Electrospun Core–Shell Nanofibrous Membranes with Nanocellulose-Stabilized Carbon Nanotubes for Use as High-Performance Flexible Supercapacitor Electrodes with Enhanced Water Resistance, Thermal Stability, and Mechanical Toughness

A high-performance flexible supercapacitor electrode with a core–shell structure is successfully developed from cellulose nanocrystal (CNC)-stabilized carbon nanotubes (CNTs). By incorporating poly(vinyl alcohol) (PVA) and poly(acrylic acid) (PAA), a cross-linked nanofibrous membrane (CNT–CNC/PVA–PAA) is prepared as the core material via directional electrospinning, followed by a thermal treatment. The flexible supercapacitor electrodes are eventually fabricated via the in situ polymerization of polyaniline (PANI), which was used as the coating shell material, on the aligned electrospun nanofibers. By taking advantage of the thermally induced esterification cross-linking that occurs among PVA, PAA, and the CNT–CNC nanohybrids, the membranes present with enhanced water resistance, mechanical strength, and thermal stability. After the surface coating of the PANI shell, the optimized PANI@CNT–CNC/PVA–PAA nanofibrous membranes exhibit a large porosity, an enhanced specific surface area, a superior tensile strength of ∼54.8 MPa, and a favorable electroconductivity of ∼0.44 S m–1. As expected, the nanofibrous electrodes with a specific capacitance of 164.6 F g–1 can maintain 91% of the original capacitance after 2000 cycles. The symmetrical solid-state supercapacitor assembled by the nanofibrous electrodes shows an excellent capacitance of 155.5 F g–1 and a remarkable capacitance retention of 92, 90, and 89% after 2000 cycles under flat, bending, and twisting deformations, respectively.