硫化物电解质的界面调控及研究进展

doi:10.11949/0438-1157.20250416

摘要/Abstract

摘要：

全固态锂电作为下一代高能量密度、高安全性能储能器件，其核心固态电解质的研究备受关注。硫化物固态电解质凭借超高的离子电导率、优异的机械性能以及较好的界面兼容性，展现出显著的产业化潜力。然而，硫化物电解质仍面临空气稳定性差、界面副反应及锂枝晶生长等挑战。系统综述了硫化物基固态电解质的分类及其结构特性，深入分析了空气稳定性和电化学稳定性失效机制并总结优化策略。最后，针对规模化制备、界面优化及薄层电解质开发等关键问题，提出了未来研究方向，为硫化物电解质的实用化提供理论参考。

关键词: 全固态电池, 固态电解质, 硫化物电解质, 硫化物, 电极

Abstract:

All-solid-state lithium batteries, as the next-generation high-energy-density and high-safety-performance energy storage devices, have drawn significant attention to the research of their core solid-state electrolytes. Sulfide solid-state electrolytes, with their ultra-high ionic conductivity, excellent mechanical properties, and good interface compatibility, have shown remarkable industrialization potential. However, sulfide electrolytes still face challenges such as poor air stability, interfacial side reactions, and lithium dendrite growth. This paper systematically reviews the classification and structural characteristics of sulfide-based solid-state electrolytes, deeply analyzes the failure mechanisms of air stability and electrochemical stability, and summarizes the optimization strategies. Finally, it proposes future research directions for key issues such as large-scale preparation, interface optimization, and thin-layer electrolyte development, providing theoretical references for the practical application of sulfide electrolytes.

Key words: all-solid-state battery, solid electrolyte, Sulfide electrolyte, Sulfide, electrode

中图分类号:

TQ 152

徐彦芹, 蔡文静. 硫化物电解质的界面调控及研究进展[J]. 化工学报, DOI: 10.11949/0438-1157.20250416.

Wenjing CAI, Yanqin XU. Interface Regulation and Research Progress of Sulfide Electrolytes[J]. CIESC Journal, DOI: 10.11949/0438-1157.20250416.

图/表 5

表1 常见硫化物电解质及其离子电导率

Table 1 Common sulfide electrolytes and their ionic conductivity

体系类别	电解质	离子电导率/(S·cm^-1)	出处
Li-P-S	Li₇P₃S₁₁	3.2×10^-3	^[22]
	Li₇P₃S₁₁	1.7×10^-2	^[23]
	β-Li₃PS₄	1.6×10^–4	^[24]
Thio-LISICON	Li₄SnS₄	7.0×10^-5	^[25]
	Li_3.25Ge_0.25P_0.75S_3.25	2.2×10^-3	^[26]
LGPS	Li₁₀SiP₂S₁₂	2.3×10^-3	^[27]
	Li₁₀SnP₂S₁₂	4×10^-3	^[28]
	Li₁₀GeP₂S₁₂	1.2×10^-2	^[26]
	Li_9.54Si_1.74P_1.44S_11.7Cl_0.3	2.5×10^-2	^[29]
	Li_9.54(Si_0.6Ge_0.4)_1.74P_1.44S_11.1Br_0.3O_0.6	3.2×10^-2	^[5]
硫银锗矿型	Li₆PS₅Cl	4.9×10^-3	^[30]
	Li₆PS₅Br	2.6×10^-3	^[31]
	Li₆PS₅I	10^-7	^[32]
	Li_5.5PS_4.5Cl_1.5	9.4×10^-3	^[33]
	Li_6.6Sb_0.4Si_0.6S₅I	1.48×10^-2	^[34]

图1 (a) Li10GeP2S12结构及传导途径；(b) Li9.54Si1.74P1.44S11.7Cl0.3结构；注:(c) Li9.54(Si0.6Ge0.4)1.74P1.44S11.1Br0.3O0.6 structure[5, 26, 29](c) Li9.54(Si0.6Ge0.4)1.74P1.44S11.1Br0.3O0.6结构[5, 26, 29]

Fig.1 (a) The structure and conduction pathway of Li10GeP2S12; (b) Li9.54Si1.74P1.44S11.7Cl0.3 structure;

图2 (a) Li6PS5X的晶体结构；(b) 离子传输路径[46]

Fig.2 (a) The crystal structure of Li6PS5X; (b) Ion transport pathway[46]

图3 硫化物基全固态锂电池中各种界面问题的示意图[54]

Fig.3 A schematic diagram of various interface issues in sulfide-based all-solid-state lithium batteries[54]

图4 高电流密度下的锂金属/Li6PS5Cl界面示意图[75]

Fig.4 Schematic diagram of the lithium metal/Li6PS5Cl interface under high current density[75]

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