Continuously Reinforced Carbon Nanotube Film Sea-Cucumber-like Polyaniline Nanocomposites for Flexible Self-Supporting Energy-Storage Electrode Materials

The charge storage mechanism and capacity of supercapacitors completely depend on the electrochemical and mechanical properties of electrode materials. Herein, continuously reinforced carbon nanotube film (CNTF), as the flexible support layer and the conductive skeleton, was prepared via the floating catalytic chemical vapor deposition (FCCVD) method. Furthermore, a series of novel flexible self-supporting CNTF/polyaniline (PANI) nanocomposite electrode materials were prepared by cyclic voltammetry electrochemical polymerization (CVEP), with aniline and mixed-acid-treated CNTF film. By controlling the different polymerization cycles, it was found that the growth model, morphology, apparent color, and loading amount of the PANI on the CNTF surface were different. The CNTF/PANI-15C composite electrode, prepared by 15 cycles of electrochemical polymerization, has a unique surface, with a "sea-cucumber-like" 3D nanoprotrusion structure and microporous channels formed via the stacking of the PANI nanowires. A CNTF/PANI-15C flexible electrode exhibited the highest specific capacitance, 903.6 F/g, and the highest energy density, 45.2 Wh/kg, at the current density of 1 A/g and the voltage window of 0 to 0.6 V. It could maintain 73.9% of the initial value at a high current density of 10 A/g. The excellent electrochemical cycle and structural stabilities were confirmed on the condition of the higher capacitance retention of 95.1% after 2000 cycles of galvanostatic charge/discharge, and on the almost unchanged electrochemical performances after 500 cycles of bending. The tensile strength of the composite electrode was 124.5 MPa, and the elongation at break was 18.9%.