Effect of Host Incompatibility and Polarity Contrast on Ion Transport in Ternary Polymer-Polymer-Salt Blend Electrolytes

BK Wheatle and NA Lynd and V Ganesan, MACROMOLECULES, 53, 875-884 (2020).

DOI: 10.1021/acs.macromol.9b02510

We study ternary polymer-polymer-salt blend electrolytes using coarse grained molecular dynamics. We specifically examine the influence of the polymer hosts' incompatibility and polarity contrast on electrolyte ion transport characteristics. We find that, at moderate- to high-polarity contrasts, improving the miscibility of the polymer hosts by reducing their inherent incompatibility improves ionic transport, as measured by the ionic conductivity. However, contrary to expectations, ionic conduction slows with increased miscibility in low-polarity contrast electrolytes. Upon examining the underlying material properties, we find that ionic aggregation exhibits trends similar to ionic conductivity and is thus likely the controlling factor in these polymer-blend electrolytes. Our results suggest that ionic conduction can be improved in real polymer electrolytes by choosing chemistries that promote simultaneous miscibility and polarity contrast between the polymer hosts.

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