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Solid polymer electrolytes are considered a promising alternative totraditional liquid electrolytes in energy storage applications because of theirgood mechanical properties, and excellent thermal and chemical stability. Agap, however, still exists in understanding ion transport mechanisms andimproving ion transport in solid polymer electrolytes. Therefore, it is crucialto bridge composition--structure and structure--property relationships. Here wedemonstrate that size asymmetry, $\lambda$, represented by the ratio ofcounterion to charged monomer size, plays a key role in both the nanostructureand in the ionic dynamics. More specifically, when the nanostructure ismodified by the external electric field such that the mobility cannot bedescribed by linear response theory, two situations arise. The ionic mobilityincreases as $\lambda$ decreases (small counterions) in the weak electrostatics(high dielectric constant) regime. Whereas in systems with strong electrostaticinteractions, ionomers with higher size symmetry ($\lambda \approx 1$) displayhigher ionic mobility. Moreover, ion transport is found to be dominated by thehopping of the ions and not by moving ionic clusters (also known as"vehicular'' charge transport). These results serve as a guide for designingion-containing polymers for ion transport related applications.

Control of Ionic Mobility via Charge Size Asymmetry in Random Ionomers