Structure of the polymer electrolyte poly(ethylene oxide)6:LiAsF6

环氧乙烷 电解质 聚合物 氧化物 锂(药物) 电导率 材料科学 快离子导体 摩尔质量 晶体结构 化学 化学工程 高分子化学 结晶学 离子电导率 无机化学 物理化学 有机化学 共聚物 内分泌学 工程类 医学 电极
作者
Graham S. MacGlashan,Yuri G. Andreev,Peter G. Bruce
出处
期刊:Nature [Nature Portfolio]
卷期号:398 (6730): 792-794 被引量:447
标识
DOI:10.1038/19730
摘要

Polymer electrolytes—salts (such as LiCF3SO3) dissolved in solid, high-molar-mass polymers (for example, poly(ethylene oxide), PEO)1,2,3—hold the key to the development of all-solid-state rechargeable lithium batteries4. They also represent an unusual class of coordination compounds in the solid state5. Conductivities of up to 10−4 S cm−1 may be obtained, but higher levels are needed for applications in batteries5,6,7. To achieve such levels requires a better understanding of the conduction mechanism, and crucial to this is a knowledge of polymer-electrolyte structure. Crystalline forms of polymer electrolytes are obtained at only a few discrete compositions. The structures of 3 : 1 and 4 : 1 complexes (denoting the ratio of ether oxygens to cations) have been determined5,8,9. But the 6 : 1 complex is of greater interest as the conductivity of polymer electrolytes increases significantly on raising the polymer content from 3 : 1 to 6 : 1 (refs 10, 11). Furthermore, many highly conducting polymer-electrolyte systems form crystalline 6 : 1 complexes whereas those with lower conductivities do not. Here we report the structure of the PEO:LiAsF6 complex with a 6 : 1 composition. Determination of the structure was carried out abinitio by employing a method for flexible molecular structures, involving full profile fitting to the X-ray powder diffraction data by simulated annealing12. Whereas in the 3 : 1 complexes the polymer chains form helices, those in the 6 : 1 complex form double non-helical chains which interlock to form a cylinder. The lithium ions reside inside these cylinders and, in contrast to other complexes, are not coordinated by the anions.
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