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. • 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. [ABSTRACT FROM AUTHOR]