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Effect of thermal annealing on cold crystallization ability of thermoset polyurethane elastomer synthesized from fully bio-derived polyol

Jaeheon Lee, Jung Hyeun Kim*

https://doi.org/10.1016/j.cjsc.2025.100568

ABSTRACT

Bio-polyol is considered as a core material to synthesize eco-friendly polyurethane products. However, one of the popular bio-polyols, polytrimethylene ether glycol (PO3G), is reluctant to crystallize and therefore exhibits a cold crystallization behavior. This abnormal behavior causes unstable mechanical properties at low-temperature and limits its applications in shape memory devices where crystallization is an essential mechanism. To analyze the unusual phenomenon, we compared different ether polyols focusing on symmetry characteristics and the even-odd effect of carbon backbones. It is found that PO3G has a slow crystallization rate because its ether linkages require specific chain arrangement for attractive interactions. Consequently, a thermal learning mechanism is developed to restore the normal crystallization behavior of elastomers synthesized from the bio-polyol. Repetitive heating and cooling cycles with high-temperature annealing induce urethane exchange reaction and reconstruct the chain orientations for fast crystallization. Results suggest the degree of crystallizations in polyurethane elastomer can be precisely controlled by introducing repetitive thermal treatments to enhance the potential applications of bio-polyols in the polymer industries.

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