功能硅烷在有机-无机复合固态电解质中的应用研究进展

doi:10.11949/0438-1157.20210327

摘要/Abstract

摘要：

有机-无机复合固态电解质不仅具有聚合物电解质的柔韧性和界面相容性，还能显著提高离子传导性和力学性能。然而，构建良好的填料/聚合物分散体系是制备此类复合电解质的难点，设计新型有强相互作用的功能化填料以调控界面渗流结构也面临巨大挑战。通过功能硅烷对无机填料进行化学键联改性或原位合成是解决无机填料与聚合物间分散性和界面相容性问题的有效策略。本文综述了在复合固态电解质中利用功能硅烷对无机填料进行表面改性和原位合成、功能硅烷作为复合固态电解质的交联中心和制备离子胶类复合固态电解质四方面的研究进展，重点阐述了硅烷功能化填料与固态电解质结构和性能之间的关系。最后对功能硅烷在有机-无机复合固态电解质中的应用研究进行了总结和展望。

关键词: 有机-无机复合固态电解质, 功能硅烷, 纳米填料, 表面改性, 原位合成, 离子胶

Abstract:

The organic-inorganic composite solid electrolyte not only has the advantages of polymer electrolyte with high flexibility and interface compatibility, but also possesses the merits of improved ionic conductivity and mechanical properties. However, it is difficult to construct a highly dispersive system for the preparation of such composite electrolytes, and it is also a great challenge to regulate the interfacial percolation structure of inorganic fillers with strong molecular interaction. Chemical modification or in-situ synthesis of inorganic fillers by functional organosilane is an effective strategy to solve the problems mentioned above. In this review, the research progress of using functional organosilane for organic-inorganic composite solid electrolytes through surface modification, in-situ synthesis of inorganic fillers, as cross-linking center, or preparation of ionogel based composite solid electrolytes are summarized in detail. The relationship between the organosilane functionalized fillers and the structure/properties of solid electrolytes are disclosed. Finally, the future application of functional organosilane in organic-inorganic composite solid electrolytes is summarized and prospected.

Key words: organic-inorganic composite solid electrolyte, functional organosilane, nano-filler, surface modification, in situ synthesis, ionogels

中图分类号:

O 646

唐子龙,肖凡凡,尹玉华,李森雨,汪靖伦. 功能硅烷在有机-无机复合固态电解质中的应用研究进展[J]. 化工学报, 2021, 72(10): 5002-5015.

Zilong TANG,Fanfan XIAO,Yuhua YIN,Senyu LI,Jinglun WANG. Recent advances in application of functional organosilane for organic-inorganic composite solid electrolyte[J]. CIESC Journal, 2021, 72(10): 5002-5015.

图/表 11

图1 各类固态电解质性能对比雷达图（a）[5]和相关研究论文增长趋势图（b）

Fig.1 The radar chart of various solid electrolytes (a) [5] and the research growth trend of reported articles(b)

图2 接枝和共接枝纳米SiO2或Al2O3 的制备路线[41]

Fig.2 Synthetic route to obtain grafted and co-grafted SiO2 or Al2O3 nanoparticles[41]

图3 PEO/FMS-TFSISPE复合固态电解质合成示意图[42]

Fig.3 Schematic synthetic route of a single-ion conducting nanohybrid solid polymer electrolyte (PEO/FMS-TFSISPE) [42]

图4 离子键(IBN)和共价键修饰(CBN)纳米SiO2合成路线[43]

Fig.4 Schematic illustration of the preparation procedure of IBNs and CBNs[43]

图5 PEO/PEG-LGPS复合固态电解质制备路线图[19]

Fig.5 Schematic illustration of the as prepared PEO/PEG-LGPS structure[19]

图6 原位水解制备复合固态电解质和分子间相互作用机理示意图[30]

Fig.6 In-situ preparation of PEO-SiO2 composite electrolyte and schematic representation of molecular interaction[30]

图7 PEO/LiClO4@SiO2复合固态电解质膜的合成路线[52]

Fig. 7 Synthetic routes of the PEO/LiClO4@SiO2 composite polymer electrolytes membrane[52]

图8 ORMOCERs复合固态电解质的制备[53]

Fig.8 The preparation of ORMOCERs composite solid electrolyte[53]

图9 POSS/PEO交联复合固态电解质的制备过程[58]

Fig.9 The preparation of POSS/PEO based composite solid electrolyte[58]

图10 离子胶类复合固态电解质微观结构示意图[70]（1 ? =0.1 nm）

Fig.10 Microstructure of ionogel based composite solid electrolyte[70]

表1 功能硅烷化学结构及在复合固态电解质中应用

Table 1 Chemical structure of functional silane and its application in composite solid electrolyte

复合固态电解质	离子电导率/(S/cm)	功能硅烷化学式	功能硅烷作用	文献
原位制备SiO₂复合PEO基固态电解质	4.4×10^-5@30℃	(C₂H₅O)₄Si	高分散性	[30]
聚乙二醇基三维交联复合电解质	8.0×10^-5@room temp.	(C₂H₅O)₃Si(CH₂)₃OCH₂(CHCH₂O)	交联中心	[55]
丙烯酸酯交联SiO₂复合丁二腈基固态电解质	7.0×10^-4@25℃	(C₂H₅O)₃SiCH $? ??????$ CH₂	交联中心	[59]
接枝改性SiO₂复合聚乙烯醇基复合电解质	1.5×10^-4@25℃	(C₂H₅O)₃SiCH₂CH₂CH₂NH₂	化学键联	[56]
接枝改性Al₂O₃复合PEO基复合电解质	1.9×10^-4@70℃	(CH₃O)₃Si(CH₂)₃O(CH₂CH₂O)_nCH₃(n=6~9)	化学键联	[41]
离子键修饰SiO₂复合PEO基固态电解质	3.6×10^-5@30℃	(C₂H₅O)₃SiCH₂CH₂CH₂SH	化学键联	[44]
离子胶类固态电解质	3.2×10^-3@30℃	(C₂H₅O)₄Si	离子胶	[71]
SiO₂复合PEO基复合电解质	2.0×10^-6@30℃	物理混合，无硅烷功能化	—	[40]
Al₂O₃复合PEO基复合电解质	1.0×10^-6@30℃	物理混合，无硅烷功能化	—	[38]

表1 功能硅烷化学结构及在复合固态电解质中应用

Table 1 Chemical structure of functional silane and its application in composite solid electrolyte

复合固态电解质	离子电导率/(S/cm)	功能硅烷化学式	功能硅烷作用	文献
原位制备SiO₂复合PEO基固态电解质	4.4×10^-5@30℃	(C₂H₅O)₄Si	高分散性	[30]
聚乙二醇基三维交联复合电解质	8.0×10^-5@room temp.	(C₂H₅O)₃Si(CH₂)₃OCH₂(CHCH₂O)	交联中心	[55]
丙烯酸酯交联SiO₂复合丁二腈基固态电解质	7.0×10^-4@25℃	(C₂H₅O)₃SiCH $? ??????$ CH₂	交联中心	[59]
接枝改性SiO₂复合聚乙烯醇基复合电解质	1.5×10^-4@25℃	(C₂H₅O)₃SiCH₂CH₂CH₂NH₂	化学键联	[56]
接枝改性Al₂O₃复合PEO基复合电解质	1.9×10^-4@70℃	(CH₃O)₃Si(CH₂)₃O(CH₂CH₂O)_nCH₃(n=6~9)	化学键联	[41]
离子键修饰SiO₂复合PEO基固态电解质	3.6×10^-5@30℃	(C₂H₅O)₃SiCH₂CH₂CH₂SH	化学键联	[44]
离子胶类固态电解质	3.2×10^-3@30℃	(C₂H₅O)₄Si	离子胶	[71]
SiO₂复合PEO基复合电解质	2.0×10^-6@30℃	物理混合，无硅烷功能化	—	[40]
Al₂O₃复合PEO基复合电解质	1.0×10^-6@30℃	物理混合，无硅烷功能化	—	[38]

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