Self-healable and stretchable ionogels serve as electrolytes and substrates for integrated all-in-one micro-supercapacitors

A type of ionogel electrolytes on the basis of a dual-dynamic network was prepared, composed of metal-ligand (Li+-PEO) coordination and hydrogen bonding, and a facile and versatile strategy for the construction of integrated all-in-one micro-supercapacitors was proposed to deliver promising electrochemical performance. [Display omitted] •Self-stand ionogels are designed based on a dual-dynamic network.•The ionogels possess high self-healing efficiency with excellent stretchability.•The ionogels own high ionic conductivity and operating voltage window.•MSCs was prepared with ionogels acting as electrolyte and substrate simultaneously.•The capacitance retention rate of MSCs reaches 98% after 5th healing process. Self-healable and stretchable electrolytes are extremely desirable for next-generation flexible energy storage devices. Nevertheless, most of previously reported autonomous self-healing electrolytes possess only moderate mechanical strength and recoverability, as well as poor ionic conductivity and low operating voltage window. In this work, a type of ionogel electrolytes is reported on the basis of a dual-dynamic network composed of metal-ligand (Li+-PEO) coordination and hydrogen bonding. Impressively, the ionogel electrolytes exhibit high tensile fracture strength (0.96 MPa), stretchability (≈1847%) and electrochemical stability up to about −4 to 4 V. A novel all-in-one self-healable micro-supercapacitor prototype is proposed by adopting direct ink writing technique, whereas the electrode material is directly printed onto the ionogel film which acts as a flexible substrate and gel-electrolyte simultaneously. The maximum energy density of the all-in-one micro-supercapacitor reaches 81.88 μWh cm−2 at a power density of 0.75 mW cm−2. In the absence of external stimulus, the damaged micro-supercapacitor can achieve up to 98% self-healing efficiency after 2 min at room temperature. Our research provides new fundamental insights into the construction of stretchable and self-healable ionogels and offers guidelines for the design of integrated micro-supercapacitors to deliver better electrochemical performance.