Three-dimensional porous ceramic framework reinforcing composite electrolyte

Cui Long-Fei; Ju Jiang-Wei; Cui Guang-Lei

doi:10.7498/aps.69.20201552

Abstract

All solid-state lithium batteries demonstrate excellent characteristics of high safety and energy density, which make them very promising energy storage devices. Among various kinds of solid electrolytes, rigid-flexible coupling composite electrolyte combines the advantages of rigid solid inorganic ceramic electrolytes, i.e., excellent room temperature ionic conductivity, and of flexible solid polymer electrolytes, i.e., the flexibility, and thereby is considered to be one of the most ideal electrolyte candidates for all solid-state lithium batteries. Dispersing 0- or 1-dimensional inorganic fillers is a widespread method to fabricate rigid-flexible coupling composite, where the ionic conductivity of polymer can be improved by one order of magnitude mainly due to the decreased degree of crystallinity. However, aim to further increase the ionic conductivity by increasing the filler content cannot be accomplished because of the fillers' tendency to aggregation. what's more, the highly conductive inorganic fillers are separated by the polymer phase and thus cannot form fast and continuous Li⁺ transportation channels. Accordingly, inorganic fillers which can provide percolated pathway for Li⁺ transportation and avoid aggregating are highly desirable. To this end, different from adding 0- or 1-dimensional inorganic fillers into polymer matrices, polymers can be cast into porous inorganic substrates, that is, 3-dimensional porous ceramic framework, to obtain organic-inorganic composite electrolyte, in which organic phase, inorganic phase, and organic/inorganic interfacial phase are all continuous for fast Li⁺ transportation. And meanwhile, its self-supported structure prevents the agglomeration of inorganic particles. In recent years, the 3-dimensional porous ceramic framework has been more and more frequently used in rigid-flexible coupling composite electrolytes. To have a deep insight into the positive function of 3-dimensional porous ceramic framework, in this review, we firstly reveal the mechanism of the huge improvement in the ionic conductivity and thermostability of the composite electrolyte. Then, we summarize the frequently used preparation methods of the 3-dimensional porous ceramic framework reported recently. Finally, for the future perspective of rigid-flexible coupling composite electrolyte development, we propose two feasible improvement strategies. This review can thereby provide great significance of designing solid electrolytes with comprehensive performance for all solid-state lithium batteries with high energy density and superior safety.

Keywords:

Authors and contacts

1.
Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China
2.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Cui Guang-Lei, cuigl@qibebt.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51902325)

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References

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Cited By

图 1 三维骨架在锂电池中的应用发展历史概览^[29-39]

Figure 1. Development history of three-dimensional framework in lithium battery^[29-39].

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图 2 三维多孔陶瓷骨架增强的复合电解质概览^[41-44]

Figure 2. Overview of the three-dimensional porous ceramic framework reinforcing composite electrolyte^[41-44].

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图 3 刚柔并济的有机-无机复合电解质的不同微观结构及其锂离子传输通道的示意图^[41]　(a) 单相传输: 有机相连续; (b) 双相传输: 有机相、有机/无机界面相连续; (c) 三相传输: 无机相、有机相、有机/无机界面相连续

Figure 3. Schematic view of rigid-flexible coupling composites with different microstructures and various Li⁺ transportation pathway^[41]: (a) Single-phase percolation: percolated organic phase; (b) double-phase percolation: percolated organic and organic/inorganic interfacial phase; (c) triple-phase percolation: percolated organic, inorganic, and organic/inorganic interfacial phase.

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图 4 不同固态电解质离子电导率及提升因子的比较^{[23-27,42,48-50]}. 提升因子: 复合电解质电导率与聚合物电导率之比

Figure 4. Ionic conductivity and the promotion factor comparison of different solid electrolytes^{[23-27,42,48-50]}. The promotion factor is defined as the ratio of the conductivity of composite to the conductivity of polymer.

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图 5 (a) 以零维颗粒和三维骨架为无机填料的复合电解质在400 ℃下加热2 h前后对比图^[48]; (b) 150 ℃加热3 h对具有三维骨架的复合电解质(上)和纯聚合物电解质(下)进行加热测试^[55]

Figure 5. (a) Photographs of composite electrolytes with 0 dimensional particles and three dimensional framework before and after heating at 400 ℃ for 2 h^[48]; (b) heating experiments operated at 150 ℃ for 3 h on the three dimensional composite electrolyte (top) and pure polymer electrolyte (bottom)^[55].

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图 6 (a) 以零维颗粒和三维骨架为无机填料的复合电解质进行燃烧测试^[38]; (b) 对商用隔膜和具有三维骨架的复合电解质进行燃烧测试^[43]

Figure 6. (a) Flammability test of composite electrolytes with 0-dimensional particles and three-dimensional framework^[38]; (b) flammability test of commercial separator and composite electrolyte with three-dimensional framework^[43].

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图 7 模板法制备三维骨架　(a) 以细菌纤维素为模板制备三维骨架的合成过程示意图^[49]; (b) 以海绵作为模板制备三维骨架的合成过程示意图^[53]; (c) 采用Li_6.4La₃Zr₂Al_0.2O₁₂/PEO的LiFePO₄-Li全固态电池在0.2 C下的循环性能^[53]

Figure 7. Template method to prepare three-dimensional skeleton: (a) Schematic demonstrating of the procedure to prepare three-dimensional skeleton with bacteria cellulose as a template^[49]; (b) schematic illustration for the synthesis of three-dimensional skeleton with sponge as a template^[53]; (c) cycle performance of LiFePO₄|Li_6.4La₃Zr₂Al_0.2O₁₂/PEO|Li battery at 0.2 C^[53].

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图 8 (a) 静电纺丝陶瓷-聚乙烯吡咯烷酮纳米纤维的装置示意图^[38]; (b) 静电纺丝法制备纤维增强的聚合物电解质示意图^[38]; (c) 纺织纳米纤维网络的扫描电子显微镜图像^[38]; (d) 三维骨架网络的扫描电子显微镜图像^[38]; (e) 溶液喷涂法制备复合电解质膜示意图^[51]

Figure 8. (a) Schematic setup of electrospinning garnet-PVP nanofibers^[38]; (b) schematic procedure to fabricate the FRPC lithium-ion–conducting membrane^[38]; (c) SEM images of the as-spun nanofiber network^[38]; (d) SEM image of the garnet nanofiber network^[38]; (e) schematic illustration of the fabrication procedure of the composite electrolyte film prepared by solution spraying method^[51].

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图 9 (a) 溶胶–凝胶法制备复合电解质的示意图^[42]; (b) 3D打印法制备复合电解质的示意图及各阶段相应的SEM图像^[52]

Figure 9. (a) Schematic representation of the synthesis of composite electrolytes generated by sol-gel method^[42]; (b) schematic of the templating procedure used for the synthesis of structured composite electrolyte, generated by 3D printing. Corresponding SEM images of each synthesis stage are included below each schematic^[52].

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表 1 不同方法制备三维骨架的优缺点

Table 1. Advantages and disadvantages of three-dimensional framework prepared by different methods.

常用制备方法	优点	缺点	文献
模板法	工艺简单、成本低、可大批量制备	微观形貌受限于模板	[28,49,53]
静电纺丝法	可调控三维骨架的微观形貌	调控精度低、操作过程复杂	[38,55]
溶液喷涂法	可调控三维骨架的厚度、无机相占比较大	工艺繁琐、机械性能差	[51]
溶胶-凝胶法	工艺简便、三维骨架孔隙率大	微观形貌难以调控	[42]
流延成型法	可制备薄的三维骨架、可调控厚度	所需粘结剂浓度高	[56-58]
3D打印法	可较精准地调控三维骨架微观形貌	成本高、制备过程繁琐	[52]

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[26]	Ban X Y, Zhang W Q, Chen N, Sun C W 2018 J. Phys. Chem. C 122 9852 Google Scholar
[27]	Li D, Chen L, Wang T S, Fan L Z 2018 ACS Appl. Mater. Interfaces 10 7069 Google Scholar
[28]	Li Z, Sha W X, Guo X 2019 ACS Appl. Mater. Interfaces 11 26920 Google Scholar
[29]	Kotobuki M, Suzuki Y, Munakata H, Kanamura K, Sato Y, Yamamoto K, Yoshida T 2010 J. Electrochem. Soc. 157 A493 Google Scholar
[30]	Gowda S R, Reddy A L M, Shaijumon M M, Zhan X B, Ci L J, Ajayan P M 2011 Nano Lett. 11 101 Google Scholar
[31]	Xie X, Hu L B, Pasta M, Wells G F, Kong D, Criddle C S, Cui Y 2011 Nano Lett. 11 291 Google Scholar
[32]	Jia H P, Gao P F, Yang J, Wang J L, Nuli Y, Yang Z 2011 Adv. Energy Mater. 1 1036 Google Scholar
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