Exploring the failure mechanisms of quasi/all solid-state Li-ion batteries with Si-based electrodes

Lithium-ion batteries are widely applied in the field of energy storage due to their high energy density and long cycle life. However, traditional liquid electrolytes have safety hazards such as leakage and thermal runaway. The quasi-solid-state battery (QSSB) and all-solid-state battery (ASSB) have emerged as promising alternatives with higher safety and stability. In addition, Si-based electrodes are attractive due to their high theoretical capacity. Currently, researchers apply Si-based electrodes in QSSB and ASSB, but the failure mechanisms within them are not fully summarized and organized. Herein, this work systematically studies the failure mechanisms of QSSB and ASSB with Si-based electrodes, including particle fracture, solid electrolyte interphase breakdown, pore evolution, and electrical contact loss. The influence of rigid solid electrolytes on ASSB is discussed, as well as the limitations of quasi-solid electrolytes, such as low ionic conductivity and side reactions. The strategies for alleviating these problems are also reviewed, including the structural design of Si electrodes, electrolyte optimization, and interface engineering. This article aims to summarize the key failure mechanisms and provide guidance and technological development directions for the subsequent development of high-energy density and long-life batteries.