Magnetic Nanoparticles Improve Flow Rate and Enable Self-Healing in Covalent Adaptable Networks

Covalent adaptable networks (CANs) combine the mechanical and chemical stability of thermosets with the reprocessability of thermoplastics through the incorporation of stimuli-responsive dynamic crosslinks. To allow for processing through induction heating, we have created associative CANs that include fillers in the polymer matrix for efficient heat transfer. While the inclusion of inorganic fillers often decreases flow rate in CANs and complicates reprocessing of the material, the presence of Fe₃O₄ nanoparticles had no detrimental effect on flow behavior in a vinylogous urethane vitrimer, an observation we attribute to the catalytic nature of nanoparticles on the dynamic exchange chemistry. We employed two methods of nanoparticle incorporation: blending bare nanoparticles and crosslinking chemically modified nanoparticles. The vitrimers with covalently crosslinked nanoparticles exhibited a decreased relaxation time compared to those with blended nanoparticles. The magnetic character of the Fe₃O₄ nanoparticles enabled self-healing of the vitrimer composite materials upon exposure to an alternating electromagnetic field during induction heating.