Structure and stress relaxation in shape memory polymers (SMPs), which show the time-dependent response to temperature and mechanical loading, respectively, are usually thought to be the primary mechanisms of shape memory effects (SMEs). However, the synergistic effect of structure and stress relaxation has not been well investigated. What's more, convenient and economic manufacturing and structural customization of SMPs can be easily achieved by four-dimensional (4D) printing technology. Thus, in this paper, we comprehensively analyze the working mechanisms of synergistic-relaxation effects in both traditional and 4D-printed SMPs using theoretical calculations and experimental confirmation. Specifically, the calculations are based on the thermo-mechanical and electro-thermo-mechanical models, and multiple sets of experimental data are used to verify the model results. The model results agree well with the experimental data and demonstrate that synergistic-relaxation mechanisms play an important role in thermo-mechanical behaviors.
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