Flexible and alternately layered high electrochemical active electrode based on MXene, carboxymethylcellulose, and carbon nanotube for asymmetric micro-supercapacitors

Recent studies have shown that Ti-based MXene has great potential for electrochemical energy storage applications, including Li-ion batteries and micro-supercapacitors. However, self-stacking and weak interlayer interactions lead to poor electrochemical properties. Herein, a simple one-step vacuum filtration method was used to prepare a MXene/carboxymethylcellulose/carbon nanotube (Ti3C2Tx/CMC/CNT) hybrid membrane. Due to the unique adhesion and flexibility of CMC, it can be interwoven with CNT to form an interconnected mesh structure, which on the one hand mitigates the self-aggregation of CNT, and on the other hand, the CNT entangled on the surface of CMC imparts its electrical conductivity. Moreover, the -OH of CMC can form hydrogen bonds with the reactive terminal groups (-O, -OH, -F) of Ti3C2Tx, resulting in the tight anchoring of CMC and CNT to Ti3C2Tx nanosheet layers and bridging adjacent Ti3C2Tx nanosheets to form a complete conductive pathway. As a result, the mechanical property test indicates that the Ti3C2Tx/CMC/CNT hybrid film could achieve a maximum tensile strength of 64.9 MPa. Furthermore, an asymmetric micro-supercapacitor (MSC) using Ti3C2Tx/CMC/CNT as the cathode and reduced graphene oxide/carboxymethylcellulose/polypyrrole (RGO/CMC/PPy) as the anode was fabricated, which exhibited a high energy density of 258.8 μWh cm-2 at a power density of 750 μW cm-2, and an ultra-long cycle life (93.2% capacitance retention after 15,000 GCD cycles). The simple and scalable preparation process makes this MSC device very promising for commercial electronics applications.