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Glass Transition Temperature and Ion Binding Determine Conductivity and Lithium–Ion Transport in Polymer Electrolytes

机译:玻璃化转变温度和离子结合确定聚合物电解质中的电导率和锂离子输送

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摘要

Polymer electrolytes with high Li~(+)-ion conductivity provide a route toward improved safety and performance of Li~(+)-ion batteries. However, most polymer electrolytes suffer from low ionic conduction and an even lower Li~(+)-ion contribution to the conductivity (the transport number, t _(+)), with the anion typically transporting over 80% of the charge. Here, we show that subtle and potentially undetected associations within a polymer electrolyte can entrain both the anion and the cation. When removed, the conductivity performance of the electrolyte can be improved by almost 2 orders of magnitude. Importantly, while some of this improvement can be attributed to a decreased glass transition temperature, T _(g), the removal of the amide functional group reduces interactions between the polymer and the Li~(+) cations, doubling the Li~(+)t _(+) to 0.43, as measured using pulsed-field-gradient NMR. This work highlights the importance of strategic synthetic design and emphasizes the dual role of T _(g) and ion binding for the development of polymer electrolytes with increased total ionic conductivity and the Li~(+) ion contribution to it.
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