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

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 and Holger Frauenrath ()
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Daniel Görl: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Shuichi Haraguchi: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Yevhen Hryshunin: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Sophia Thiele: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Giorgia Scetta: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Alexandre Simula: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Matthieu Wendling: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Oguzhan Oguz: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Nicolas Candau: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Torne Tänzer: Paul Scherrer Institute Photon Science Division 5232 Villigen PSI
Marianne Liebi: Paul Scherrer Institute Photon Science Division 5232 Villigen PSI
Christopher J. G. Plummer: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials
Holger Frauenrath: Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory of Macromolecular and Organic Materials

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-024-55166-1

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