抑制高容量阳极石榴石基固态电池界面失效:机制与策略。

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zhexi Xiao, Zewei Zou, Kehao Zhao, Zhenkang Lin, Bingchen Zhang, Yaxiong Yu, Chang Zhu, Kang Xu, Lidan Xing, Weishan Li
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引用次数: 0

摘要

石榴石基固态电解质(sse)具有优异的还原稳定性和优异的离子电导率,已成为下一代固态电池(ssb)的有希望的候选者。然而,在实际实现中仍然存在关键的接口挑战。本文从机械电化学的角度系统地研究了高容量阳极(Si,金属Li)石榴石SSE系统的界面失效机制。对于硅基阳极,通过分析应变错配引起的降解,将不同内部微观结构,粒径和外部压力下的离子传输屏障与锂化动力学相关联,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消除策略。在锂金属界面方面,重点介绍了晶界(GB)电荷分布对锂丝传播影响的突破性认识,以及动力学抑制的创新解决方案。特别强调的是干电池电极(DBE)制造技术,作为实现工业规模SSB生产中亲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,本工作首次定量解耦了Si/石榴石界面的应变-锂化相互作用,锂枝晶上GB电荷分布的调节规律以及DBE与流化床技术相结合的工业潜力,为工业ssb绘制了一条可行的路径,能量密度为100 - 400 Wh kg-1。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Inhibiting Interfacial Failure in Garnet-Based Solid-State Batteries with High-Capacity Anodes: Mechanism and Strategies.

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-1 energy density.

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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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