Abstract
Recently we showed the potential of unaligned lithium-ion doped nematic Liquid Crystal Elastomer (LCE)-based quasi-solid (gel-polymer) electrolytes for batteries demonstrating excellent charge-discharge capacities. In this work, we study the effect of the alignment of LCE on the battery performance. We report the first investigation of homeotropically aligned LCEs in lithium-ion batteries and systematically compare their performance with planar aligned samples. We demonstrate that with increased ionic liquid (IL) loading, the homeotropic alignment (director is perpendicular to the electrodes) exhibits higher conductivity compared to planar alignment (director is parallel to the electrodes), underscoring the tunability of LCE-based electrolytes. The samples with the highest IL loading in both alignments exhibit a room temperature conductivity of ∼1 mS cm(-1) and an electrochemical stability window of ∼4.8 V. Additionally we find that LCE based batteries with homeotropic alignment charge more rapidly. These findings provide new insights into optimizing electrolyte performance through liquid crystal alignment control, thereby advancing the development of lithium-ion batteries.