mass additive to create a hierarchical structure characterized by regularly spaced nanofibrils interconnected by entangled polymer segments. The modified materials show a rubbery plateau at temperatures above their melting point, associated with strongly increased melt strength, extraordinary melt extensibility, improved dimensional stability, and accelerated crystallization. These thermomechanical property changes open up otherwise inaccessible processing routes and offer considerable scope for improving solid-state properties, thereby addressing typical shortcomings of sustainable alternatives to conventional plastics.https://doi.org/10.1038/s41467-024-55166-1
spellingShingle Daniel Görl
Shuichi Haraguchi
Yevhen Hryshunin
Sophia Thiele
Giorgia Scetta
Alexandre Simula
Matthieu Wendling
Oguzhan Oguz
Nicolas Candau
Torne Tänzer
Marianne Liebi
Christopher J. G. Plummer
Holger Frauenrath
Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performance
Nature Communications
title Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performance
title_full Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performance
title_fullStr Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performance
title_full_unstemmed Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performance
title_short Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performance
title_sort supramolecular modification of sustainable high molar mass polymers for improved processing and performance
url https://doi.org/10.1038/s41467-024-55166-1
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