Electronic‐rich functional groups and flexible segments have long been perceived to be the decisive factors influencing lithium‐ion transfer in polymer electrolytes, while crystallinity is regarded as the great scourge. Actually, the research on the influence of crystalline phase and crystalline plane is still in scarcity. Herein, taking poly(vinylidene fluoride)‐hexafluoropropylene (PVDF‐HFP) as an example, new (111/201) crystal planes (belonged to β‐phase) are regulated by dissolving process and clarified by Synchrotron radiation X‐ray diffraction and X‐ray diffraction. Density functional theory calculation indicates that the newly exposed (111/201) crystal planes provide higher binding energy with lithium ions and are conducive to provide more ion transport channels.7Li nuclear magnetic resonance of new crystalline planes contained PVDF‐HFP based electrolyte shows lower field and sharper peak intensity, further proves the rapid lithium ion transfer. Therefore, a high ionic conductivity of 6.42×10−4 S cm−1 and a large lithium‐ion transfer number of 0.7 are achieved. This study offers a new insight into the influence of crystalline phase and crystalline plane on the transfer of lithium ion for polymer electrolytes.

中文翻译：

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调节聚合物电解质的结晶相/晶面以实现快速锂离子转移


长期以来，富含电子的官能团和柔性链段一直被认为是影响聚合物电解质中锂离子转移的决定性因素，而结晶度则被认为是最大的祸害。实际上，关于晶相和晶面影响的研究仍然很少。本文以聚偏二氟乙烯-六氟丙烯 （PVDF-HFP） 为例，新的（111/201）晶面（属于β相）通过溶解过程进行调节，并通过同步辐射 X 射线衍射和 X 射线衍射进行澄清。密度泛函理论计算表明，新暴露的 （111/201） 晶面与锂离子的结合能更高，有利于提供更多的离子传输通道.7 含有 PVDF-HFP 基电解质的新晶面的 Li 核磁共振显示出更低的磁场和更尖锐的峰强度，进一步证明了锂离子的快速转移。因此，实现了 6.42×10-4 S cm-1 的高离子电导率和 0.7 的大锂离子转移数。这项研究为晶相和晶面对聚合物电解质锂离子转移的影响提供了新的见解。