Microphase separation of block copolymers provides a promising route towards engineering a mechanically robust ion conducting film for electrochemical devices. The separation into two different nano-domains enables the film to simultaneously exhibit both high ion conductivity and mechanical robustness, material properties inversely related in most homopolymer and random copolymer electrolytes. To exhibit the maximum conductivity and mechanical robustness, both domains would span across macroscopic length scales enabling uninterrupted ion conduction. One way to achieve this architecture is through external alignment fields that are applied during the microphase separation process. In this review, we present the progress and challenges for aligning the ionic domains in block copolymer electrolytes. A survey of alignment and characterization is followed by a discussion of how the nanoscale architecture affects the bulk conductivity and how alignment may be improved to maximize the number of participating conduction domains.
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