Controlled synthesis of Fe3O4 microparticles with interconnected 3D network structures for high-performance flexible solid-state asymmetric supercapacitors

The eco-friendly Fe-based oxides have attracted broad attention in supercapacitors on account of large theoretical capacities and cost-effective technologies associated with production and recycling. However, inferior conductivity and bad structural stability are still the main obstacles for its promoted application than the competition. In this work, well-designed Fe 3 O 4 microparticles with homogeneous size distribution, high crystallinity, and amorphous carbon shell have been synthesized and deposited on carbon fabric as an anode electrode via a series of feasible techniques, including anodic electrodeposition, polymerization, and annealing. The interconnected 3D network structures of electroactive materials are featured by high specific surface area and fast diffusion rate of ions. The sufacial carbon layer of Fe 3 O 4 particles, serves as the armor, which not only boosts electrical conductivity, but also maintains structural stability of the electrode during electrochemical processes. The electrochemical results show that the binder-free anode exhibits a remarkable areal capacitance of 0.95 F·cm −2 , a wide potential window of 1.2 V, and an outstanding cycling stability in 1 M KOH electrolyte (capacitance retention of 93.39 % over 8000 charge-discharge cycles). After combining with a NiCo-based cathode, 4.93 F·cm −3 volumetric capacitance, 1.8 mWh·cm −3 energy density, and 198 mW·cm −3 power density are achieved for the flexible solid-state asymmetric supercapacitor, which displays impressive cycling stability, excellent mechanical flexibility, and obvious performance advantages as compared with previously reported flexible energy storage devices. This work provides a feasible strategy to design a flexible Fe-based anode with superior conductivity and long-term stability for high-performing flexible solid-state asymmetric supercapacitor towards practical applications. • High crystallinity Fe 3 O 4 microparticles were deposited on CF via stepwise strategy. • Polypyrrole was served as carbon source and barrier material during annealing. • The 3D network structures embrace good conductivity and fast diffusion rate. • The anode exhibits large capacitance, wide potential window and good stability. • Bending test and 8000 GCD cycles demonstrate the flexibility and cycling stability.