Nucleotide‐Tackified Organohydrogel Electrolyte for Environmentally Self‐Adaptive Flexible Supercapacitor with Robust Electrolyte/Electrode Interface

Abstract Hydrogel electrolytes have attracted enormous attention in flexible and safe supercapacitors. However, the interfacial contact problem between hydrogel electrolyte and electrodes, and the environmental instability are the key factors restricting the development of hydrogel‐based supercapacitors. Here, a nucleotide‐tackified adhesive organohydrogel electrolyte is successfully constructed and exhibits freezing resistance and water‐holding ability based on the water/glycerol binary solvent system. Adenosine monophosphate enables the organohydrogels to possess outstanding adhesion and mechanical robustness. The robust adhesion can ensure close contact between the organohydrogel electrolyte and electrodes for constructing an all‐in‐one supercapacitor with low interfacial contact resistance. Impressively, the integrated organohydrogel‐based supercapacitors display an areal specific capacitance of 163.6 mF cm −2 . Besides, the supercapacitors feature prominent environmental stability with capacitance retention of 90.6% after 5000 charging/discharging cycles at −20 °C. Furthermore, based on the strong interfacial adhesion, the supercapacitors present excellent electrochemical stability without delamination/displacement between electrolyte and electrodes even under severe deformations such as bending and twisting. It is anticipated that this work will provide an encouraging way for developing flexible energy storage devices with electrochemical stability and environmental adaptability.