The integration of capacitive and faradaic energy storage mechanism in the form of hybrid materials, electrodes and devices aims at increasing energy and power densities for the next generation of electrochemical energy storage devices.

Flexible solid-state supercapacitors (FSSCs) are frontrunners in energy storage device technology and have attracted extensive attention owing to recent significant breakthroughs in modern wearable electronics. In this study, we review the state-of-the-art advancements in FSSCs to provide new insights on mechanisms, emerging electrode materials, flexible gel electrolytes and novel cell designs. The review begins with a brief introduction on the fundamental understanding of charge storage mechanisms based on the structural properties of electrode materials. The next sections briefly summarise the latest progress in flexible electrodes (i.e., freestanding and substrate-supported, including textile, paper, metal foil/wire and polymer-based substrates) and flexible gel electrolytes (i.e., aqueous, organic, ionic liquids and redox-active gels). Subsequently, a comprehensive summary of FSSC cell designs introduces some emerging electrode materials, including MXenes, metal nitrides, metal–organic frameworks (MOFs), polyoxometalates (POMs) and black phosphorus. Some potential practical applications, such as the development of piezoelectric, photo-, shape-memory, self-healing, electrochromic and integrated sensor-supercapacitors are also discussed. The final section highlights current challenges and future perspectives on research in this thriving field.

Different nanostructures (Ns), such as nanobelts, nanobricks and nanosheets, of polypyrrole (PPy) were successfully fabricated on stainless steel substrates by simply varying the scan rate of deposition in the potentiodynamic mode. These PPy Ns were characterized using X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and surface area measurement. The XRD analysis showed the formation of amorphous PPy thin films, and the FTIR studies confirmed characteristic chemical bonding in the PPy materials. SEM images depicted that a high scan rate of deposition can form multilayer nanosheets with high porosity leading to a system with excellent processability. The PPy nanosheets possess a higher Brunauer–Emmett–Teller (BET) surface area of 37.1 m² g⁻¹ than PPy nanobelts and nanobricks. The supercapacitive performances of different PPy Ns were evaluated using cyclic voltammetry (CV) and galvanostatic charge–discharge techniques in 0.5 M H₂SO₄. A maximum specific capacitance of 586 F g⁻¹ was obtained for multilayer nanosheets at a scan rate of 2 mV s⁻¹. In addition, impedance measurements of the different Ns of PPy electrodes were performed suggesting that the PPy electrodes with multilayer nanosheets are promising materials for the next generation high performance electrochemical supercapacitors.