Catalyst-Free Dynamic Networks for Recyclable, Self-Healing Solid Polymer Electrolytes

Polymer networks with dynamic covalent cross-links act as solids but can flow at high temperatures. They have been widely explored as reprocessable and self-healing materials, but their use as solid electrolytes is limited. Here we report poly(ethylene oxide)-based networks with varying amounts of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) to understand the impact of a salt on the ion transport and network dynamics. We observed that the conductivity of our dynamic networks reached a maximum of 3.5 × 10^-4 S/cm at an optimal LiTFSI concentration. Rheological measurements showed that the amount of LiTFSI significantly affects the mechanical properties, as the shear modulus varies between 1 and 10 MPa and the stress relaxation by 2 orders of magnitude. Additionally, we found that these networks can efficiently dissolve back to pure monomers and heal to recover their conductivity after damage, showing the potential of dynamic networks as sustainable solid electrolytes.