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Polymer Electrolytes Containing Solvate Ionic Liquids: A New Approach To Achieve High Ionic Conductivity, Thermal Stability, and a Wide Potential Window
Chemistry of Materials ( IF 8.6 ) Pub Date : 2017-12-26 00:00:00 , DOI: 10.1021/acs.chemmater.7b04274
Yuzo Kitazawa 1 , Kaori Iwata 1 , Ryosuke Kido 1 , Satoru Imaizumi 1 , Seiji Tsuzuki 2 , Wataru Shinoda 3 , Kazuhide Ueno 1 , Toshihiko Mandai 4 , Hisashi Kokubo 1 , Kaoru Dokko 1 , Masayoshi Watanabe 1
Affiliation  

We describe here the electrochemical properties and battery performance of polymer electrolytes composed of ABA-triblock copolymers and Li-glyme solvate ionic liquids (SILs), which consist of the [Li(glyme)]+ complex cation and bis(trifluoromethanesulfoly)amide ([TFSA]) anion, to simultaneously achieve high ionic conductivity, thermal stability, and a wide potential window. Three different block copolymers, consisting of a SIL-incompatible A segment (polystyrene, PSt) and SIL-compatible B segments (poly(methyl methacrylate) (PMMA), poly(ethylene oxide) (PEO), and poly(butyl acrylate) (PBA)) were synthesized. The SILs were solidified with the copolymers through physical cross-linking by the self-assembly of the PSt segment. The thermal and electrochemical properties of the polymer electrolytes were significantly affected by the stability of the [Li(glyme)]+ complex in the block copolymer B segments, and the preservation of the SILs contributed to their thermal stabilities and oxidation stabilities greater than 4 V vs Li/Li+. Pulsed-field gradient spin–echo nuclear magnetic resonance measurements of the polymer electrolytes and molecular dynamics simulation indicate that the [Li(glyme)]+ complex cation is unstable in the PEO matrix because of the competitive coordination of the PEO chain and glyme with Li+. On the other hand, the complex structure of [Li(glyme)]+ is stable in the PMMA- and PBA-based polymer electrolytes because of the weak interaction between Li+ and the polymer chains. By use of the PMMA- and PBA-based polymer electrolytes, 4-V class Li batteries with a LiCoO2 cathode and a Li metal anode could be operated stably at 60 °C; in contrast, this was not possible using the PEO-based electrolyte.

中文翻译:

包含溶剂化离子液体的聚合物电解质:一种实现高离子电导率,热稳定性和宽电位窗的新方法

我们在这里描述由ABA-三嵌段共聚物和Li-甘醇二甲酸酯离子液体(SILs)组成的聚合物电解质的电化学性能和电池性能,该电解质由[Li(glyme)] +络合阳离子和双(三氟甲磺酰胺)酰胺([ TFSA] -)阴离子,以同时实现高离子电导率,热稳定性和宽电位窗。三种不同的嵌段共聚物,由SIL不相容的A链段(聚苯乙烯,PSt)和SIL相容的B链段(聚甲基丙烯酸甲酯(PMMA),聚环氧乙烷(PEO)和聚丙烯酸丁酯)组成(合成)。通过PSt链段的自组装,通过物理交联将SIL与共聚物固化。聚合物电解质的热和电化学性质受到嵌段共聚物B段中[Li(glyme)] +配合物的稳定性的显着影响,并且SIL的保存有助于其热稳定性和大于4 V的氧化稳定性vs李/李+。聚合物电解质的脉冲场梯度自旋回波核磁共振测量和分子动力学模拟表明,由于PEO链和乙二醇与锂的竞争性配位,PEO基质中的[Li(glyme)] +复合阳离子不稳定。+。另一方面,由于Li +与聚合物链之间的弱相互作用,[Li(glyme)] +的复杂结构在基于PMMA和PBA的聚合物电解质中是稳定的。通过使用基于PMMA和PBA的聚合物电解质,具有LiCoO 2阴极和Li金属阳极的4-V级Li电池可以在60°C的温度下稳定运行。相反,使用基于PEO的电解质是不可能的。
更新日期:2017-12-26
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