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

Zhang, Zhen; Luo, Jiancheng; Zhao, Sheng; Ge, Sirui; Carrillo, Jan-Michael Y.; Keum, Jong K.; Do, Changwoo; Cheng, Shiwang; Wang, Yangyang; Sokolov, Alexei P.; Cao, Peng-Fei

doi:10.1016/j.matt.2021.11.007

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

Journal Article · 04 January 2022 · Matter (Online)

DOI: https://doi.org/10.1016/j.matt.2021.11.007 · OSTI ID:1838960

Zhang, Zhen ^[1]; Luo, Jiancheng ^[1]; Zhao, Sheng ^[2];

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^[5]; Cheng, Shiwang ^[6];

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS) & Neutron Scattering Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Michigan State Univ., East Lansing, MI (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States)

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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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1838960

Journal Information:: Matter (Online), Journal Name: Matter (Online) Journal Issue: 1 Vol. 5; ISSN 2590-2385

Publisher:: Cell Press/ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
elastomers
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Title: Surpassing the stiffness-extensibility trade-off of elastomers via mastering the hydrogen-bonding clusters

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