Additive Fabrication of Polyaniline and Carbon-Based Composites for Energy Storage

The growing demand for efficient energy storage systems, particularly in portable electronics and electric vehicles, has led to increased interest in supercapacitors, which offer high power density, rapid charge/discharge rates, and long cycle life. However, improving their energy density without compromising performance remains a challenge. In this study, we developed novel 3D-printed reduced graphene oxide (rGO) electrodes coated with polyaniline (PANI) to enhance their electrochemical properties. The rGO 3D-printed electrodes were fabricated using direct ink writing (DIW), which allowed precise control over thickness, ranging from 4 to 24 layers. A unique ink formulation was optimized for the printing process, consisting of rGO, cellulose acetate (CA) as a binder, and acetone as a solvent. The PANI coating was applied via chemical oxidative polymerization (COP) with up to five deposition cycles. Electrochemical testing, including cyclic voltammetry (CV), galvanostatic charge/discharge (GCD), and electrochemical impedance spectroscopy (EIS), revealed that 12-layer electrodes with three PANI deposition cycles achieved the highest areal capacitance of 84.32 mF/cm². While thicker electrodes (16 layers and beyond) experienced diminished performance due to ion diffusion limitations, the composite electrodes demonstrated excellent cycling stability, retaining over 80% of their initial capacitance after 1500 cycles. This work demonstrates the potential of 3D-printed PANI/rGO electrodes for scalable, high-performance supercapacitors with customizable architectures.