All-solid-state lithium metal batteries(ASSLMBs)are widely recognized as promising next-generation energy storage technologies that offer significant advantages in terms of safety and energy density.However,the long-t...All-solid-state lithium metal batteries(ASSLMBs)are widely recognized as promising next-generation energy storage technologies that offer significant advantages in terms of safety and energy density.However,the long-term cycling stability of these batteries is often compromised by interfacial failures driven by coupled mechanical and diffusion effects.This study presents a probabilistic failure prediction model that quantifies interfacial damage and capacity loss in composite electrodes under the coupled influence of mechanical-diffusion-induced processes.We first develop a pseudo3D(P3D)interface failure model for a binary particle system to evaluate interfacial failure during the critical delithiation process.The P3D model is validated through mechanical‒diffusion coupled simulations.Additionally,for multiparticle composite electrode films with heterogeneous particle sizes,we identify a key structural factor that governs the failure of the particle‒solid electrolyte interface,which follows a three-parameter Burr distribution.Building on this,we develop a probabilistic model to predict the capacity fade in multiporject composite films.This work provides a comprehensive understanding of the critical geometric factors that influence interfacial stability,offering valuable theoretical insights and practical guidance for the rapid assessment,optimization,and enhancement of cycling stability in ASSLMBs.展开更多
基金supported by the Beijing Municipal Education Commission(Grant No.KM202311232008)the National Natural Science Foundation of China(Grant No.12002343).
文摘All-solid-state lithium metal batteries(ASSLMBs)are widely recognized as promising next-generation energy storage technologies that offer significant advantages in terms of safety and energy density.However,the long-term cycling stability of these batteries is often compromised by interfacial failures driven by coupled mechanical and diffusion effects.This study presents a probabilistic failure prediction model that quantifies interfacial damage and capacity loss in composite electrodes under the coupled influence of mechanical-diffusion-induced processes.We first develop a pseudo3D(P3D)interface failure model for a binary particle system to evaluate interfacial failure during the critical delithiation process.The P3D model is validated through mechanical‒diffusion coupled simulations.Additionally,for multiparticle composite electrode films with heterogeneous particle sizes,we identify a key structural factor that governs the failure of the particle‒solid electrolyte interface,which follows a three-parameter Burr distribution.Building on this,we develop a probabilistic model to predict the capacity fade in multiporject composite films.This work provides a comprehensive understanding of the critical geometric factors that influence interfacial stability,offering valuable theoretical insights and practical guidance for the rapid assessment,optimization,and enhancement of cycling stability in ASSLMBs.