Linear/Network Poly(ε-caprolactone) Blends Exhibiting Shape Memory Assisted Self-Healing (SMASH)
Abstract
Self-healing (SH) polymers are responsive polymeric materials that can repair mechanical damage such as cracks in an autonomous fashion. In most SH polymers studies reported to date, crack closure was either unaddressed or achieved by manual intervention. Here, we report a new strategy that utilizes shape memory (SM) to prepare novel SH polymers that are capable of simultaneously closing and rebonding cracks with a simple thermal trigger. This strategy, termed "shape memory assisted self-healing (SMASH)", is demonstrated in a blend system consisting of cross-linked poly(ε-caprolactone) network (n-PCL) with linear poly(ε-caprolactone) (l-PCL) interpenetrating the network, and exhibits a combination of SM response from the network component and SH capacity from the linear component. Thermomechanical analysis revealed that the thermoset, n-PCL, demonstrates reversible plasticity -a form of shape memory where large plastic deformation at room temperature is fully recoverable upon heating. This SM action assists to close any cracks formed during deformation and/or damage while l-PCL chains tackify the crack surfaces by diffusion to the free surface and ultimately across the area of damage during the same heating step as used for SM. In our study, we investigated the controlled damage and SMASH healing of blends with varying composition using tensile testing of essential work of fracture film specimens. The healing component, l-PCL used had a high M(w) (M(w) ∼65k g/mol) to enable re-entanglement after diffusion across the interface while the shape memory component, n-PCL was prepared from PCL telechelic diacrylates and a tetrathiol cross-linker, yielding excellent shape memory. We found excellent self-healing of films by the SMASH mechanism, with near complete healing for l-PCL contents exceeding 25 wt %. Applications are envisioned in the area of self-healing bladders, inflated structure membranes, and architectural building envelopes.
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This system only works on microscopic damages and does not work on macroscopic damage such as macroscopic cracks because macroscopic crack may damage the recoverability of the polymer network.
“This system only works on microscopic damages [521,522] while not work on macroscopic damage such as macroscopic cracks because macroscopic crack may damage the recoverability of the polymer network [521,522].”
From A review of stimuli-responsive shape memory polymer composites (2013) · cites this paper as [522]
The shape memory epoxy healing system only works on microscopic damages and not on macroscopic damage such as macroscopic cracks because macroscopic crack may damage the recoverability of the polymer network.
“This system only works on microscopic damages [521,522] while not work on macroscopic damage such as macroscopic cracks because macroscopic crack may damage the recoverability of the polymer network [521,522].”
From A review of stimuli-responsive shape memory polymer composites (2013) · cites this paper as [522]
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- Authors
- Rodriguez, E. D., Luo, X., & Mather, P. T.
- Affiliations
- Syracuse University (US)
- Corresponding author
- Mather, Patrick T.
- ORCID
- Mather, Patrick T.
- Venue
- ACS Applied Materials & Interfaces
- Publisher
- American Chemical Society (ACS)
- Published
- 2011-01-21
- Volume
- 3
- Issue
- 2
- Pages
- 152-161
- ISSN
- 1944-8244 (ISSN-L)
- 1944-8252
- OpenAlex
- W1964617021
- Cited by
- 381
- References
- 37
- Citations by year
- 2026: 5 · 2025: 11 · 2024: 17 · 2023: 17 · 2022: 25 · 2021: 39 · 2020: 38 · 2019: 34 · 2018: 41 · 2017: 25 · 2016: 35 · 2015: 24 · 2014: 26 · 2013: 22 · 2012: 20
- FWCI
- 19.09
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- ACS Applied Materials & Interfaces (publishedVersion)
- PubMed (publishedVersion)
- Topics
- Physical Sciences › Materials Science › Polymers and Plastics › Polymer composites and self-healing
- Physical Sciences › Materials Science › Biomaterials › biodegradable polymer synthesis and properties
- Physical Sciences › Materials Science › Polymers and Plastics › Polymer crystallization and properties
- Keywords
- polycaprolactone, self-healing polymers, shape memory polymers, crack closure, crack healing, reversible plasticity, thermoset networks, molecular weight effects, essential work of fracture, self-healing films
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