Effects of physical aging on the self‐healing, shape memory, and crystallization behaviors of hydrogen‐bonded supramolecular polymers

Abstract Despite the profusion of studies on synthesis, structure, and properties of supramolecular polymers (SMPs), physical aging, and its effects on properties of SMPs have been rarely described in the literature. In this study, SMPs was synthesized by end‐functionalized with 2‐ureido‐4[1H]‐pyrimidione (UPy) to triblock oligomers with soft poly(butylene) segments and hard poly ( l ‐lactic acid) blocks. Effects of physical aging on thermal, self‐healing properties, shape memory, as well as mechanical properties before and after repair of such SMPs have been studied. The self‐healing efficiency of SMPs increased considerably after physical aging process. After being aged at 33 °C for 120 h, light healable SMPs with a self‐healing efficiency of 100% can be achieved, as compared to the unaged SMPs of 50%. Moreover, it was found that the strength, modulus, and toughness of SMPs decreased gradually during the physical aging; on the contrary, the recovery of strength, modulus, and toughness after repair increased dramatically. The shape recovery speed and shape memory capability of SMPs can also be facilitated by extension of aging time.