Multifunctional Poly(3,4-ethylenedioxythiophene)/Crystalline Nanofibrous Cellulose Composites for Eco-Friendly and Sustainable Electronics.

Nanocellulose constitutes promising resources for next-generation electronics, particularly when incorporated with conductive polymers due to their abundance, renewability, processability, biodegradability, flexibility, and mechanical performance. In this study, electrically conducting cellulose nanofibers were fabricated through in situ chemical polymerization of poly(3,4-ethylenedioxythiophene) (PEDOT) on the surface of sulfuric acid-treated cellulose nanofibers (SACN). The utilization of highly crystalline SACN extracted from tunicate yielded synergistic effects in PEDOT polymerization for achieving a highly conductive and molecularly uniform coating. Polymerization parameters, such as monomer concentration, molar ratio with oxidants, and temperature, were systematically investigated. High electrical conductivity of up to 57.8 S cm was obtained without utilizing the classical polystyrenesulfonate dopant. The resulting nanocomposite demonstrates the unique advantages of both electrically conductive PEDOT and mechanically robust high-crystalline cellulose nanofibers. As a proof-of-applicational concept, an electrical circuit was drawn with SACN-PEDOT as the conductive ink on flexible paper using a simple commercial extrusion-based printer. Furthermore, the flame-retardant property of SACN-PEDOT was demonstrated owing to the high crystallinity of SACN, effective char formation, and high conductivity of PEDOT. The multifunctional SACN-PEDOT developed in this study shows great promise to be employed in versatile applications as a low-cost, ecofriendly, flexible, and sustainable electrically conductive material.