Hu Xia, Yu Jiahao, Wang Yao, Guo Weiqian, Zhang Xiang, Armand Michel, Kang Feiyu, Wang Guoxiu, Zhou Dong, Li Baohua
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China.
Centre for Cooperative Research on Alternative Energies (CIC energiGUNE), Basque Research and Technology Alliance (BRTA), Alava Technology Park, Albert Einstein 48, Vitoria-Gasteiz, 01510, Spain.
Adv Mater. 2024 Feb;36(7):e2308275. doi: 10.1002/adma.202308275. Epub 2023 Dec 7.
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 Li S as a shield component considerably promotes interfacial wettability and hinders Li dendrite penetration into the bulk of garnet electrolyte. Interfacial shield-protected Li La Zr Ta O (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.
锂石榴石被认为是下一代固态锂金属电池（SSLBs）很有前景的固态电解质。然而，外部堆叠压力驱动的锂侵入会引发锂金属电池的过早失效。在此，首次报道了一种原位构建的界面屏蔽层，可有效抑制SSLBs中压力诱导的锂侵入。理论建模和实验研究表明，屏蔽层内的高硬度金属钼纳米晶体可有效抑制锂枝晶生长，而不会因合金硬化导致界面接触恶化。同时，作为屏蔽层组件的电绝缘硫化锂可显著提高界面润湿性，并阻碍锂枝晶穿透到石榴石电解质主体中。基于界面屏蔽保护的LiLaZrTaO（LLZTO）的电池在约0.2 MPa的常规压力下甚至在高达70 MPa的高压下均表现出显著增强的循环稳定性且无短路现象；这是使用石榴石电解质的SSLBs报道的最高耐受堆叠压力。这些关键发现有望推动SSLBs在宽压力范围内的应用。
