A Lithium Intrusion‐Blocking Interfacial Shield for Wide‐Pressure‐Range Solid‐State Lithium Metal Batteries

• Published in: Advanced materials (Weinheim) Vol. 36; no. 7; pp. e2308275 - n/a
• Main Authors: Hu, Xia, Yu, Jiahao, Wang, Yao, Guo, Weiqian, Zhang, Xiang, Armand, Michel, Kang, Feiyu, Wang, Guoxiu, Zhou, Dong, Li, Baohua
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 01.02.2024
• Subjects: Electric contacts; Electrolytes; Electrolytic cells; External pressure; external stack pressure; Garnets; garnet‐type oxide electrolytes; interfacial shield; Intrusion; Lithium; Lithium batteries; lithium intrusion; Molten salt electrolytes; Short circuits; Solid electrolytes; solid‐state lithium metal batteries; Wettability; interfacial shield; solid-state lithium metal batteries; lithium intrusion; external stack pressure; garnet-type oxide electrolytes
• ISSN: 0935-9648; 1521-4095
• DOI: 10.1002/adma.202308275

Lithium garnets are considered as promising solid‐state electrolytes for next‐generation solid‐state Li metal batteries (SSLBs). However, the Li intrusion driven by external stack pressure triggers premature of Li metal batteries. Herein, for the first time, an in situ constructed interfacial shield is reported to efficiently inhibit the pressure‐induced Li intrusion in SSLBs. Theoretical modeling and experimental investigations reveal that high‐hardness metallic Mo nanocrystals inside the shield effectively suppress Li dendrite growth without alloy hardening‐derived interfacial contact deterioration. Meanwhile the electrically insulated Li2S as a shield component considerably promotes interfacial wettability and hinders Li dendrite penetration into the bulk of garnet electrolyte. Interfacial shield‐protected Li6.4La3Zr1.4Ta0.6O12 (LLZTO)‐based cells exhibit significantly enhanced cyclability without short circuits under conventional pressures of ≈0.2 MPa and even at high pressure of up to 70 MPa; which is the highest endurable stack pressure reported for SSLBs using garnet electrolytes. These key findings are expected to promote the wide‐pressure‐range applications of SSLBs. A high‐efficiency Li intrusion‐blocking interfacial shield is realized for wide‐pressure‐range solid‐state lithium metal batteries, consisting of high‐hardness metallic Mo nanocrystals and electrically insulated Li2S. Interfacial shield‐protected Li6.4La3Zr1.4Ta0.6O12‐based cells exhibit significantly enhanced cyclability even at high pressure of 70 MPa.