Dielectric and thermal conductive properties of differently structured Ti3C2Tx MXene-integrated nanofibrillated cellulose films

The fabrication of nanocellulose-based substrates with high dielectric permittivity and anisotropic thermal conductivity to replace synthetic thermoplastics in flexible organic electronics remains a big challenge. Herein, films were prepared from native (CNF) and carboxylated (TCNF) cellulose nanofibrils, with and without the addition of thermally conductive multi-layered Ti 3 C 2 T x MXene, to examine the impact of polar (− OH, − COOH) surface groups on the film morphological, moisturizing, dielectric, and thermal dissipation properties. The electrostatic repulsion and hydrogen bonding interaction between the hydrophilic surface/terminal groups on CNF/TCNF and MXene was shown to render their self-assembly distribution and organization into morphologically differently structured films, and, consequently, different properties. The pristine CNF film achieved high intrinsic dielectric permittivity (ε' ~ 9), which was further increased to almost ε' ~ 14 by increasing (50 wt%) the MXene content. The well-packed and aligned structure of thinner TCNF films enables the tuning of both the composite’s dielectric permittivity (ε' ~ 6) and through-plane thermal conductivity (K ~ 2.9 W/mK), which increased strongly (ε' ~ 17) at higher MXene loading giving in-plane thermal conductivity of ~ 6.3 W/mK. The air-absorbed moisture ability of the films contributes to heat dissipation by releasing it. The dielectric losses remained below 0.1 in all the composite films, showing their potential for application in electronics. Graphic abstract