Abstract
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.
| Original language | English |
|---|---|
| Pages (from-to) | 237-252 |
| Number of pages | 16 |
| Journal | Matter |
| Volume | 5 |
| Issue number | 1 |
| DOIs | |
| State | Published - Jan 5 2022 |
Funding
This manuscript has been authored by UT-Battelle under contract no. DE-AC05-00OR22725 with the US Department of Energy. The United States Government retains (and the publisher, by accepting the article for publication, acknowledges that the United States Government retains) a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This research at the Oak Ridge National Laboratory, managed by UT-Battelle for the US Department of Energy (DOE) under contract no. DE-AC05-00OR22725, was sponsored by the Laboratory Directed Research and Development Program at Oak Ridge National Laboratory. A.P.S. also acknowledges partial financial support by the DOE, Office of Science, Basic Energy Science, Material Science, and Engineering Division. The computational/simulation aspect of this work was performed at the Center for Nanophase Materials Sciences, a DOE Office of Science User Facility. This research used resources at the SNS and OLCF, DOE Office of Science User Facilities operated by the Oak Ridge National Laboratory. P.-F.C. conceived the idea. P.-F.C. and Z.Z. designed the experiments. Z.Z. carried out the experiments. Z.Z. S.Z. S.G. and J.L. performed the characterizations. J.-M.Y.C. performed and analyzed the simulations. J.K. K. and C.D. performed the SAXS and SANS studies. S.C. and Y.W. contributed to rheology studies. A.S. contributed to the discussion. Z.Z. wrote the manuscript and P.-F.C. revised the manuscript. All authors read and edited the manuscript. The authors declare no competing interests. This research at the Oak Ridge National Laboratory, managed by UT-Battelle for the US Department of Energy (DOE) under contract no. DE-AC05-00OR22725 , was sponsored by the Laboratory Directed Research and Development Program at Oak Ridge National Laboratory . A.P.S. also acknowledges partial financial support by the DOE , Office of Science, Basic Energy Science, Material Science, and Engineering Division. The computational/simulation aspect of this work was performed at the Center for Nanophase Materials Sciences , a DOE Office of Science User Facility. This research used resources at the SNS and OLCF, DOE Office of Science User Facilities operated by the Oak Ridge National Laboratory. This manuscript has been authored by UT-Battelle under contract no. DE-AC05-00OR22725 with the US Department of Energy. The United States Government retains (and the publisher, by accepting the article for publication, acknowledges that the United States Government retains) a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).
| Funders | Funder number |
|---|---|
| Basic Energy Science, Material Science | |
| DOE Public Access Plan | |
| United States Government retains | |
| U.S. Department of Energy | DE-AC05-00OR22725 |
| Office of Science | |
| Oak Ridge National Laboratory | |
| UT-Battelle |
Keywords
- MAP3: Understanding
- elastomers
- hydrogen-bonding clusters
- interpenetrated network
- microscopic dynamic picture
- poly(dimethylsiloxane) network
- stiffness-extensibility trade-off
- ureidopyrimidone (UPy)