Stretchable and Self‐Healing Interlocking All‐in‐One Supercapacitors Based on Multiple Cross‐Linked Hydrogel Electrolytes

Stretchable, self-healable, and high-capacity supercapacitors (SCs), as a state-of-the-art energy storage technology, hold enormous potential in cutting-edge wearable electronics. However, it is challenging to achieve excellent stretchability, superior self-healing ability, and high specific capacitance in the whole device simultaneously. Herein, a new class of high-capacity, stretchable, and self-healing SCs with all-in-one structures is constructed by synergistically utilizing multiple cross-linking effect and dynamic reversible non-covalent bonding of a stretchable and self-healing hydrogel electrolyte. The interlocking all-in-one structure leads to seamless contact as well as synchronous deformation and change between the electrodes and the electrolyte. Thus, by virtue of the stretchability and the self-healing ability of the electrolyte, the whole devices exhibit both excellent stretchability (elongation at break of 1060%) and superior self-healing ability (mechanically self-healing efficiency of approximate to 80%). Moreover, by regulating the mass loading of the electrode materials along with the good interface contact of the all-in-one structure, the SCs also show high specific capacitance (109 mF cm(-2)). Their comprehensive performances are among the best in the ever-reported all-in-one SCs. Thus, this work provides a feasible strategy for constructing high-capacity, stretchable, and self-healable SCs for smart wearable electronics.