Preparation and Properties of Natural Rubber (NR)/Polycaprolactone (PCL) Bio-Based Shape Memory Polymer Blends

Shape memory NR/PCL bio-based blends, where NR served as the reversible phase and PCL served as the switching phase, were prepared using a melt blending process. Peroxide, besides its role as a cross-linking agent to NR, was used to enhance the compatibility between NR and PCL, which was confirmed via Fourier transform infrared spectra and scanning electron microscopy analyses. With increasing peroxide content, the tensile strength increased steadily with decreasing PCL contents, up to 12.3 ± 0.8 MPa for the NR/PCL (70/30) blend at 2 phr peroxide. The shape fixing ratio decreased slightly with increasing peroxide content, especially for high NR content. The values of the shape recovery ratio were high, up to 100%, regardless of PCL content. The recovery stress was found to reach its maximum value around 60°C. In order to consider both fixing ratio (R_f) and recovery ratio (R_r) together, an additional denotation of shape memory index, R_fR_r, coupling both ratios by the product of the fixing ratio and recovery ratio, is proposed. The shape memory index (R_fR_r) reached values close to 100%, at the NR/PCL composition of 50/50 and 70/30; in particular, the highest value was for the 50/50 case regardless of peroxide concentration. The shape recovery ratio and fixing ratio remained largely unchanged even after 30 cycles of deformation and recovery processes for a typical NR/PCL/DCP (30/70/0.5) blend which, thus, outperformed all known shape memory blends in the literature.