ABSTRACT: Nanocellulose, as a biobased versatile nanomaterial that can be derived with tailorable surface functionalities, dimensions, and morphologies, has considerable implications for modifying the rheology, mechanical reinforcement, and influencing the carbonization efficiency in the production of polyacrylonitrile (PAN)-based carbon fibers. Herein, we report the influence of three different nanocellulose types, varying in the derivatization method, source, and aspect ratio, on the mechanical properties and thermal transformations of solution-spun PAN/nanocellulose nanocomposite fibers into carbon fibers. The incorporation of 0.1 wt % nanocellulose into solution-spun PAN fibers led to a 7-19% increase in tensile modulus and 0-27% increase in tensile strength in the solution-spun fibers, compared to a control PAN fiber. These improvements varied depending on the nanocellulose type. After low-temperature carbonization at 1200 °C, improvements in the mechanical properties of the nanocellulose-reinforced carbon fibers, compared with a PAN fiber, were also observed. In contrast to the precursor fibers, the improvement % in the carbonized fibers was found to be dependent on the nanocellulose morphology and was linearly correlated with increasing aspect ratio of nanocellulose. For example, in carbon fibers with a cotton-derived low-aspect-ratio cellulose nanocrystal and spinifex-derived high-aspect-ratio CNC and nanofiber, up to 4, 87, and 172% improvements in tensile moduli were observed, respectively. Due to the processing methods used, the nanocellulose aspect ratio and crystallinity are inversely related, and as such, the increase in the carbon fiber mechanical properties was also related to a decrease in crystallinity of the nanocellulose reinforcers. Raman spectra and electron microscopy analysis suggest that mechanical improvement after carbonization is due to internal reinforcement by highly ordered regions surrounding the carbonized nanocellulose, within the turbostratic carbon fibers.
