A Thermoplastic/Thermoset Blend Exhibiting Thermal Mending and Reversible Adhesion
Abstract
In this paper, we report on the development of a new and broadly applicable strategy to produce thermally mendable polymeric materials, demonstrated with an epoxy/poly(-caprolactone) (PCL) phase-separated blend. The initially miscible blend composed of 15.5 wt % PCL undergoes polymerization-induced phase separation during cross-linking of the epoxy, yielding a "bricks and mortar" morphology wherein the epoxy phase exists as interconnected spheres (bricks) interpenetrated with a percolating PCL matrix (mortar). The fully cured material is stiff, strong, and durable. A heating-induced "bleeding" behavior was witnessed in the form of spontaneous wetting of all free surfaces by the molten PCL phase, and this bleeding is capable of repairing damage by crack-wicking and subsequent recrystallization with only minor concomitant softening during that process. The observed bleeding is attributed to volumetric thermal expansion of PCL above its melting point in excess of epoxy brick expansion, which we term differential expansive bleeding (DEB). In controlled thermal-mending experiments, heating of a cracked specimen led to PCL extrusion from the bulk to yield a liquid layer bridging the crack gap. Upon cooling, a "scar" composed of PCL crystals formed at the site of the crack, restoring a significant portion of the mechanical strength. When a moderate force was applied to assist crack closure, thermal-mending efficiencies exceeded 100%. We further observed that the DEB phenomenon enables strong and facile adhesion of the same material to itself and to a variety of materials, without any requirement for macroscopic softening or flow.
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In each study, authors observed PCL filled cracks due to thermal expansion, different from composite.
“In each study, the authors observed that the PCL filled the cracks due to its thermal expansion, which is different from that of the composite.”
From Modeling of the Healing Process of Polycaprolactone‐Interleaved Carbon Fiber–Reinforced Composites (2025) · cites this paper as [22]
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 [521]
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 [521]
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- Authors
- Luo, X., Ou, R., Eberly, D. E., Singhal, A., Viratyaporn, W., & Mather, P. T.
- Affiliations
- Rutgers, The State University of New Jersey (US)
- Corresponding author
- Mather, Patrick T.
- Venue
- ACS Applied Materials & Interfaces
- Publisher
- American Chemical Society (ACS)
- Published
- 2009-02-11
- Volume
- 1
- Issue
- 3
- Pages
- 612-620
- ISSN
- 1944-8244 (ISSN-L)
- 1944-8252
- OpenAlex
- W2104739711
- Cited by
- 205
- References
- 40
- Citations by year
- 2026: 6 · 2025: 9 · 2024: 16 · 2023: 9 · 2022: 9 · 2021: 18 · 2020: 21 · 2019: 11 · 2018: 13 · 2017: 10 · 2016: 19 · 2015: 14 · 2014: 10 · 2013: 11 · 2012: 12
- FWCI
- 8.14
- 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 › Engineering › Mechanical Engineering › Epoxy Resin Curing Processes
- Physical Sciences › Materials Science › Polymers and Plastics › Polymer crystallization and properties
- Keywords
- polymerization-induced phase separation, crack repair, reversible adhesion, thermal expansion mismatch, self-healing materials
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