Triple-shape memory polymers based on self-complementary hydrogen bonding
Open accessAbstract
Triple shape memory polymers (TSMPs) are a growing subset of a class of smart materials known as shape memory polymers, which are capable of changing shape and stiffness in response to a stimulus. A TSMP can change shapes twice and can fix two metastable shapes in addition to its permanent shape. In this work, a novel TSMP system comprised of both permanent covalent cross-links and supramolecular hydrogen bonding cross-links has been synthesized via a one-pot method. Triple shape properties arise from the combination of the glass transition of (meth)acrylate copolymers and the dissociation of self-complementary hydrogen bonding moieties, enabling broad and independent control of both glass transition temperature (T(g)) and cross-link density. Specifically, ureidopyrimidone methacrylate and a novel monomer, ureidopyrimidone acrylate, were copolymerized with various alkyl acrylates and bisphenol A ethoxylate diacrylate. Control of T(g) from 0 to 60 °C is demonstrated: concentration of hydrogen bonding moieties is varied from 0 to 40 wt %; concentration of the diacrylate is varied from 0 to 30 wt %. Toughness ranges from 0.06 to 0.14 MPa and is found to peak near 20 wt % of the supramolecular cross-linker. A widely tunable class of amorphous triple-shape memory polymers has been developed and characterized through dynamic and quasi-static thermomechanical testing to gain insights into the dynamics of supramolecular networks.
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The temperature-memory effect approach has been largely employed to achieve multiple-way SMPs with a broad glass transition or a broad melting transition as the switching transition.
“Such an approach has been largely employed to achieve multiple-way SMPs with a broad glass transition [82-92] and a broad melting transition [93-95] as the switching transition.”
From Two-Way and Multiple-Way Shape Memory Polymers for Soft Robotics: An Overview (2020) · cites this paper as [87]
The Introduction (page unavailable) discusses multiple-shape memory and mentions a broad-transition example. But the Conclusions describe this paper’s own triple-shape system as using a glass transition together with hydrogen-bond dissociation—not a broad glass transition as the switching transition. The paper therefore supports the general multiple-shape context, but not the claimed approach for this system. (LLM, conf=0.85)
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- Authors
- Ware, T., Hearon, K., Lonnecker, A., Wooley, K. L., Maitland, D. J., & Voit, W.
- Affiliations
- The University of Texas at Dallas (US)
- Texas A&M University (US)
- Corresponding author
- Voit, Walter
- Venue
- Macromolecules
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-01-06
- Volume
- 45
- Issue
- 2
- Pages
- 1062-1069
- ISSN
- 0024-9297 (ISSN-L)
- 1520-5835
- PMC
- PMC3265144
- OpenAlex
- W1986132969
- Cited by
- 192
- References
- 29
- Citations by year
- 2026: 3 · 2025: 6 · 2024: 4 · 2023: 12 · 2022: 8 · 2021: 10 · 2020: 18 · 2019: 19 · 2018: 13 · 2017: 22 · 2016: 16 · 2015: 16 · 2014: 16 · 2013: 20 · 2012: 8
- FWCI
- 15.08
- Type
- journal article
- Language
- en
- Open access
- green
- www.ncbi.nlm.nih.gov
- Locations
- Macromolecules (publishedVersion)
- PubMed (publishedVersion)
- Europe PMC (PubMed Central) (acceptedVersion)
- PubMed Central (acceptedVersion)
- Funders
- National Institute of Biomedical Imaging and Bioengineering (R01EB000462)
- Topics
- Physical Sciences › Materials Science › Polymers and Plastics › Polymer composites and self-healing
- Physical Sciences › Engineering › Mechanical Engineering › Advanced Materials and Mechanics
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Medicine › Hydrogels: synthesis, properties, applications
- Keywords
- supramolecular cross-linking, crosslink density, amorphous polymers, toughening, thermomechanical behavior
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