Interfacial Modulation of Ti3C2Tx MXene by Cellulose Nanofibrils to Construct Hybrid Fibers with High Volumetric Specific Capacitance

Abstract The intrinsic poor rheological properties of MXene inks result in the MXene nanosheets in dried MXene microfibers prone to self‐stacking, which is not conducive to ion transport and diffusion, thus affecting the electrochemical performance of fiber‐based supercapacitors. Herein, robust cellulose nanofibrils (CNF)/MXene hybrid fibers with high electrical conductivity (916.0 S cm −1 ) and narrowly distributed mesopores are developed by wet spinning. The interfacial interaction between CNF and MXene can be enhanced by hydrogen bonding and electrostatic interaction due to their rich surface functional groups. The interfacial modulation of MXene by CNF can not only regulate the rheology of MXene spinning dispersion, but also enhance the mechanical strength. Furthermore, the interlayer distance and self‐stacking effect of MXene nanosheets are also regulated. Thus, the ion transport path within the fiber material is optimized and ion transport is accelerated. In H 2 SO 4 electrolyte, a volumetric specific capacitance of up to 1457.0 F cm −3 (1.5 A cm −3 ) and reversible charge/discharge stability are demonstrated. Intriguingly, the assembled supercapacitors exhibit a high‐volume energy density of 30.1 mWh cm −3 at 40.0 mW cm −3 . Moreover, the device shows excellent flexibility and cycling stability, maintaining 83% of its initial capacitance after 10 000 charge/discharge cycles. Practical energy supply applications (Power for LED and electronic watch) can be realized.