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doi: 10.1038/nature11409¡¡

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Nature | Letter

Highly stretchable and tough hydrogels
Jeong-Yun Sun,1, 2 Xuanhe Zhao,3 Widusha R. K. Illeperuma,1 Ovijit Chaudhuri,1 Kyu Hwan Oh,2 David J. Mooney,1, 4 Joost J. Vlassak1 & Zhigang Suo1, 5
Affiliations Contributions Corresponding author Journal name:
Nature
Volume:
489,
Pages:
133¨C136
Date published:
(06 September 2012)
DOI:
doi:10.1038/nature11409
Received 16 February 2012 Accepted 10 July 2012 Published online 05 September 2012

Hydrogels are used as scaffolds for tissue engineering1, vehicles for drug delivery2, actuators for optics and fluidics3, and model extracellular matrices for biological studies4. The scope of hydrogel applications, however, is often severely limited by their mechanical behaviour5. Most hydrogels do not exhibit high stretchability; for example, an alginate hydrogel ruptures when stretched to about 1.2 times its original length. Some synthetic elastic hydrogels6, 7 have achieved stretches in the range 10¨C20, but these values are markedly reduced in samples containing notches. Most hydrogels are brittle, with fracture energies of about 10 J m−2 (ref. 8), as compared with ~1,000 J m−2 for cartilage9 and ~10,000 J m−2 for natural rubbers10. Intense efforts are devoted to synthesizing hydrogels with improved mechanical properties11, 12, 13, 14, 15, 16, 17, 18; certain synthetic gels have reached fracture energies of 100¨C1,000 J m−2 (refs 11, 14, 17). Here we report the synthesis of hydrogels from polymers forming ionically and covalently crosslinked networks. Although such gels contain ~90% water, they can be stretched beyond 20 times their initial length, and have fracture energies of ~9,000 J m−2. Even for samples containing notches, a stretch of 17 is demonstrated. We attribute the gels¡¯ toughness to the synergy of two mechanisms: crack bridging by the network of covalent crosslinks, and hysteresis by unzipping the network of ionic crosslinks. Furthermore, the network of covalent crosslinks preserves the memory of the initial state, so that much of the large deformation is removed on unloading. The unzipped ionic crosslinks cause internal damage, which heals by re-zipping. These gels may serve as model systems to explore mechanisms of deformation and energy dissipation, and expand the scope of hydrogel applications.
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