Modular Self-Assembly and Dynamics in Coordination Star Polymer Glasses: New Media for Ion Transport

We report modulation of the self-assembled microstructure and dynamics of Coordination Star Polymer (CSP) materials and their utilization for ion transport. Series of CSPs with identical cores but varying arm lengths were synthesized via a convergent route. The assembled structures exhibit a glassy nature with short-range structural order while long-range disorder with dynamic polymer arm domains. The hierarchical structure and mechanical properties of CSPs are tunable by controlling the size of the CSP corona. Glassy CPSs with a dynamic polymer domain were employed as matrix for the transport of alkali metal cations, and the solvent free Li+ ion conductivities of the optimized glass materials were found to be comparable to those of the well known organic polymer electrolytes. Further, we characterized that the ion transporting behavior in CSP glasses is strongly correlated to their structural ordering and local dynamics. The soft and dynamic nature of the CSPs was explored to improve solid–solid interface. The study demonstrates the potential of CSP glasses as a new class of designable inorganic organic hybrid electrolytes for solid-state applications.