Mechanically strong, flexible and thermally stable graphene oxide/nanocellulosic films with enhanced dielectric properties

Abstract

Flexible and eco-friendly films, with enhanced dielectric properties and the potential for energy storage applications, have been fabricated from ammonia-functionalized graphene oxide (NGO) nanoplatelets and wood-based cellulose nanofibrils (CNF) vs. (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO) pre-oxidized (carboxylated) CNFs (TCNF) by the solvent casting method. Various CNF-NGO (CNG) and TCNF-NGO (TCNG) composite films prepared with 0.5–3 wt% of NGO were analysed structurally by FTIR and XRD spectroscopy, and evaluated optically by UV-Vis spectroscopy. The morphological analysis using SEM showed good dispersibility of the NGO sheets in the randomly-distributed CNF, and the dense and parallel-oriented TCNF cellulose nanofibrils. Such a synergistic effect of both components contributed to ultra-strong and ultra-stiff composite films with good mechanical and thermal stability, although they were more brittle with a smoother surface and lower transmittance for the TCNF based films, due to the stronger physico–chemical interactions with NGO. The dielectric performance was verified with a higher (3 wt%) NGO loading capacity, which resulted in a dielectric constant of ∼46 vs. ∼52, and conductivity of ∼2.07 × 10⁻⁴ S m⁻¹ vs. 3.46 × 10⁻⁴ S m⁻¹ for CNG vs. TCNG films, respectively, at a frequency of 1 MHz, showing greater enhancement than other reported studies. Cyclic voltammetry and electrochemical impedance studies reveal the energy storage ability and electrochemical performance of the composite films, under kinetic- and diffusion-controlled processes for the CNG, and under a kinetic-controlled process for the TCNG films.