Toughening and Stiffening in Thermoreversible Diels–Alder Polymer Network Blends

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Abstract

The thermophysical properties, mechanical behavior, and healing performance of Diels–Alder-based polymer networks can be tuned widely by changing the molar mass, functionality, and stoichiometric ratio of the multifunctional diene (e.g., furan) and dienophile (e.g., maleimide) monomers. Blending furan-functionalized monomers with a high and low molar mass opens a new dimension in tuning the properties of the resulting reversible polymer network blends (RPNBs), containing different ratios of elastomeric and thermoset phases, with low and high crosslink densities and glass transitions below and above room temperature, respectively. Increasing the thermoset content up to 20 wt % raises the gel transition temperature (Tgel), relaxation time (τ), rubbery plateau modulus, ultimate stress, and Young’s modulus of the stiffened elastomers, while the strain at fracture and self-healing efficiency remained mostly unchanged. Conversely, the addition of up to 20 wt % of the elastomer phase drastically toughens the thermosets because of stress dissipation, which can suppress the stress concentration in the phase-separated network blends. The blends showed higher stress and strain at break while retaining similar Young’s moduli. The toughness increases up to an order of magnitude at 50 wt %, compared to the pure thermoset. The phase-separated morphologies were evidenced by the presence of the Tg’s of the pure networks in DSC and DMA.
Original languageEnglish
Pages (from-to)4325–4335
Number of pages11
JournalMacromolecules
Volume56
Issue number11
DOIs
Publication statusPublished - 24 May 2023

Bibliographical note

Funding Information:
This research was performed in relation to and funded by the Open Project SHINTO (101057960) and the FWO SBO Project AMSeR (G028218N). In addition, the authors gratefully acknowledge the Fonds Wetenschappelijk Onderzoek (FWO) for the personal grants to S.T. (1100416N) and J.B. (12E1123N).

Publisher Copyright:
© 2023 American Chemical Society.

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