Self-Healing, Flexible and Smart 3D Hydrogel Electrolytes Based on Alginate/PEDOT:PSS for Supercapacitor Applications

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.