Perspective: Morphology and ion transport in ion-containing polymers from multiscale modeling and simulations

Ion-containing polymers are soft materials composed of polymeric chains and mobile ions. Over the past several decades they have been the focus of considerable research and development for their use as the electrolyte in energy conversion and storage devices. Recent and significant results obtained from multiscale simulations and modeling for proton exchange membranes (PEMs), anion exchange membranes (AEMs), and polymerized ionic liquids (polyILs) are reviewed. The interplay of morphology and ion transport is emphasized. We discuss the influences of polymer architecture, tethered ionic groups, rigidity of the backbone, solvents, and additives on both morphology and ion transport in terms of specific interactions. Novel design strategies are highlighted including precisely controlling molecular conformations to design highly ordered morphologies; tuning the solvation structure of hydronium or hydroxide ions in hydrated ion exchange membranes; turning negative ion-ion correlations to positive correlations to improve ionic conductivity in polyILs; and balancing the strength of noncovalent interactions. The design of single-ion conductors, well-defined supramolecular architectures with enhanced one-dimensional ion transport, and the understanding of the hierarchy of the specific interactions continue as challenges but promising goals for future research.