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抑制基于石榴石的高容量阳极固态电池中的界面失效:机理与策略

Inhibiting Interfacial Failure in Garnet-Based Solid-State Batteries with High-Capacity Anodes: Mechanism and Strategies.

作者信息

Xiao Zhexi, Zou Zewei, Zhao Kehao, Lin Zhenkang, Zhang Bingchen, Yu Yaxiong, Zhu Chang, Xu Kang, Xing Lidan, Li Weishan

机构信息

School of Chemistry, South China Normal University, Guangzhou, 510006, China.

National and Local Joint Engineering Research Center of MPTES in High, Energy and Safety LIBs, Engineering Research Center of MTEES (Ministry of Education), Research Center of BMET(Guangdong Province), and Key Lab. Of ETESPG (GHEI), South China Normal University, Guangzhou, 510006, China.

出版信息

Adv Mater. 2025 Sep;37(38):e2507188. doi: 10.1002/adma.202507188. Epub 2025 Jun 23.

DOI:10.1002/adma.202507188
PMID:40545988
Abstract

Garnet-based solid-state electrolytes (SSEs) with exceptional reductive stability and superior ionic conductivity have emerged as promising candidates for next-generation solid-state batteries (SSBs). However, critical interface challenges still persist in practical implementations. This review systematically examines interfacial failure mechanisms in garnet SSE systems with high-capacity anodes (Si, metallic Li) through combined mechanical-electrochemical perspectives. For Si-based anodes, a microstructure-property-performance relationship is established by analyzing strain mismatch-induced degradation, correlating ionic transport barriers with lithiation kinetics under varying internal microstructures, particle sizes, and external pressures. Multiscale stress-relief strategies spanning atomic-level interface engineering to macroscopic pressure optimization are proposed. Regarding Li metal interfaces, breakthrough understandings of grain boundary (GB) charge distribution effects on Li filament propagation are highlighted, along with innovative solutions for kinetic inhibition. Particular emphasis is placed on dry battery electrode (DBE) fabrication techniques as scalable approaches for achieving intimate interfacial contact in industrial-scale SSB production. By integrating fundamental mechanical-electrochemical insights with practical engineering considerations, this work quantitatively decouple the strain-lithiation interplay at Si/garnet interfaces, the regulation law of GB charge distribution on lithium dendrites and the industrial potential of combining DBE with fluidized bed technology for the first time, charting a viable path toward industrial SSBs with >400 Wh kg energy density.

摘要

具有卓越还原稳定性和优异离子导电性的石榴石基固态电解质(SSE)已成为下一代固态电池(SSB)的有前途的候选材料。然而,在实际应用中,关键的界面挑战仍然存在。本综述通过机械 - 电化学相结合的视角,系统地研究了具有高容量负极(硅、金属锂)的石榴石SSE系统中的界面失效机制。对于硅基负极,通过分析应变失配引起的降解,将离子传输障碍与不同内部微观结构、粒径和外部压力下的锂化动力学相关联,建立了微观结构 - 性能 - 性能关系。提出了从原子级界面工程到宏观压力优化的多尺度应力缓解策略。关于锂金属界面,强调了对晶界(GB)电荷分布对锂丝传播影响的突破性理解,以及动力学抑制的创新解决方案。特别强调了干电池电极(DBE)制造技术,作为在工业规模的SSB生产中实现紧密界面接触的可扩展方法。通过将基本的机械 - 电化学见解与实际工程考虑相结合,这项工作首次定量地解耦了硅/石榴石界面处的应变 - 锂化相互作用、晶界电荷分布对锂枝晶的调控规律以及DBE与流化床技术结合的工业潜力,为能量密度>400 Wh/kg的工业固态电池绘制了一条可行的路径。

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