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-1 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.

Precisely tuned photonic properties of crystalline nanocellulose biocomposite coatings by gradually tailored nanoarchitectures.

Inspired by nature, we fabricated optically tuned bio-organic films of cellulose nanofibers (CNFs) and chitosan by precisely structuring layer-by-layer (LBL) assembly techniques. Directly extracted from tunicate, highly crystalline CNFs were deposited into gradual nanoporous structures, which dictates wave-like behaviors of optical transmittance and cyclic patterns of structural coloration. The optical transmittance of a glass substrate increased from 91% to 98.2% at a wavelength of 550 nm by reflectivity attenuation controls. The monochromic structural colors were discretely varied from orange to purple, seen only at a specific angle of the incident light, demonstrating visibly hidden security potential. Furthermore, we could modulate the coloration cycles by accelerating the LBL processes with polydopamine-coated CNFs. The 3D nanoporous structures of CNFs also provide synergies, including superhydophilic surface-driven antifogging properties. Our optically versatile biofilms made by all-natural CNFs and chitosan provide various potential applications, including solar cells, securities, and eco-friendly colors.