English

Sulfide Solid Electrolyte Synthesized by Liquid Phase Approach and Application in All-Solid-State Lithium Batteries

• Mingyang Men ^{1, 2,} ,
• Jinghua Wu ^{1, 2,} ,
• Gaozhan Liu ^{1, 2,} ,
• Jing Zhang ^{1, 2,} ,
• Nini Zhang ^{1, 2,} ,
• Xiayin Yao ^{1, 2, ,}

• 1.

  Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, Zhejiang Province, China

• 2.

  Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Xiayin Yao, Email: yaoxy@nimte.ac.cn; Tel.: +86-574-8632-4359

• Received Date: 12 September 2023
  Accepted Date: 30 October 2023
  Revised Date: 11 October 2023
  Available Online: 15 January 2025
• Fund Project:

  the National Natural Science Foundation of China 

  the National Natural Science Foundation of China 

  the Ningbo S&T Innovation 2025 Major Special Program 

  the Ningbo S&T Innovation 2025 Major Special Program 

  the Zhejiang Provincial Key R&D Program of China 

  the Youth Innovation Promotion Association CAS 

Abstract: Current commercialized lithium ion batteries generally suffer from safety issues due to using flammable organic liquid electrolytes. All-solid-state lithium batteries employing solid electrolytes instead of organic liquid electrolytes and separators possess the advantages of both good safety and high energy density, which is expected to be the most promising energy storage devices for the next generation electric vehicles and smart grid. Sulfide solid electrolytes are regarded as crucial components for all-solid-state rechargeable batteries for the merits of their high room temperature ionic conductivities that approaches or exceeds liquid organic electrolytes and excellent mechanical ductility. The preparation methods of sulfide solid electrolytes are mainly divided into three categories, i.e. solid-state sintering, ball milling and liquid-phase method. However, solid-state sintering and ball milling are time-consuming accompanied by high energy consumption. At the same time, the synthesized electrolyte particles are large in size, which seriously limits the practical application of sulfide electrolytes. In contrast, the liquid-phase method, using organic solvents as the medium, can synthesize sulfide solid electrolytes with controlled particle sizes, which is a simple and time-saving process and more suitable for large-scale production. In this review, we begin by introducing the crystal structures and ion transport mechanisms of major sulfide electrolytes including Li₂S-P₂S₅ binary sulfide solid electrolytes, Li₁₀GeP₂S₁₂ and Li₆PS₅X (X = Cl, Br, I) ternary systems, and summarize the progress of sulfide solid electrolytes prepared by liquid phase method in recent years. Based on the solubility state of the reagents in the solvent, the liquid-phase synthesis of sulfide electrolytes can be categorized into suspension type, solution type and mixed type, and their reaction mechanisms are discussed separately. Subsequently, we summarize the effect of solvents on the properties of liquid-phase synthesized sulfide electrolytes, such as purity, morphology, crystallinity and ionic conductivity. In addition, the application of liquid-phase synthesized sulfide solid electrolytes for all-solid-state lithium batteries is presented from six aspects: sulfide electrolytes coated on active materials, electrolyte-active material composites, electrolyte injection into porous electrodes, interfacial modification at solid-solid contact triple-interfaces within electrode layers, electrolyte elemental doping and electrolyte film preparation, which demonstrates the superior scalability of the liquid-phase method and the diverse application prospects. Finally, according to the current research status of the sulfide solid electrolytes synthesized by liquid phase method, the advantages and limitations of the liquid phase synthesis of sulfide solid electrolytes are also analyzed, providing the development direction for the liquid phase synthesized sulfide solid electrolyte for all-solid-state lithium batteries in future.

Key words:
• All-solid-state battery
•  /  Sulfide solid electrolyte
•  /  Liquid phase method
•  /  Wet-chemical synthesis
•  /  Reaction mechanism

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