When polymer composites containing magnetic nanoparticles (MNPs) are exposed to an alternating magnetic field, heat is generated to melt the surrounding polymer locally, partially filling voids across any cracks or deformities. Such materials are of interest for structural applications; however, structural polymers with high melting temperatures pose the challenge of generating high localised temperatures enabling self-healing. A method to prepare a multiferroic-Polyamide 6 (PA6) nanocomposite with tuneable magnetocaloric properties is reported. Tunability arises from varying the MNP material (and any coating, its dispersion, and agglomerate sizes in the nanocomposite). The superparamagnetic MNPs (SMNPs) and iron oxide MNPs with and without surface functionalization were dispersed into PA6 through in situ polymerization, and their magnetic properties were compared. Furthermore, computer simulations were used to quantify the dispersion state of MNPs and assess the influence of the interaction radius on the magnetic response of the self-healable magnetic nanoparticle polymer (SHMNP) composite. It was shown that maintaining the low interaction radius through the dispersion of the low coercivity MNPs could allow tuning of the bulk magnetocaloric properties of the resulting mesostructures. An in-situ polymerization method improved the dispersion and reduced the maximum interaction radius value from ca. 806 to 371 nm and increased the magnetic response for the silica-coated SMNP composite. This sample displayed ca. three orders of magnitude enhancement for magnetic saturation compared to the unfunctionalized Fe3O4 MNP composite.
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