Simultaneously Enhancing the Mechanical Strength and Ionic Conductivity of Stretchable Ionogels Enabled by Polymerization-Induced Phase Separation

Stretchable ionogels have been considered as ideal materials for constructing flexible electronics. However, current ionogels suffer from the well-known trade-off between mechanical strength and conductivity. Here, we develop a simple strategy based on polymerization-induced phase separation to simultaneously enhance the mechanical performance and conductivity of the ionogels by randomly copolymerizing a hydrophobic and a hydrophilic monomer in a hydrophobic ionic liquid (IL). The polymerization process induced the formation of a bicontinuous network containing a polymer-rich phase and a solvent-rich phase. The polymer-rich domains with hydrogen bonds can bear loading, greatly improving the mechanical strength; meanwhile, the solvent-rich domains form conductive nanochannels to enhance the conductivity. The resulting copolymer ionogel is highly stretchable (500% strain), and the optimal fracture stress and conductivity are 0.29 MPa and 3.4 mS/cm, achieving 7.8- and 2.3-fold enhancements compared with that of the prepared homogeneous (pure PMEA) ionogel at the same IL content, respectively. Moreover, the ionogels also exhibit anti-swelling properties in various liquids and self-adhesiveness. Potential applications of this ionogel as a wearable sensor in a complex environment are further demonstrated.