Salt Effects on the Mechanical Properties of Ionic Conductive Polymer: A Molecular Dynamics Study

Functional polymers can be used as electrolyte and binder materials in solid-state batteries. This often requires performance targets in terms of both the transport and mechanical properties. In this work, a model ionic conductive polymer system, i.e., poly(ethylene oxide)-LiTFSI, was used to study the impact of salt concentrations on mechanical properties, including different types of elastic moduli and the viscoelasticity with both nonequilibrium and equilibrium molecular dynamics simulations. We found an encouragingly good agreement between experiments and simulations regarding Young's modulus, bulk modulus, and viscosity. In addition, we identified an intermediate salt concentration at which the system shows high ionic conductivity, high Young's modulus, and short elastic restoration time. Therefore, this study laid the groundwork for investigating ionic conductive polymer binders with self-healing functionality from molecular dynamics simulations.