用于固态锂离子电池的基于高介电聚偏二氟乙烯共聚物的高性能三元固体聚合物电解质,ACS Applied Materials & Interfaces

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用于固态锂离子电池的基于高介电聚偏二氟乙烯共聚物的高性能三元固体聚合物电解质
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-06-28 , DOI: 10.1021/acsami.3c03361
João C Barbosa _{1,

2} , Daniela M Correia ₃ , Arkaitz Fidalgo-Marijuan _{4,

5} , Renato Gonçalves ₃ , Stanislav Ferdov ₁ , Verónica de Zea Bermudez _{2,

6} , Senentxu Lanceros-Mendez _{1,

4,

7} , Carlos M Costa _{1,

8}

Affiliation

可再生能源需要高效的储能系统。锂离子电池在这些系统中脱颖而出，但安全性和循环稳定性问题仍需改进。这可以通过采用固体聚合物电解质（SPE）代替通常使用的分离器/电解质系统来实现。因此，基于聚偏二氟乙烯-co的三元SPE被开发出来。-六氟丙烯）（PVDF-HFP）和聚（偏二氟乙烯-三氟乙烯-氯氟乙烯），P（VDF-TrFE-CFE）作为主体聚合物，添加斜发沸石（CPT）沸石以稳定电池循环性能，以及离子液体（IL） (1-丁基-3-甲基咪唑鎓硫氰酸盐([BMIM][SCN]))、1-甲基-1-丙基吡咯烷鎓双(三氟甲基磺酰基)亚胺([PMPyr][TFSI])或双(三氟甲磺酰基)亚胺锂(LiTFSI)，加入以增加离子电导率。样品通过刮刀处理并在 160 °C 下蒸发溶剂。聚合物基体和填料的性质影响样品的形貌和机械性能，并对离子电导率值、电化学窗口稳定性和锂迁移数等电化学参数发挥重要作用。PVDF-HFP-CPT-[PMPyr][TFSI] 样品获得^–5 S cm ^{–1 ) 和锂迁移数 (0.59)。}C/10 充放电电池测试显示出优异的电池性能，无论使用何种聚合物基质和 IL，50 次循环后电池容量均为 150 mAh g ^{–1 。}在倍率性能测试中，最好的 SPE 是基于 P(VDF-TrFE-CFE) 主体聚合物的 SPE，其倍率放电值为 98.7 mAh g ^–1，因为它促进离子解离。该研究首次证明了P(VDF-TrFE-CFE)作为SPE在锂离子电池中的适用性，显示了在三元配方中正确选择聚合物基体、IL类型和锂盐的相关性SPE，以优化固态电池性能。特别是，必须强调IL提供的离子电导率的增强以及高介电常数聚合物P(VDF-TrFE-CFE)在改善电池在宽放电倍率范围内的循环性能方面的作用。

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High Performance Ternary Solid Polymer Electrolytes Based on High Dielectric Poly(vinylidene fluoride) Copolymers for Solid State Lithium-Ion Batteries

Renewable energy sources require efficient energy storage systems. Lithium-ion batteries stand out among those systems, but safety and cycling stability problems still need to be improved. This can be achieved by the implementation of solid polymer electrolytes (SPE) instead of the typically used separator/electrolyte system. Thus, ternary SPEs have been developed based on poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) and poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene), P(VDF-TrFE-CFE) as host polymers, clinoptilolite (CPT) zeolite added to stabilize the battery cycling performance, and ionic liquids (ILs) (1-butyl-3-methylimidazolium thiocyanate ([BMIM][SCN])), 1-methyl-1-propylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([PMPyr][TFSI]) or lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), incorporated to increase the ionic conductivity. The samples were processed by doctor blade with solvent evaporation at 160 °C. The nature of the polymer matrix and fillers affect the morphology and mechanical properties of the samples and play an important role in electrochemical parameters such as ionic conductivity value, electrochemical window stability, and lithium-transference number. The best ionic conductivity (4.2 × 10^–5 S cm^–1) and lithium transference number (0.59) were obtained for the PVDF-HFP-CPT-[PMPyr][TFSI] sample. Charge–discharge battery tests at C/10 showed excellent battery performance with values of 150 mAh g^–1 after 50 cycles, regardless of the polymer matrix and IL used. In the rate performance tests, the best SPE was the one based on the P(VDF-TrFE-CFE) host polymer, with a discharge value at C-rate of 98.7 mAh g^–1, as it promoted ionic dissociation. This study proves for the first time the suitability of P(VDF-TrFE-CFE) as SPE in lithium-ion batteries, showing the relevance of the proper selection of the polymer matrix, IL type, and lithium salt in the formulation of the ternary SPE, in order to optimize solid-state battery performance. In particular, the enhancement of the ionic conductivity provided by the IL and the effect of the high dielectric constant polymer P(VDF-TrFE-CFE) in improving battery cyclability in a wide range of discharge rates must be highlighted.

更新日期：2023-06-28

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