Multifunctional Polyoxometalates‐Based Ionohydrogels toward Flexible Electronics

Abstract Multifunctional flexible electronics present tremendous opportunities in the rapidly evolving digital age. One potential avenue to realize this goal is the integration of polyoxometalates (POMs) and ionic liquid‐based gels (ILGs), but the challenge of macrophase separation due to poor compatibility, especially caused by repulsion between like‐charged units, poses a significant hurdle. Herein, the possibilities of producing diverse and homogenous POMs‐containing ionohydrogels by nanoconfining POMs and ionic liquids (ILs) within an elastomer‐like polyzwitterionic hydrogel using a simple one‐step random copolymerization method, are expanded vastly. The incorporation of polyzwitterions provides a nanoconfined microenvironment and effectively modulates excessive electrostatic interactions in POMs/ILs/H₂O blending system, facilitating a phase transition from macrophase separation to a submillimeter scale worm‐like microphase‐separation system. Moreover, combining POMs‐reinforced ionohydrogels with a developed integrated self‐powered sensing system utilizing strain sensors and Zn‐ion hybrid supercapacitors has enabled efficient energy storage and detection of external strain changes with high precision. This work not only provides guidelines for manipulating morphology within phase‐separation gelation systems, but also paves the way for developing versatile POMs‐based ionohydrogels for state‐of‐the‐art smart flexible electronics.