Journal
MATTER
Volume 5, Issue 1, Pages 237-+Publisher
CELL PRESS
DOI: 10.1016/j.matt.2021.11.007
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Funding
- US Department of Energy [DE-AC05-00OR22725]
- Laboratory Directed Research and Development Program at Oak Ridge National Laboratory [DE-AC05-00OR22725]
- DOE, Office of Science, Basic Energy Science, Material Science, and Engineering Division
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The current paradigm of elastomer design often faces a trade-off between stiffness and extensibility. However, this study demonstrates two approaches that can surpass this trade-off and provide significant improvements in both parameters by introducing rationally arranged hydrogen-bonding units.
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., cross-linked 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.
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