(649b) Computational Study of Ion Transport in Polymer Electrolytes Near Glass Transition
AIChE Annual Meeting
2021 Annual Meeting
Materials Engineering and Sciences Division
Transport Phenomena in Polymer Systems II
Thursday, November 11, 2021 - 3:30pm to 3:45pm
Improving ion transport in polymer electrolytes has been one of the primary priorities in engineering materials for solid-state batteries and energy storage applications. Polymer charge fraction and architectures, the size asymmetry between monomers and counterions and their electrostatic coupling strength are among the most relevant design parameters that govern the ion transport properties of these materials. In this study, using coarse-grained simulations and advanced sampling techniques, we analyze the influences of these key parameters on the coupling between the assembled nanostructures and ion dynamics. In the presence of an external electric field, the dominating ion transport mechanism is shown to strongly depend on the size asymmetry between the monomers and the counterions, in addition to the Coulombic interaction strength. Furthermore, as polymer charge fraction increases, dynamical heterogeneity at the polymer segment length scales near glass transition can be enhanced, allowing the ions to move faster in the kinetically arrested polymer matrix. The findings allow us to propose design principles of the ionomers for improving ion mobility, and to develop data models that predict ion transport properties from polymer architectures and operating conditions.