1.远景睿泰动力技术(上海)有限公司,上海 201315
2.复旦大学智能材料与未来能源创新学院,上海 200433
余乐(1983—),男,博士,研究方向为锂电池电解液及固态电解质材料,E-mail:kevin.yu@aesc-group.com;
收稿:2026-04-09,
修回:2026-07-09,
网络首发:2026-07-11,
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余乐, 李谦, 周永宁. 热处理提升Li7P3S11固态电解质的空气稳定性和电化学性能[J]. 储能科学与技术, XXXX, XX(XX): 1-12. DOI: 10.19799/j.cnki.2095-4239.2026.0313.
Yu Le, Li Qian, Zhou Yong-Ning. Investigation on the Effect of Thermal Treatment on the Air Stability and Electrochemical Performance of Li7P3S11 Solid Electrolyte[J]. Energy Storage Science and Technology, XXXX, XX(XX): 1-12. DOI: 10.19799/j.cnki.2095-4239.2026.0313.
余乐, 李谦, 周永宁. 热处理提升Li7P3S11固态电解质的空气稳定性和电化学性能[J]. 储能科学与技术, XXXX, XX(XX): 1-12. DOI: 10.19799/j.cnki.2095-4239.2026.0313. DOI:
Yu Le, Li Qian, Zhou Yong-Ning. Investigation on the Effect of Thermal Treatment on the Air Stability and Electrochemical Performance of Li7P3S11 Solid Electrolyte[J]. Energy Storage Science and Technology, XXXX, XX(XX): 1-12. DOI: 10.19799/j.cnki.2095-4239.2026.0313. DOI:
全固态锂电池因其潜在的高能量密度、优异的安全性和长循环寿命,被认为是下一代电动汽车动力电池的重要发展方向。然而,全固态锂电池中最常用的硫化物固态电解质在空气中的化学和电化学稳定性较差,制约了其规模化应用。本研究采用机械化学法,成功合成了室温离子电导率超过1.0 mS/cm的Li
7
P
3
S
11
固态电解质,系统研究了其在空气中暴露后的性能衰减机理,及后续热处理对其晶体结构和离子电导率的恢复作用。发现空气暴露会使得Li
7
P
3
S
11
固态电解质结晶度降低,并部分分解生成杂质相,导致其离子电导率显著下降。将经270
℃
热处理的Li
7
P
3
S
11
分别应用于单电解质层和双电解质层(引入Li
3
InCl
6
)结构的全固态电池中,正极采用高镍层状材料LiNi
0.9
Mn
0.05
Co
0.05
O
2
,负极为锂铟合金。研究结果表明,热处理后的Li
7
P
3
S
11
在两种全固态电池结构中均实现了超过200 圈的稳定循环,其中单电解质层结构展现出更高的比容量与更优的循环保持率。电化学阻抗谱分析表明,双电解质层结构性能劣化主要源于空气暴露后Li
7
P
3
S
11
与Li
3
InCl
6
之间界面阻抗的显著增大。本研究揭示了热处理对空气暴露后Li
7
P
3
S
11
的性能恢复机制,并明确了单电解质层结构在界面稳定性方面的优势,为硫化物基全固态电池的实用化设计提供了重要依据。
All-solid-state lithium batteries (ASSLBs) are regarded as promising candidates for next-generation electric vehicle power sources due to their potential for high energy density
excellent safety
and long cycle life. However
the poor chemical and electrochemical stability of sulfide-based solid electrolytes in ambient air significantly limits their larg
e-scale application. In this study
we successfully synthesized Li
7
P
3
S
11
solid electrolyte with a room-temperature ionic conductivity exceeding 1.0 mS/cm via a mechanochemical method. The effects of moisture exposure in air on its performance and the subsequent influence of thermal treatment on its structure and ionic conductivity were systematically investigated. It is revealed that air exposure reduces the crystallinity of Li7P3S11 solid electrolyte and partially decomposes it to form impurity phases
resulting in a significant decrease in its ionic conductivity. Thermally treated (270
℃
) Li
7
P
3
S
11
was incorporated into ASSLBs paired with a high-nickel layered cathode material (LiNi
0.9
Mn
0.05
Co
0.05
O
2
) and a Li-In alloy anode
using both a single-layer electrolyte structure and a bilayer configuration that included Li
3
InCl
6
. The results demonstrated that both configurations achieved stable cycling for over 200 cycles
with the single-layer structure exhibiting higher specific capacity and better cycling stability. Electrochemical impedance spectroscopy revealed that the inferior performance of the bilayer structure was primarily due to increased interfacial resistance between Li
7
P
3
S
11
and Li
3
InCl
6
after air exposure. This work provides important experimental insights and design strategies for improving the practical performance of sulfide-based ASSLBs.
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