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Rheo-2DIR spectroscopy reveals strain-induced hydrogen-bond redistribution in polyurethane

View ORCID ProfileGiulia Giubertoni, Michiel Hilbers, Hajo Groen, Anne Van der Weide, Daniel Bonn, Sander Woutersen
doi: https://doi.org/10.1101/2022.10.04.510759
Giulia Giubertoni
University of Amsterdam, Science Park 904, 1098XH Amsterdam, The Netherlands
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  • For correspondence: g.giubertoni@uva.nl
Michiel Hilbers
University of Amsterdam, Science Park 904, 1098XH Amsterdam, The Netherlands
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Hajo Groen
University of Amsterdam, Science Park 904, 1098XH Amsterdam, The Netherlands
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Anne Van der Weide
University of Amsterdam, Science Park 904, 1098XH Amsterdam, The Netherlands
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Daniel Bonn
University of Amsterdam, Science Park 904, 1098XH Amsterdam, The Netherlands
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Sander Woutersen
University of Amsterdam, Science Park 904, 1098XH Amsterdam, The Netherlands
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Abstract

The remarkable elastic properties of polymers are ultimately due to their molecular structure, but the relation between the macroscopic and molecular properties is often difficult to establish, in particular for (bio)polymers that contain hydrogen bonds, which can easily rearrange upon mechanical deformation. Here we show that two-dimensional infrared spectroscopy on polymer films in a miniature stress tester sheds new light on how the hydrogen-bond structure of a polymer is related to its visco-elastic response. We study thermoplastic polyurethane, a block copolymer consisting of hard segments of hydrogen-bonded urethane groups embedded in a soft matrix of polyether chains. The conventional infrared spectrum shows that upon deformation, the number of hydrogen bonds increases, a process that is largely reversible. However, the 2DIR spectrum reveals that the distribution hydrogen-bond strengths becomes slightly narrower after a deformation cycle, due to the disruption of weak hydrogen bonds, an effect that could explain the strain-cycle induced softening (Mullins effect) of polyurethane. These results show how rheo-2DIR spectroscopy can bridge the gap between the molecular structure and the macroscopic elastic properties of (bio)polymers.

Competing Interest Statement

The authors have declared no competing interest.

Footnotes

  • ↵* E-mail: g.giubertoni{at}uva.nl; s.woutersen{at}uva.nl

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The copyright holder for this preprint is the author/funder, who has granted bioRxiv a license to display the preprint in perpetuity. All rights reserved. No reuse allowed without permission.
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Posted October 04, 2022.
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Rheo-2DIR spectroscopy reveals strain-induced hydrogen-bond redistribution in polyurethane
Giulia Giubertoni, Michiel Hilbers, Hajo Groen, Anne Van der Weide, Daniel Bonn, Sander Woutersen
bioRxiv 2022.10.04.510759; doi: https://doi.org/10.1101/2022.10.04.510759
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Rheo-2DIR spectroscopy reveals strain-induced hydrogen-bond redistribution in polyurethane
Giulia Giubertoni, Michiel Hilbers, Hajo Groen, Anne Van der Weide, Daniel Bonn, Sander Woutersen
bioRxiv 2022.10.04.510759; doi: https://doi.org/10.1101/2022.10.04.510759

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