5 years ago

Tough Elastomers with Superior Self-Recoverability Induced by Bioinspired Multiphase Design

Tough Elastomers with Superior Self-Recoverability Induced by Bioinspired Multiphase Design
Hirotaka Ejima, Shoma Yoshida, Naoko Yoshie
Incorporating reversible sacrificial bonds in network polymers not only toughens these materials but also endows them with self-recoverability. However, self-recoverability is only realized for dispersed energy less than 10 MJ m−3. It remains a challenge to achieve simultaneous high stretchability, toughness, and recoverability. Here, inspired by the structure of mussel byssus cuticles, a new design strategy is proposed and demonstrated to improve both the toughness and self-recoverability of elastomers by introducing a microphase-separated structure with different physical crosslink densities. This structure can be achieved using a carefully designed comonomer sequence distribution of hydrogen bonding units in an ABA-type triblock copolymer. The A blocks form hard domains with dense crosslinking that prevents macroscopic deformation, while the B blocks form a softer matrix with sparse and dynamic crosslinks that serve as sacrificial bonds. This elastomer exhibits high toughness (≈62 MJ m−3), self-healing, and most notably, excellent self-recovery (recovery against 650% elongation and 17 MPa tensile stress with a dissipated energy >27 MJ m−3 at room temperature). This combination of toughness, self-healing, and self-recovery expands the range of applications of these advanced dynamic materials. Polymers with toughness and excellent self-recoverability are achieved by a bioinspired microphase-separated structure with different physical crosslink densities. This structure is realized by a carefully designed comonomer sequence distribution of an ABA type triblock copolymer where the A and B blocks contain high and low amount of quadruple hydrogen-bonding 2-ureido-4[1H]-pyrimidinone groups, respectively.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/adfm.201701670

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