Hydrogel electrolytes for energy storage devices have made great progress, yet they present a major challenge in the assembly of flexible supercapacitors with high ionic conductivity and self-healing properties. Herein, a smart self-healing hydrogel electrolyte based on alginate/poly (3,4-ethylenedioxythiophene):poly(styrenesulfonate) (alginate/PEDOT:PSS)(A/P:P) was prepared, wherein H2SO4 was employed as a polymeric initiator, as well as a source of ions. PEDOT:PSS is a semi-interpenetrating network (IPN) that has been used in recent studies to exhibit quick self-healing properties with the H₂SO₃ additive, which further improves its mechanical strength and self-healing performance. A moderate amount of PEDOT:PSS in the hydrogel (5 mL) was found to significantly improve the ionic conductivity compared to the pure hydrogel of alginate. Interestingly, the alginate/PEDOT:PSS composite hydrogel exhibited an excellent ability to self-heal and repair its original composition within 10 min of cutting. Furthermore, the graphite conductive substrate-based supercapacitor with the alginate/PEDOT:PSS hydrogel electrolyte provided a high specific capacitance of 356 F g−1 at 100 mV/s g−1. The results demonstrate that the A/P:P ratio with 5 mL PEDOT:PSS had a base sheet resistance of 0.9 Ω/square. This work provides a new strategy for designing flexible self-healing hydrogels for application in smart wearable electronics.

Globally, researchers have devoted consistent efforts to producing excellent coating properties since coating plays an essential role in enhancing electrochemical performance and surface quality. In this study, TiO2 nanoparticles in varying concentrations of 0.5, 1, 2, and 3 wt.% were added into the acrylic-epoxy polymeric matrix with 90:10 wt.% (90A:10E) ratio incorporated with 1 wt.% graphene, to fabricate graphene/TiO2-based nanocomposite coating systems. Furthermore, the properties of the graphene/TiO2 composites were investigated by Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), ultraviolet-visible (UV-Vis) spectroscopy, water contact angle (WCA) measurements, and cross-hatch test (CHT), respectively. Moreover, the field emission scanning electron microscope (FESEM) and the electrochemical impedance spectroscopy (EIS) tests were conducted to investigate the dispersibility and anticorrosion mechanism of the coatings. The EIS was observed by determining the breakpoint frequencies over a period of 90 days. The results revealed that the TiO2 nanoparticles were successfully decorated on the graphene surface by chemical bonds, which resulted in the graphene/TiO2 nanocomposite coatings exhibiting better dispersibility within the polymeric matrix. The WCA of the graphene/TiO2 coating increased along with the ratio of TiO2 to graphene, achieving the highest CA of 120.85° for 3 wt.% of TiO2. Excellent dispersion and uniform distribution of the TiO2 nanoparticles within the polymer matrix were shown up to 2 wt.% of TiO2 inclusion. Among the coating systems, throughout the immersion time, the graphene/TiO2 (1:1) coating system exhibited the best dispersibility and high impedance modulus values (|Z|0.01 Hz), exceeding 1010 Ω cm2.

A conductive cotton hydrogel with graphene and ions can come into contact with electrodes in solid electrolytes at the molecular level, leading to a more efficient electrochemical process in supercapacitors. The inherently soft nature of cotton mixed with hydrogel provides superior flexibility of the electrolyte, which benefits the devices in gaining high flexibility. Herein, we report on the current progress in solid-state hydrogel electrolytes based on 3D pure cotton/graphene and present an overview of the future direction of research. The ionic conductivity of a complex hydrogel significantly increased by up to 13.9 × 10−3 S/cm at 25 °C, due to the presence of graphene, which increases ionic conductivity by providing a smooth pathway for the transport of charge carriers and the polymer. Furthermore, the highest specific capacitance of 327 F/g at 3 mV/s was achieved with cyclic voltammetry measurement and a galvanostatic charge–discharge measurement showed a peak value of 385.4 F/g at 100 mA/g current density. Furthermore, an electrochemical analysis demonstrated that a composite cotton/graphene-based hydrogel electrolyte is electrically stable and could be used for the design of next-generation supercapacitors.

We report Na-Alginate-based hydrogels with high ionic conductivity and water content fabrication using poly (3,4-ethylene dioxythiophene) (PEDOT): poly (4-styrene sulfonic acid) (PSS) and a hydrogel matrix based on dimethyl sulfoxide (DMSO). DMSO was incorporated within the PEDOT:PSS hydrogel. A hydrogel with higher conductivity was created through the in-situ synthesis of intra-Na-Alginate, which was then improved upon by H2SO4 treatment. Field emission scanning electron microscopy (FESEM) was used to examine the surface morphology of the pure and synthetic hydrogel. Structural analysis was performed using Fourier-transform infrared spectroscopy (FTIR). Thermogravimetric analysis (TGA), which examines thermal properties, was also used. A specific capacitance of 312 F/g at 80 mV/s (energy density of 40.58 W/kg at a power density of 402.20 W/kg) at 100 DC mA/g was achieved by the symmetric Na-Alginate/PEDOT:PSS based flexible supercapacitor. The electrolyte achieved a higher ionic conductivity of 9.82 × 10−2 and 7.6 × 10−2 Scm−1 of Na-Alginate and a composite of Na-Alginate/PEDOT:PSS at 25 °C. Furthermore, the supercapacitor Na-Alginate/PEDOT:PSS//AC had excellent electrochemical stability by showing a capacity retention of 92.5% after 3000 continuous charge–discharge cycles at 10 mA current density. The Na- Alginate/PEDOT:PSS hydrogel displayed excellent flexibility and self-healing after re-contacting the two cut hydrogel samples of electrolyte for 90 min because of the dynamic cross-linking network efficiently dissipated energy. The illumination of a light-emitting diode (LED) verified the hydrogel’s capacity for self-healing.