Conductive Carbon Microfibers Derived from Wet-Spun Lignin/Nanocellulose Hydrogels

We introduce an eco-friendly process to dramatically simplify carbon microfiber fabrication from biobased materials. The microfibers are first produced by wet-spinning in aqueous calcium chloride solution, which provides rapid coagulation of the hydrogel precursors comprising wood-derived lignin and 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibrils (TOCNF). The thermomechanical performance of the obtained lignin/TOCNF filaments is investigated as a function of cellulose nanofibril orientation (wide angle X-ray scattering (WAXS)), morphology (scanning electron microscopy (SEM)), and density. Following direct carbonization of the filaments at 900 °C, carbon microfibers (CMFs) are obtained with remarkably high yield, up to 41%, at lignin loadings of 70 wt % in the precursor microfibers (compared to 23% yield for those produced in the absence of lignin). Without any thermal stabilization or graphitization steps, the morphology, strength, and flexibility of the CMFs are retained to a large degree compared to those of the respective precursors. The electrical conductivity of the CMFs reach values as high as 103 S cm^-1, making them suitable for microelectrodes, fiber-shaped supercapacitors, and wearable electronics. Overall, the cellulose nanofibrils act as structural elements for fast, inexpensive, and environmentally sound wet-spinning while lignin endows CMFs with high carbon yield and electrical conductivity.