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Surpassing the stiffness-extensibility trade-off of elastomers via mastering the hydrogen-bonding clusters...

Publication Type
Journal Name
Advances in Condensed Matter Physics
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1 to 1

The current paradigm of elastomer design typically falls into the trade-off between stiffness and extensibility. With a few reports on circumventing this trade-off behavior, e.g. increasing Young’s modulus without sacrificing extensibility, the design principles to achieve improvements in both stiffness and extensibility have rarely been demonstrated. Herein, with a model system, i.e., crosslinked polydimethylsiloxane (PDMS) network, we demonstrate two approaches that can surpass the stiffness-extensibility trade-off and provide significant improvement in both parameters. Such an achievement is realized by introducing rationally arranged hydrogen-bonding units, i.e., ureidopyrimidone (UPy), leading to simultaneously improved Young’s modulus and extensibility up to 158 and 3 times, respectively. Based on the experimental results, we also propose a microscopic picture of network rearrangement during the stretching process. Moreover, using this picture we further improved Young’s modulus of the elastic network without affecting its extensibility through mastering the distribution/topology of UPy clusters.