Li Guocheng, Zhang Taolue, Tang Jiayue, Liu Mingtao, Xie Yizhan, Yu Jingya, Hui Xiaobin, Deng Canbin, Lu Xibin, Kim Yoonseob, Huang Jiaqiang, Xu Zheng-Long
Research Center for Deep Space Explorations, Department of Industrial and Systems Engineering, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR, 999077, P. R. China.
Sustainable Energy and Environment Thrust and Guangzhou Municipal Key Laboratory of Materials Informatics, The Hong Kong University of Science and Technology (Guangzhou), Guangdong, 511400, P. R. China.
Adv Mater. 2025 Jul;37(30):e2417770. doi: 10.1002/adma.202417770. Epub 2025 May 15.
All solid-state lithium (Li) metal batteries (ASSLBs) using ceramic-polymer hybrid solid electrolytes hold the promise for high-performance energy storage application, but they still suffer from the interfacial deterioration and dendritic Li penetration issues, particularly under low stack pressures. Therefore, understanding and mastering the underlying chemo-mechanical failure mechanisms become essential. Herein, the chemo-mechanical evolutions by operando monitoring the amplitude and heterogeneity of interfacial stress through an embedded optical fiber sensor are revealed. It is found that the uneven stripping/deposition of Li metal induces rapid and non-uniform stress growth at the interface, deteriorating interfacial contact with the Li-filament growth. Based on these insights, Li metal is replaced with an architectural lithium-tin anode, which demonstrates uniform stress and improved performance even under low stack pressure. This work not only offers a quantitative way to operando track the uniformity of interfacial stress but also provides critical insights into mastering the chemo-mechanics of ASSLBs.
所有使用陶瓷-聚合物混合固体电解质的全固态锂金属电池都有望应用于高性能储能领域，但它们仍面临界面劣化和锂枝晶穿透问题，尤其是在低堆叠压力下。因此，理解和掌握潜在的化学-机械失效机制变得至关重要。在此，通过嵌入光纤传感器对界面应力的振幅和不均匀性进行原位监测，揭示了化学-机械演变过程。研究发现，锂金属的不均匀剥离/沉积会在界面处导致快速且不均匀的应力增长，从而随着锂丝生长而使界面接触恶化。基于这些见解，用一种结构锂锡阳极替代锂金属，该阳极即使在低堆叠压力下也能表现出均匀的应力和改善的性能。这项工作不仅提供了一种原位跟踪界面应力均匀性的定量方法，还为掌握全固态锂金属电池的化学-力学提供了关键见解。
