Pom Functionalized Ionogels with Tunable Optical, Mechanical, Electrical, and Sensory Properties

Abstract Ionogels, with wide applications in tissue engineering, soft robotics, and flexible iontronic devices, require tunable optical, mechanical, and electrical properties for advanced functionality applications. Here, a facile strategy is reported to tune a set of properties of ionogels via tuning the redox states of the added polyoxometalate (POM) clusters. Upon external electrical stimuli, the POM clusters in the ionogels can be reversibly tuned from a transparent, oxidized state to a blue, reduced state. The redox states of the POM anions influence the POM‐polymer interactions, which promotes the in situ modulation of the ionogel properties reversibly over a large window: optical transparency from 91% to 7%, dissipated energy from 0.9 to 3.1 MJ m⁻³, elastic modulus from 1.5 to 2 MPa, conductivity from 1.6 × 10⁻⁴ to 2.2 × 10⁻⁴ S cm⁻¹. Meanwhile, the sensory properties of the ionogels can be modulated simultaneously. For strain sensing and pressure sensing, the GF can be tuned from 2.3 to 7.2, and the sensitivity can be tuned from 0.8 to 1.2 kPa⁻¹. Such an ionogel with tunable optical, mechanical, and electrical properties may find a variety of applications meeting specific demands. The POM functionalization strategy may also bring new insights into the design of the stimuli‐responsive ionogels.