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

Author

Listed:
  • 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
    Science & Innovation Center
    Department of Chemistry and Chemical Engineering)

  • 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
    Departament de Ciència i Enginyeria de Materials (CEM))

  • Torne Tänzer

    (Paul Scherrer Institute Photon Science Division 5232 Villigen PSI
    Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory for X-ray Characterization of Materials)

  • Marianne Liebi

    (Paul Scherrer Institute Photon Science Division 5232 Villigen PSI
    Ecole Polytechnique Fédérale de Lausanne (EPFL), Institute of Materials, Laboratory for X-ray Characterization of Materials)

  • 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)

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.

Suggested Citation

  • Daniel Görl & Shuichi Haraguchi & Yevhen Hryshunin & Sophia Thiele & Giorgia Scetta & Alexandre Simula & Matthieu Wendling & Oguzhan Oguz & Nicolas Candau & Torne Tänzer & Marianne Liebi & Christopher, 2025. "Supramolecular modification of sustainable high-molar-mass polymers for improved processing and performance," Nature Communications, Nature, vol. 16(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-024-55166-1
    DOI: 10.1038/s41467-024-55166-1
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    References listed on IDEAS

    as
    1. Yunqing Zhu & Charles Romain & Charlotte K. Williams, 2016. "Sustainable polymers from renewable resources," Nature, Nature, vol. 540(7633), pages 354-362, December.
    2. Emmanuel Croisier & Su Liang & Thomas Schweizer & Sandor Balog & Marijana Mionić & Ruben Snellings & Joël Cugnoni & Véronique Michaud & Holger Frauenrath, 2014. "A toolbox of oligopeptide-modified polymers for tailored elastomers," Nature Communications, Nature, vol. 5(1), pages 1-10, December.
    3. Manuel Häußler & Marcel Eck & Dario Rothauer & Stefan Mecking, 2021. "Closed-loop recycling of polyethylene-like materials," Nature, Nature, vol. 590(7846), pages 423-427, February.
    4. Philippe Cordier & François Tournilhac & Corinne Soulié-Ziakovic & Ludwik Leibler, 2008. "Self-healing and thermoreversible rubber from supramolecular assembly," Nature, Nature, vol. 451(7181), pages 977-980, February.
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