Tailoring Organic–Organic Poly(vinylpyrrolidone) Microparticles and Fibers with Multiwalled Carbon Nanotubes for Reinforced Composites

Polymeric-based microparticles and fibers are tailorable for a wide range of common industrial and biomedical applications, while multiwalled carbon nanotubes (MWCNTs) are among the most useful macromolecules based on their outstanding electronic, mechanical, and optical properties at the nanoscale. If one combines these nanostructures with various polymeric precursors, their range of potential applications becomes even greater. One of the simplest and most affordable methods for fabricating micro- and nanostructures is electrospinning. Herein we demonstrate how MWCNTs may be used to produce tailor-made organic–organic poly­(vinylpyrrolidone) (PVP) microparticles and fibers via electrospinning by studying their structural, vibrational, rheological, and mechanical properties’ dependence on their solvent (ethanol (EtOH) or dimethyl­formamide (DMF)) and resulting morphology. Specifically, we find clear differences in morphologies from perfectly spherical and isolated microparticles to fibers mats, or a combination of fibers with entangled beads, with solvent type and concentration. On the basis of our findings, we propose that the mechanism governing the shape and size of the particles is a competition between the solvent’s surface tension, dielectric constant, and viscoelastic properties. We show, based on both our experimental results and density functional theory (DFT) calculations, that OH functionalization of the MWCNTs is essential for achieving high PVP coverages and promoting the stability of the resulting PVP/MWCNT nanocomposite. Finally, by fabricating PVP/MWCNT fiber mats, we demonstrate that low concentrations (0.01–0.1 wt %) of MWCNTs led to a qualitative improvement (∼250%) in the resulting mechanical properties, i.e., a reinforced composite. These results show how by controlling the solvent’s dielectric constant, surface tension, and polymer concentration, one may produce tailor-made polymeric nanomaterials in combination with other organic/inorganic nanoparticles, i.e., silver, gold, or carbon allotropes, for next-generation applications.