The development of self-healing polymers can extend the service life of polymer materials. However, it is still a challenge to prepare a polyurethane with high healing efficiency and maximum retention of the properties of polyurethane itself. In this research, we proposed a new scheme for the industrial production of self-healing polyurethane and successfully synthesized a self-healing polyurethane using diacetyl oxime as the chain extender and triethanolamine as the cross-linking agent. Oximeblocked isocyanates deblock at a higher temperature and regenerate oxime urethanes at a lower temperature, thereby achieving thermal reversibility and self-healing due to the concise and efficient thermal reversible reaction of oxime urethanes. Fourier transform infrared and differential scanning calorimetry experiments confirmed that the oxime urethanes in the polyurethane deblock efficiently at around 90 °C and re-block after the temperature is lowered. The process can be cycled at least three times. Microscopic observation confirmed that the cracks disappeared within 60−90 min at 90 °C. The tensile test shows that the synthetic DiO-c-PU has a self-healing efficiency of over 94% at 90 °C for 1.5 h, which is more efficient. From the results, it appears that DiO-c-PU has good self-healing properties.
Increasing the molecular weight of polyurethanes (PU) is an effective way to improve its mechanical properties, while, it is at the expense of sacrificing processability. Congruent modification in both mechanical and processing performances is still a challenge. Here, bis‐phenol‐A (BPA) derivatives, including tetrachlorobisphenol‐A and tetrabromobisphenol‐A, were chosen as the extender to synthesize thermoplastic PUs (TPU) containing blocked isocyanate units. This blocked isocyanate has a temperature‐responsive reversible reaction due to phenol urethane bonds, so as to ensure the good mechanical properties at the service temperature and better processing performance via deblocking into smaller molecular weight at the processing temperature; in addition, negative induction effect of the halogen substituents endow BPA derivatives with deblocking reaction at lower temperature. The experimental results confirmed that the blocking reaction carried out completely at 70°C, and accompanying by the dramatical increase of molecular weight. The obvious deblocking reaction happened at 140°C, where the average molecular weight of TPUs decreased from 22,600 g/mol to 13,690 g/mol. Meanwhile, the melt flow index increased significantly with the extension of heating time, indicating that the PU has good processing properties. After the deblocking and re‐blocking reactions were repeated alternatively, there is almost no change in its tensile properties, molecular weight and melt outflow index within two cycles under air atmosphere. This article proposes a strategy of congruent modification in both mechanical and processing performances of TPU.
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