Two-Way Reversible Shape Memory in a Semicrystalline Network
Abstract
Cooling-induced crystallization of cross-linked poly(cyclooctene) films under a tensile load results in significant elongation and subsequent heating to melt the network reverses this elongation (contracting), yielding a net two-way shape memory (2W-SM) effect. The influence of cross-linking density on the thermal transitions, mechanical properties, and the related 2W-SM effect was studied by varying the concentration of cross-linking agent dicumyl peroxide (DCP) and using differential scanning calorimetry (DSC), gel fraction measurements, dynamic mechanical analysis (DMA), and customized 2W-SM analysis. The latter showed that there is crystallization-induced elongation on cooling and melting-induced shrinkage on heating (2W-SM), with lower cross-link density leading to higher elongation at the same applied stress. For a given cross-link density, however, increasing the tensile stress applied during cooling resulted in greater stress-induced crystallization. We further observed that the onset temperatures for elongation on cooling ( T c ) and contraction on heating ( T m ) shifted to higher temperatures with decreasing cross-link density. Similarly, the degree of molecular orientation achieved upon deformation was found to increase with decreasing cross-link density. The impact of stress on the 2W-SM effect was examined using wide-angle X-ray diffraction (WAXD), revealing a transition from bimodal to unimodal orientation. As the crystalline structure evolves from bimodal (low stress) to unimodal (high stress), the crystallization occurs along a single preferred orientation thus inducing greater elongation along the stretching direction. We anticipate that the observed 2W-SM property in a semicrystalline network will enable applications heretofore possible only with costly shape memory alloys and liquid crystalline elastomers.
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PEG-2 before isomerization shows reversible shape memory performance when temperature is switched between −20 and 80 °C, with 20% reversible strain under a constant stress of 0.8 MPa.
“PEG-2 (before isomerization) shows reversible shape memory performance32 when the temperature is switched between −20 and 80 °C, with 20% reversible strain under a constant stress of 0.8 MPa (Fig. 4a).”
From On demand shape memory polymer via light regulated topological defects in a dynamic covalent network (2020) · cites this paper as [32]
Once the working temperature during cooling reached the PCO crystallization temperature, a significant increase in strain was observed revealing a potential 2W-SME.
“Once the working temperature during the cooling step reached the PCO crystallization temperature, a significant increase in strain was observed revealing a potential 2W-SME.”
From Shape-memory polymers for multiple applications in the materials world (2016) · cites this paper as [86]
Permanent systems such as crosslinked semi-crystalline polymers, nematic liquid-crystalline elastomers, and glass-forming polydomain nematic networks open the door to the design of polymeric actuators.
“It has been reported that permanent systems, such as crosslinked semi-crystalline polymers [84-86], nematic liquid-crystalline elastomers [87], and glass-forming polydomain nematic networks [88], open the door to the design of polymeric actuators.”
From Shape-memory polymers for multiple applications in the materials world (2016) · cites this paper as [86]
When the sample is heated upon constant stress, a tensile contraction of PCO appeared responsible for recovery of shape similar to the one observed before crystallization.
“In the case when the sample is heated upon constant stress, a tensile contraction of the PCO appeared responsible for the recovery of shape similar to the one observed before crystallization.”
From Shape-memory polymers for multiple applications in the materials world (2016) · cites this paper as [86]
In 2008 Chung et al. unexpectedly discovered 2W-SME in poly(cyclooctene) (PCO) films covalently cross-linked by dicumyl peroxide.
“In 2008 Chung et al. unexpectedly discovered such behavior in poly(cyclooctene) (PCO) films covalently cross-linked by dicumyl peroxide [86].”
From Shape-memory polymers for multiple applications in the materials world (2016) · cites this paper as [86]
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- Authors
- Chung, T., Romo-Uribe, A., & Mather, P. T.
- Affiliations
- Case Western Reserve University (US)
- Department of Macromolecular Science and Engineering, Case Western Reserve University, 2100 Adelbert Road, Cleveland, Ohio 44106, and Instituto de Ciencias Fisicas, Universidad Nacional Autonoma de Mexico Cuernavaca, Morelos 62210, Mexico
- Corresponding author
- Mather, Patrick T.
- ORCID
- Mather, Patrick T.
- Venue
- Macromolecules
- Publisher
- American Chemical Society (ACS)
- Published
- 2007-12-13
- Volume
- 41
- Issue
- 1
- Pages
- 184-192
- ISSN
- 0024-9297 (ISSN-L)
- 1520-5835
- OpenAlex
- W2124046972
- Cited by
- 531
- References
- 27
- Citations by year
- 2026: 19 · 2025: 23 · 2024: 27 · 2023: 29 · 2022: 39 · 2021: 31 · 2020: 49 · 2019: 40 · 2018: 32 · 2017: 34 · 2016: 30 · 2015: 32 · 2014: 34 · 2013: 27 · 2012: 19
- FWCI
- 11.79
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Macromolecules (publishedVersion)
- Funders
- Division of Materials Research
- Topics
- Physical Sciences › Materials Science › Polymers and Plastics › Polymer composites and self-healing
- Physical Sciences › Engineering › Mechanical Engineering › Advanced Materials and Mechanics
- Physical Sciences › Materials Science › Polymers and Plastics › Polymer crystallization and properties
- Keywords
- two-way shape memory effect, cross-linked polymer films, stress-induced crystallization, crosslink density, dicumyl peroxide, molecular orientation, polymer crystallization, shape memory polymers
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