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Volume 115
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Unveiling the size-dependent electro-chemo-mechanical failure mechanisms of silicon anodes in sulfide-based all-solid-state batteries
Shi-Jie Yang a b 1, Ao-Long Yue a b 1, Hong Yuan a b c *, Ming-Xuan Xu a b, Zi-Hao Zuo a b, Di-Chen Wu b c, Yao-Hui Zhu b c, Chen Ling a b, Jia-Qi Huang a b c *
a School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081, China
b School of Interdisciplinary Science, Beijing Institute of Technology, Beijing, 100081, China
c School of Interdisciplinary Science, Beijing Institute of Technology, Zhuhai, 519088, China
10.1016/j.partic.2026.04.028
Volume 115, August 2026, Pages 118-125
Received 2 April 2026, Revised 28 April 2026, Accepted 29 April 2026, Available online 20 May 2026, Version of Record 29 May 2026.
E-mail: yuanhong@bit.edu.cn; jqhuang@bit.edu.cn
Highlights

• Electrochemical performance of Si-anodes with different particle sizes.

• Establishing the interfacial structural evolution of Si anodes.

• Unveiling the electro-chemo-mechanical failure mechanisms of Si anodes.


Abstract

High-capacity silicon anodes hold great promise for safe and energy-dense all-solid-state lithium batteries (ASSLBs), yet their practical application is hindered by interfacial degradation and mechanical fracture, which severely limit their cycle life. Herein, we unravel the particle-size-dependent electro-chemo-mechanical failure mechanisms of Si anodes in sulfide-based ASSLBs. The micro-sized Si (μm-Si) anode exhibits favorable initial Coulombic efficiency (ICE, 79.15%) and reversible capacity (2260.5 mAh g−1) but succumbs to progressive particle fracture under prolonged cycling due to cumulative mechanical stress from large volume swings. By contrast, the nano-sized Si (nm-Si) anode suffers from severe interfacial side reactions and irreversible volume expansion due to its larger specific area and dense electrode structure, resulting in lower initial performance (ICE of 72.21%, 1372.7 mAh g−1). In subsequent cycles, the nm-Si anode experiences continuous interfacial side reactions, leading to substantial accumulation of interfacial decomposition byproducts and sustained capacity decay. These contrasting failure pathways establish electro-chemo-mechanical coupling as the governing principle and provide a particle-size-dependent design framework for high-performance Si-based ASSLBs.

Graphical abstract
Keywords
All-solid-state batteries; Silicon anode; Failure mechanisms; Particle size; Solid electrolyte interphase
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