Toughening elastomers using mussel-inspired iron-catechol complexes

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Science  27 Oct 2017:
Vol. 358, Issue 6362, pp. 502-505
DOI: 10.1126/science.aao0350

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Combining stiffness and stretchiness

There is usually a trade-off between making a material stretchy, so that it can absorb energy on deformation, and making a material stiff, so that it does not extend very much when stretched. Mussels have long been an inspiration for developing adhesives that work when wet. Filippidi et al. produced an extensible polymeric material containing catechol groups whose mechanical properties were augmented when dry through the addition of iron ions (see the Perspective by Winey). The iron ions lead to sacrificial metal coordination bonds, creating a reversible load-bearing network that does not trade extensibility for stiffness.

Science, this issue p. 502; see also p. 449


Materials often exhibit a trade-off between stiffness and extensibility; for example, strengthening elastomers by increasing their cross-link density leads to embrittlement and decreased toughness. Inspired by cuticles of marine mussel byssi, we circumvent this inherent trade-off by incorporating sacrificial, reversible iron-catechol cross-links into a dry, loosely cross-linked epoxy network. The iron-containing network exhibits two to three orders of magnitude increases in stiffness, tensile strength, and tensile toughness compared to its iron-free precursor while gaining recoverable hysteretic energy dissipation and maintaining its original extensibility. Compared to previous realizations of this chemistry in hydrogels, the dry nature of the network enables larger property enhancement owing to the cooperative effects of both the increased cross-link density given by the reversible iron-catecholate complexes and the chain-restricting ionomeric nanodomains that they form.

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