Thermo-sensitive multiphase polymer networks with triple-shape capability have been recently introduced as a new class of active polymers that can change on demand from a first shape A to a second shape B and from there to a permanent shape C. Such multiphase polymer networks consist of covalent cross-links that determine shape C and at least two phase-segregated domains with distinct thermal transitions T trans,A and T trans,B , that are associated to shape A and B. In general the application of a two step programming or a one step programming procedure is required for creation of triple-shape functionality. In this study we report about a series of CLEGC nanocomposites consisting of silica coated nanoparticles (SNP) incorporated in a multiphase graft polymer network matrix from crystallisable poly(ε-caprolactone) diisocyanatoethyl methacrylate (PCLDIMA) and poly(ethylene glycol) monomethyl ether monomethacrylate (PEGMA) forming crystallisable side chains. These CLEGC nanocomposites were designed to enabling non contact activation of triple-shape effect in alternating magnetic field. Composites with variable PCLDIMA content ranging from 30 wt-% and 70 wt-% and different SNP amounts (0 wt-%, 2.5 wt-%, 5 wt-% and 10 wt-%) were realized by thermally induced polymerization. The thermal and mechanical properties of the CLEG nanocomposites were explored by means of DSC, DMTA and tensile tests. The triple-shape properties were quantified in cyclic, thermomechanical experiments, which consisted of a two step programming procedure and a recovery module under stress-free conditions for recovery of shapes B and C. While the thermal properties and the Young’s modulus of the investigated polymer networks were found to be independent from the incorporated amount of SNP, the elongation at break (εB) decreases with increasing nanoparticle content. All investigated composites exhibit excellent triple-shape properties showing a well separated two step shape recovery process.
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