AI Article Synopsis
- This study explores the design of single-ion conducting liquid electrolytes for lithium secondary batteries, emphasizing the importance of increasing the Li+ transference number for better performance during rapid charging and discharging.
- Researchers investigated the effects of Li+-anion interactions in glyme-Li salt mixtures, finding that a specific combination (triglyme and lithium trifluoroacetate) exhibited a high Li+ transference number of 0.90, influenced by strong coupling between Li+ ions and anions.
- Advanced techniques like X-ray scattering and molecular dynamics simulations revealed that Li+ ions and trifluoroacetate anions form ionic clusters, which, although could lower ionic conductivity, are
Article Abstract
To achieve single-ion conducting liquid electrolytes for the rapid charge and discharge of Li secondary batteries, improvement in the Li+ transference number of the electrolytes is integral. Few studies have established a feasible design for achieving Li+ transference numbers approaching unity in liquid electrolytes consisting of low-molecular-weight salts and solvents. Previously, we studied the effects of Li+-solvent interactions on the Li+ transference number in glyme- and sulfolane-based molten Li salt solvates and clarified the relationship between this transference number and correlated ion motions. In this study, to deepen our insight into the design principles of single-ion conducting liquid electrolytes, we focused on the effects of Li+-anion interactions on Li ion transport in glyme-Li salt equimolar mixtures with different counter anions. Interestingly, the equimolar triglyme (G3)-lithium trifluoroacetate (Li[TFA]) mixture ([Li(G3)][TFA]) demonstrated a high Li+ transference number, estimated via the potentiostatic polarization method (tPPLi = 0.90). Dynamic ion correlation studies suggested that the high tPPLi could be mainly ascribed to the strongly coupled Li+-anion motions in the electrolytes. Furthermore, high-energy X-ray total scattering measurements combined with all-atom molecular dynamics simulations showed that Li+ ions and [TFA] anions aggregated into ionic clusters with a relatively long-range ion-ordered structure. Therefore, the collective motions of the Li ions and anions in the form of highly aggregated ion clusters, which likely diminish rather than enhance ionic conductivity, play a significant role in achieving high tPPLi in liquid electrolytes. Based on the dynamic ion correlations, a potential design approach is discussed to accomplish single-ion conducting liquid electrolytes with high ionic conductivity.
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| http://dx.doi.org/10.1039/d0cp06381a | DOI Listing |
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