Recent designs of solid polymer electrolytes (SPE) for Li+ conduction consider polarity and mobility contrast to achieve improved conductivity. To assess this idea, we employ MD simulations to compare Li+ solvation and transport behaviors in poly (oligoethylene methacrylate) (POEM) versus in its copolymers with poly(glycerol carbonate methacrylate) (PGCMA). Unexpectedly, the highly polar PGCMA does not actively solvate Li+. Instead, the Li+-ether solvation is favored due to its relatively low entropic penalty. Further, we find that the presence of PGCMA promotes single-chain solvation and thereby suppresses inter-chain hopping. Finally, compared to PGCMA-r-POEM, the less-mixed PGCMA-b-POEM shows decreased Li+ transport. The observed trend is explained by further analysis on solvation site network connectivity. The discussions on thermodynamic driving forces for ion solvation preferences and on effects of mixing on long-range Li+ transport are insightful for future mixed SPE designs.

Solvation against polarity: A simulation study on Li+ transport in mixed-polarity graft polymer electrolytes

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ACS Fall 2022

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