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Enhancing Cation Diffusion and Suppressing Anion Diffusion via Lewis-Acidic Polymer Electrolytes (1610.06838v1)

Published 20 Oct 2016 in physics.chem-ph, cond-mat.mes-hall, cond-mat.mtrl-sci, and cond-mat.soft

Abstract: Solid polymer electrolytes (SPE) have the potential to increase both the energy density and stability of lithium-based batteries, but low Li-ion conductivity remains a barrier to technological viability. SPEs are designed to maximize Li-ion diffusivity relative to the anion, while maintaining sufficient salt solubility. It is thus remarkable that polyethylene oxide (PEO), the most widely used SPE, exhibits Li-ion diffusivity that is an order of magnitude smaller than that of typical counter-ions, such as TFSI, at moderate salt concentrations. Here, we show that Lewis-basic polymers like PEO intrinsically favor slow cation and rapid anion diffusion while this relationship can be reversed in Lewis-acidic polymers. Using molecular dynamics (MD) simulations, Lewis-acidic polyboranes are identified that achieve up to a ten-fold increase in Li-ion diffusivity and a significant decrease in anion diffusivity, relative to PEO. The results for this new class of Lewis-acidic SPEs illustrate a general principle for increasing Li-ion diffusivity and transference number with polymer chemistries that exhibit weaker cation and stronger anion coordination.

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