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The exceptional properties of carbon nanoparticles, such as graphene, promise to expand the performance and functionality of many materials. The reinforcement of polymers is of keen interest due to their low density and flexible manufacturing methods. However, dispersing graphene in them has proven to be an enduring challenge due to the particles’ propensity to form performance-degrading agglomerations. Furthermore, effective solvents for nanoparticle dispersion are commonly harmful, non-renewable, petrochemicals. In this work, a bio-derived solvent, 1,4-cineole, is demonstrated as a renewable alternative to these solvents that can be used to form highly stable graphene nanoplatelet (GnP) suspensions and used to gel spin well-dispersed UHMWPE/GnP nanocomposite fibers. The GnP concentration in the fibers was varied across three orders of magnitude, 0.01 to 1 wt%, to examine its effect on fiber microstructure and properties. At low concentrations, the particles act as point defects without affecting the fiber microstructure, and poor particle/matrix interfacial adhesion results in significantly reduced mechanical properties. At 1 wt% GnPs, a network effect takes hold thereby reinforcing the fibers, but the particles also impede the growth and orientation of crucial load-carrying crystalline structures in the fiber. Unveiling the microstructural effects of GnPs on highly oriented and crystalline polymers in this study provides crucial insights for future work developing high-performance polymer nanocomposite fibers.

Three-dimensional carbon nanotube (CNT) forest microstructures are synthesized using sequenced, site-specific synthesis techniques. Thin-film layers of Al2O3and Al2O3/Fe are patterned to support film-catalyst and floating-catalyst chemical vapor deposition (CVD) in specific areas. Al2O3regions support only floating-catalyst CVD, whereas regions of layered Al2O3/Fe support both film- and floating-catalyst CNT growth. Sequenced application of the two CVD methods produced heterogeneous 3D CNT forest microstructures, including regions of only film-catalyst CNTs, only floating-catalyst CNTs, and vertically stacked layers of each. The compressive mechanical behavior of the heterogeneous CNT forests was evaluated, with the stacked layers exhibiting two distinct buckling plateaus. Finite element simulation of the stacked layers demonstrated that the relatively soft film-catalyst CNT forests were nearly fully buckled prior to large-scale deformation of the bottom floating-catalyst CNT forests.