Highly stretchable ionically crosslinked acrylate elastomers inspired by polyelectrolyte complexes

Cai, Hongyi; Wang, Zhongtong; Utomo, Nyalaliska W.; Vidavsky, Yuval; Silberstein, Meredith N.

doi:10.1039/d2sm00755j

Title: Highly stretchable ionically crosslinked acrylate elastomers inspired by polyelectrolyte complexes

Journal Article · Thu Sep 22 00:00:00 EDT 2022 · Soft Matter

DOI:https://doi.org/10.1039/d2sm00755j· OSTI ID:1905601

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Cornell Univ., Ithaca, NY (United States)
Cornell Univ., Ithaca, NY (United States); Soreq NRC, Yavne (Israel)

Dynamic bonds are a powerful approach to tailor the mechanical properties of elastomers and introduce shape-memory, self-healing, and recyclability. Among the library of dynamic crosslinks, electrostatic interactions among oppositely charged ions have been shown to enable tough and resilient elastomers and hydrogels. In this work, we investigate the mechanical properties of ionically crosslinked ethyl acrylate-based elastomers assembled from oppositely charged copolymers. Using both infrared and Raman spectroscopy, we confirm that ionic interactions are established among polymer chains. We find that the glass transition temperature of the complex is in between the two individual copolymers, while the complex demonstrates higher stiffness and more recovery, indicating that ionic bonds can strengthen and enhance recovery of these elastomers. We compare cycles to increasing strain levels at different strain rates, and hypothesize that at fast strain rates ionic bonds dynamically break and reform while entanglements do not have time to slip, and at slow strain rates ionic interactions are disrupted and these entanglements slip significantly. Further, we show that a higher ionic to neutral monomer ratio can increase the stiffness, but its effect on recovery is minimal. Lastly, taking advantage of the versatility of acrylates, ethyl acrylate is replaced with the more hydrophilic 2-hydroxyethyl acrylate, and the latter is shown to exhibit better recovery and self-healing at a cost of stiffness and strength. The design principles uncovered for these easy-to-manufacture polyelectrolyte complex-inspired bulk materials can be broadly applied to tailor elastomer stiffness, strength, inelastic recovery, and self-healing for various applications.

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Research Organization:: Cornell Univ., Ithaca, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019141; # DE-SC0019141

OSTI ID:: 1905601

Alternate ID(s):: OSTI ID: 1890252

Journal Information:: Soft Matter, Vol. 18, Issue 39; Related Information: https://www.rsc.org/suppdata/d2/sm/d2sm00755j/d2sm00755j1.pdf; ISSN 1744-683X

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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