Effect of the content and strength of hard segment on the viscoelasticity of the polyurethane elastomer: insights from molecular dynamics simulation

Due to the wide application, it is very crucial to understand the viscoelasticity of the polyurethane elastomer (PU, denoted by soft-hard block copolymer), which contains the soft segments (SS) and hard segments (HS). Thus, in this work, the effect of the content and strength of HS on the viscoelasticity of PU is explored in detail by adopting a coarse-grained model. First, the phase morphology of PU is characterized where both the single continuous phase and the bicontinuous phase are observed by varying the content of HS. Then, the viscoelasticity of PU is calculated by analyzing the storage modulus, the loss modulus, and the loss factor, which depends on the content and strength of HS. To further elucidate the mechanism for the storage modulus, the normalized interaction energy, the order parameter, and the formation probability of the HS or SS phase are characterized with the shear strain amplitude, which reflects the deformation of the phase structure. Then, the energy dissipation is quantified, which can rationalize the loss modulus well. A parameter is introduced, which considers the relative slippage and the content of HS or SS. It can explain the change in the loss factor with the content and strength of HS. In summary, this work can help to further understand how the content and strength of hard segments affect the viscoelasticity of the soft-hard block PU and structure evolution at the molecular level.