Enormous-stiffness-changing polymer networks by glass transition mediated microphase separation

The rapid development of flexible electronics and soft robotics has an urgent demand for materials with wide-range switchable stiffness. Here, we report a polymer network that can isochorically and reversibly switch between soft ionogel and rigid plastic accompanied by a gigantic stiffness change from about 600 Pa to 85 MPa. This transition is realized by introducing polymer vitrification to regulate the liquid–liquid phase separation, namely the Berghmans’ point in the phase diagram of binary gel systems. Regulating the Lewis acid-base interactions between polymer and ionic liquids, the stiffness-changing ratio of polymer network can be tuned from 10 to more than 10(5). These wide-range stiffness-changing ionogels show excellent shape adaptability and reconfigurability, which can enhance the interfacial adhesion between ionogel and electrode by an order of magnitude and reduce interfacial impedance by 75%.