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Reversible radical deactivation during gelation narrows the chain length distribution of polymer networks, compromising stress delocalization, energy dissipation, and fracture toughness. 

Recent experimental results have demonstrated that zwitterionic ionogel comprised of polyzwitterion (polyZI)-supported lithium salt-doped ionic liquid exhibits improved conductivities and lithium transference numbers than the salt-doped base ionic liquid electrolyte (ILE). However, the underlying mechanisms of such observations remain unresolved. In this work, we pursued a systematic investigation to understand the impact of the polyZI content and salt concentration on the structural and dynamic properties of the poly(MPC) ionogel of our model polyZI ionogel, poly(2-methacryloyloxyethyl phosphorylcholine) [poly(MPC)] supported LiTFSI/N-butyl-N-methylpyrrolidinium TFSI base ionic liquid electrolyte. Our structural analyses show strong lithium–ZI interaction consistent with the physical network characteristic observed in the experiments. An increase in polyZI content leads to an increased fraction of Li+ ions coordinated with the polyZI. In contrast, an increase in salt concentration leads to a decreased fraction of Li+ ions coordinated with the polyZI. The diffusivities of the mobile ions in the poly(MPC) ionogel were found to be lower than the base ILE in agreement with experiments at T > 300 K. Analysis of ion transport mechanisms shows that lithium ions within the poly(MPC) ionogel travel via a combination of structural, vehicular diffusion, as well as hopping mechanism. Finally, the conductivity trend crossover between the poly(MPC) ionogel and the base ILE was rationalized via a temperature study that showed that the base ILE ions are influenced more by the variation of temperature when compared to the poly(MPC) ions.