Toughening hydrogels through force-triggered chemical reactions that lengthen polymer strands. 2021

Zi Wang, and Xujun Zheng, and Tetsu Ouchi, and Tatiana B Kouznetsova, and Haley K Beech, and Sarah Av-Ron, and Takahiro Matsuda, and Brandon H Bowser, and Shu Wang, and Jeremiah A Johnson, and Julia A Kalow, and Bradley D Olsen, and Jian Ping Gong, and Michael Rubinstein, and Stephen L Craig
Department of Chemistry, Duke University, Durham, NC, USA.

The utility and lifetime of materials made from polymer networks, including hydrogels, depend on their capacity to stretch and resist tearing. In gels and elastomers, those mechanical properties are often limited by the covalent chemical structure of the polymer strands between cross-links, which is typically fixed during the material synthesis. We report polymer networks in which the constituent strands lengthen through force-coupled reactions that are triggered as the strands reach their nominal breaking point. In comparison with networks made from analogous control strands, reactive strand extensions of up to 40% lead to hydrogels that stretch 40 to 50% further and exhibit tear energies that are twice as large. The enhancements are synergistic with those provided by double-network architectures and complement other existing toughening strategies.

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