Giant (Aug 2023)

Highly stretchable and tough elastomers from cyclic polymers

  • Yang Chen,
  • Zhiwei Fan,
  • Yong Liu,
  • Yiru Wang,
  • Zeyu Wang,
  • Rongchun Zhang,
  • Bingxu Ma,
  • Yiliu Liu,
  • Wei Zhang,
  • Liqun Tang,
  • Taolin Sun

Journal volume & issue
Vol. 15
p. 100177

Abstract

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Developing solvent-free elastomers with a high stretchability and toughness is crucial for practical applications in flexible electronics and smart actuators. However, the stretchability of chemically crosslinked elastomers derived from linear polymers is often limited due to the trapped entanglements between polymer chains and a lack of energy dissipation mechanism. In this study, we developed a type of soft, highly stretchable, and tough elastomer derived from cyclic polymers by eliminating chain entanglements, and incorporating dynamic hydrogen bonds to provide an energy dissipation mechanism within the network. The non-concatenated cyclic polymers were synthesized through the ring-expansion metathesis polymerization (REMP), and the brush-modification of cyclic polymers clearly confirmed the desired cyclic species through atomic force microscope (AFM) observation. The non-concatenated cyclic polymers were further interconnected to form elastomers using the thiol-ene click reaction. In comparison to elastomers crosslinked from linear polymers with comparable molecular weights, cyclic polymer elastomers exhibit a combination of lower softness (E: 235.1 kPa), higher stretchability (λmax: 16.7) and toughness (We: 8.2 MJ/m3) due to their lower trapped entanglements and higher compact conformations.

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