Li3PS4 固态电解质的研究进展

doi:10.19799/j.cnki.2095-4239.2021.0513

储能科学与技术 ›› 2022, Vol. 11 ›› Issue (5): 1368-1382.doi: 10.19799/j.cnki.2095-4239.2021.0513

Li₃PS₄ 固态电解质的研究进展

魏超超¹^,²(), 余创¹(), 吴仲楷¹^,², 彭林峰¹^,³, 程时杰¹, 谢佳¹()

^1.华中科技大学电气与电子工程学院强电磁工程与新技术国家重点实验室
^2.华中科技大学化学与化工学院
^3.华中科技大学物理学院，湖北武汉 430074

收稿日期:2021-10-08 修回日期:2021-11-08 出版日期:2022-05-05 发布日期:2022-05-07
通讯作者: 余创,谢佳 E-mail:weichaochao@hust.edu.cn;cyu2020@hust.edu.cn;xiejia@hust.edu.cn
作者简介:魏超超（1994—），男，博士研究生，研究方向为固态电池与固态电解质，E-mail：weichaochao@hust.edu.cn；
基金资助:
国家自然科学基金项目(51821005)

Research progress of Li₃PS₄ solid electrolyte

Chaochao WEI¹^,²(), Chuang YU¹(), Zhongkai WU¹^,², Linfeng PENG¹^,³, Shijie CHENG¹, Jia XIE¹()

^1.State Key Laboratory of Strong Electromagnetic Engineering and New Technology, School of Electrical and Electronic Engineering, Huazhong University of Science and Technology
^2.School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology
^3.School of Physics, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China

Received:2021-10-08 Revised:2021-11-08 Online:2022-05-05 Published:2022-05-07
Contact: Chuang YU, Jia XIE E-mail:weichaochao@hust.edu.cn;cyu2020@hust.edu.cn;xiejia@hust.edu.cn

摘要/Abstract

摘要：

全固态锂电池因其高安全性和高能量密度成为最有望替代传统液态锂电池的体系之一。固态电解质是全固态锂电池的核心组成部分，其中硫化物电解质因其高离子电导率、良好的机械延展性等优势成为最具潜力的固态电解质之一。Li₃PS₄固态电解质具有高离子电导率、宽电化学窗口、低成本等优势，是极具代表的硫化物固态电解质，也是近年来研究较多的硫化物固态电解质，然而其空气/水汽稳定性差、与正负极材料的兼容性较差等缺点限制了其在高性能全固态锂电池中的大规模应用。本文通过对近期Li₃PS₄固态电解质等相关文献的探讨，综述了Li₃PS₄固态电解质的结构机理和制备路线，总结并分析了Li₃PS₄固态电解质在提高离子电导率、改善化学/电化学稳定性、强化力学性能等方面采取的策略及研究进展，最后归纳了近年来基于Li₃PS₄固态电解质和各种正负极材料构筑的高性能全固态电池。基于以上的分析，本文也指出了当前Li₃PS₄固态电解质仍存在的不足并展望了Li₃PS₄等硫化物电解质在未来的研究重点及发展方向。

关键词: 固态电解质, Li₃PS₄, 全固态电池, 电化学性能, 固态锂硫电池, 电导率

Abstract:

All-solid-state lithium battery has become one of the most promising candidates to replace the traditional lithium battery utilizing liquid organic electrolytes due to its high safety and high energy density. The solid electrolyte is the crucial component of all-solid-state lithium battery, and sulfide electrolytes are attractive among solid electrolytes due to their high ionic conductivities and good mechanical ductility. Li₃PS₄ solid electrolyte with high ionic conductivity, wide electrochemical windows and low cost has been attracted significant attention in recent years. However, its poor air/moisture stability and low compatibility towards cathode/anode materials limit its large-scale application in high-performance all-solid-state lithium batteries. In this paper, the structural mechanism and preparation route of Li₃PS₄ solid electrolyte were reviewed by discussing the recent literature on Li₃PS₄ solid electrolyte. Then, the strategies applied to enhance the ionic conductivity, improve the chemical/electrochemical stability, and strengthen the mechanical properties of Li₃PS₄ are summarized, and the applications of Li₃PS₄ electrolytes in solid-state batteries combined with different kinds of electrode materials are reviewed. Based on the above analysis, this paper also pointed out the shortcomings of the current Li₃PS₄ solid electrolyte and prospected the research focus and development direction of Li₃PS₄ and other sulfide electrolytes in the future.

Key words: solid electrolyte, Li₃PS₄, all-solid-state battery, electrochemical performance, solid state lithium sulfur battery, conductivity

中图分类号:

TM 911

魏超超, 余创, 吴仲楷, 彭林峰, 程时杰, 谢佳. Li₃PS₄ 固态电解质的研究进展[J]. 储能科学与技术, 2022, 11(5): 1368-1382.

Chaochao WEI, Chuang YU, Zhongkai WU, Linfeng PENG, Shijie CHENG, Jia XIE. Research progress of Li₃PS₄ solid electrolyte[J]. Energy Storage Science and Technology, 2022, 11(5): 1368-1382.

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Composition	Conductivity(RT)/(S/cm)	Ref.
β-Li₃PS₄	1.60×10^-4	[54]
Li_3.06P_0.98Zn_0.02S_3.98O_0.02	1.12×10^-3	[54]
75Li₂S·(23)P₂S₅-2P₂O₅	2.53×10^-4	[56]
75Li₂S·23P₂S₅-2P₂Se₅	6.00×10^-4	[55]
90Li₃PS₄-10LLZO 98Li₃PS₄-2Al₂O₃ 98Li₃PS₄-2SiO₂ 86.9Li₃PS₄-13.1LiAlS₂ 2Li₃PS₄-LiI	2.40×10^-4 2.28×10^-4 1.84×10^-4 6.00×10^-4 6.30×10^-4	[57] [57] [57] [58] [59]

Sample	Conductivity(RT)/(S/cm)	E/GPa
Li₃PS₄	2.4×10^-4	23
95 Li₃PS₄-5LiI	2.9×10^-4	21
90 Li₃PS₄-10LiI	4.7×10^-4	21
80 Li₃PS₄-20LiI	1.1×10^-3	20
70 Li₃PS₄-30LiI	1.5×10^-3	19

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Li₃PS₄ 固态电解质的研究进展

Research progress of Li₃PS₄ solid electrolyte

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