文章基本信息

标题：Small Groups, Big Impact: Eliminating Li + Traps in Single-Ion Conducting Polymer Electrolytes
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作者：Kristina Borzutzki ; Dengpan Dong ; Christian Wölke 等
期刊名称：iScience
印刷版ISSN：2589-0042
出版年度：2020
卷号：23
期号：8
页码：1-43
DOI：10.1016/j.isci.2020.101417
语种：English
出版社：Elsevier
摘要：SummarySingle-ion conducting polymer electrolytes exhibit great potential for next-generation high-energy-density Li metal batteries, although the lack of sufficient molecular-scale insights into lithium transport mechanisms and reliable understanding of key correlations often limit the scope of modification and design of new materials. Moreover, the sensitivity to small variations of polymer chemical structures (e.g., selection of specific linkages or chemical groups) is often overlooked as potential design parameter. In this study, combined molecular dynamics simulations and experimental investigations reveal molecular-scale correlations among variations in polymer structures and Li+transport capabilities. Based on polyamide-based single-ion conducting quasi-solid polymer electrolytes, it is demonstrated that small modifications of the polymer backbone significantly enhance the Li+transport while governing the resulting membrane morphology. Based on the obtained insights, tailored materials with significantly improved ionic conductivity and excellent electrochemical performance are achieved and their applicability in LFP||Li and NMC||Li cells is successfully demonstrated.Graphical AbstractDisplay OmittedHighlights•Relations between polymer structure and charge transport properties are revealed•Identification of Li+“traps” in the polymer by combined MD simulations and experiments•Duplication of ionic conductivity by reduction of the polymer backbone•Change in membrane morphology by variation of a chemical group in the polymer backbonePolymer Chemistry; Electrochemical Energy Storage; Polymers