Two new thermoresponsive self‐healing polyurethanes (1DA1T and 1.5DA1T) based on the Diels–Alder (DA) reaction between furan and maleimide moieties are developed that use the shape‐memory effect to bring crack faces into intimate contact such that healing can take place. Unlike other self‐healing polymers, these polymers do not require external forces to close cracks but rather they use the shape‐memory effect to autonomously close the crack. Both polyurethanes have a stable polymer structure and comparable mechanical properties to commercial epoxies. A differential scanning calorimeter is employed to check the glass transition temperature of the polymers as well as the DA and retro‐DA (rDA) reaction temperatures. These DA and rDA reactions are confirmed with variable‐temperature proton nuclear magnetic resonance. Healing efficiency is calculated using a measurement of the failure load from compact tension testing. The results show that the shape‐memory effect can replace external forces to close two crack surfaces and the DA reaction can be repeatedly employed to heal the cracks.
On page 5261, Heo and Sodano report new thermo‐responsive self‐healing polyurethanes that use the shape memory effect to bring the crack faces into intimate contact, such that healing can take place, thus eliminating the need for an external force to close the crack. The image shows the specimen before and after healing, demonstrating the reformation of the polymer, which can be done repeatably.
Thermally responsive self-healing polyurethanes (1DA1T, 1.5DA1T, and 2DA1H) with shape memory property were developed and the fully reversible Diels-Alder (DA) and retro Diels-Alder (rDA) reactions were employed for the healing mechanism. The transition temperatures of the DA and rDA reactions were confirmed through a differential scanning calorimetry and the molecular level of analysis on the reversibility and the repeatability between the DA and rDA reactions were completed though a variable temperature proton nuclear magnetic resonance at the reaction temperatures. Also, compact tension specimens were made to observe the healing efficiencies. These specimens were healed without the use of external forces to close the crack surfaces after testing for the repeatable healing ability with three cycles. As a result, the average first healing cycle efficiencies of 80%, 84%, and 96% for 1DA1T, 1.5DA1T and 2DA1H, respectively, were achieved and small drops for the second and third healing cycles were observed. Then, using two of the self-healing polyurethanes as resins, continuous carbon fiber fabric reinforced polymer matrix composites (C1.5DA1T and C2DA1H) were fabricated and short beam shear testing was conducted to determine the healing capability on the delamination. Accordingly, the first healing efficiencies of 88% and 85% were measured without any additional treatments on the fibers; however, an external pressure was applied during the composite healing process.
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