Local Structural Analysis of Sulfide Polymer Electrolytes Prepared via I2-Induced Polymerization of Li3PS4
Local Structural Analysis of Sulfide Polymer Electrolytes Prepared via I2-Induced Polymerization of Li3PS4
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通过 I2 诱导聚合 Li3PS4 制备的硫化物聚合物电解质的局部结构分析
DOI：
10.1021/acs.jpcc.2c09078
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Ohara Koji
中科院分区：
文献类型：
--
作者：
Hiroi Satoshi;Utsuno Futoshi;Higuchi Hiroyuki;Kato Atsutaka;Yamamoto Mari;Takahashi Masanari;Ohara Koji
为了避免全固态电池在充放电过程中与电极活性材料相关的体积变化，必须开发一种有效的粘合剂，以改善固体电解质和电极活性材料之间的接触。为此，硫化固体电解质li3ps4的聚合提供了一条很有前途的途径。然而，所得到的固体电解质的局部结构，即LiI晶体和玻璃状硫化物聚合物的混合物，需要被阐明，以进一步开发硫化物聚合物作为粘合剂。本文通过x射线全散射的微分对分布函数分析，分析了分离混合物的局部结构。在玻璃相中，ps4阴离子之间存在二硫键。二硫键配位数为0.65，每个ps4四面体与两个四面体相连，形成含有Li离子的（−P-S-S -）非键聚合物链结构。玻璃相中围绕ps4阴离子的Li离子配位数远小于纯li3ps4玻璃中的配位数。该聚合物可作为锂离子导电粘合剂应用于具有低电阻和高容量保持的片状全固态电池中。
To avoid the volume change associated with the electrode active material during charge/discharge in all-solid-state batteries, an effective binder that improves the contact between the solid electrolyte and the electrode active material must be developed. To this aim, the polymerization of the sulfide solid electrolyte Li3PS4offers a promising route. However, the local structure of the resulting solid electrolyte, i.e., a mixture of LiI crystals and glassy sulfide polymers, needs to be elucidated for further development of sulfide polymers as binders. Herein, we analyze the local structure of the isolated mixture via a differential pair distribution function analysis using X-ray total scattering. The presence of disulfide bonds between PS4anions is confirmed in the glassy phase. The coordination number of the disulfide bonds is 0.65, and each PS4tetrahedron is connected to two tetrahedrons to form a polymer chain structure of (−P–S–S−)nbonds containing Li ions. The coordination number of Li ions surrounding PS4anions in the glassy phase is much smaller than that in the pure Li3PS4glasses. This polymer may find application as a Li-ion conductive binder in sheet-type all-solid-state batteries having low resistance and high capacity retention.
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