Designing multiple-shape memory polymers with miscible polymer blends: Evidence and origins of a triple-shape memory effect for miscible PLLA/PMMA blends
Abstract
Shape memory properties of polymers represent one of the most expanding fields in polymer science related to numerous smart applications. Recently, multiple-shape memory polymers (multiple-SMPs) have attracted significant attention and can be achieved with complex polymer architectures. Here, miscible PLLA/PMMA blends with broad glass transitions are investigated as an alternative platform to design multiple-SMPs. Dual-shape memory experiments were first conducted at different stretching temperatures to identify the so-called “temperature memory effect”. The switch temperature of the symmetric 50% PLLA/50% PMMA blend smoothly shifted from 70 to 90 °C for stretching temperatures increasing from 65 to 94 °C, attesting for a significant “temperature memory effect”. Asymmetric formulations with 30% and 80% PMMA also present a “temperature memory effect”, but the symmetric blend clearly appeared as the most efficient formulation for multiple-shape memory applications. A programming step designed with two successive stretchings within the broad glass transition consequently afforded high triple-shape memory performances with tunable intermediate shapes, demonstrating that the symmetric blend could represent an interesting candidate for future developments. Advanced shape recovery processes are consistent with a selective activation of specific “soft domains” or nanodomains arising from the broad glass transition and the large distribution of relaxation time observed by DSC and dielectric spectroscopy. Polarized IR measurements pointed out that the composition of activated/oriented “soft domains” could vary with stretching temperature, giving rise to the “temperature-memory effect”. Consequently, from a polymer physics standpoint, nanoscale compositional heterogeneities within the symmetric blend could be suspected and discussed on the basis of available models for miscible blends and for multiple-SMPs.
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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 [88]
PLLA/PMMA blends processed by twin-screw mini-extruder showed a unique and broad Tg, especially for the 50%/50% blend.
“Indeed, PLLA/PMMA blends processed by twin-screw mini-extruder showed a unique and broad Tg, especially for the 50%/50% blend.”
From Shape-memory polymers for multiple applications in the materials world (2016) · cites this paper as [83]
A recent work from our group investigated m-SME in miscible polymer pairs with a broad Tg.
“Finally, a recent work from our group investigated m-SME in miscible polymer pairs with a broad Tg [83].”
From Shape-memory polymers for multiple applications in the materials world (2016) · cites this paper as [83]
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- Authors
- Samuel, C., Barrau, S., Lefebvre, J.-M., Raquez, J.-M., & Dubois, P.
- Affiliations
- University of Mons (BE)
- Centre National de la Recherche Scientifique (FR)
- Laboratory of Polymeric and Composite Materials (LPCM), Center of Innovation and Research in Materials and Polymers (CIRMAP), University of Mons - UMONS, Place du Parc 23, B-7000 Mons, Belgium
- Corresponding author
- Samuel, Cédric
- Venue
- Macromolecules
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-09-17
- Volume
- 47
- Issue
- 19
- Pages
- 6791-6803
- ISSN
- 0024-9297 (ISSN-L)
- 1520-5835
- OpenAlex
- W2067262806
- Cited by
- 175
- References
- 46
- Citations by year
- 2026: 7 · 2025: 12 · 2024: 10 · 2023: 10 · 2022: 17 · 2021: 16 · 2020: 19 · 2019: 22 · 2018: 14 · 2017: 14 · 2016: 18 · 2015: 16
- FWCI
- 11.18
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Macromolecules (publishedVersion)
- PolyPublie (École Polytechnique de Montréal) (submittedVersion)
- Funders
- European Commission
- Fonds De La Recherche Scientifique - FNRS
- Fonds de la Recherche Fondamentale Collective
- 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 › Materials Chemistry › Material Dynamics and Properties
- Keywords
- triple shape memory effect, miscible polymer blends, temperature memory effect, nanodomains, distribution of relaxation times, shape recovery, polymer nanocomposites
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