Crack pinning enables stable cycling of micro-sized silicon anodes for wide-temperature lithium-ion batteries

Abstract

Silicon anodes promise revolutionary lithium-ion battery energy density, yet commercial viability remains constrained by catastrophic volume expansion and interfacial degradation under demanding thermal conditions. Here, we demonstrate engineered crack pinning mechanisms within a gradient-structured hybrid solid–electrolyte interphase (H-SEI) that enables unprecedented cycling stability of micro-sized silicon anodes across extreme temperatures. The dual-layer H-SEI architecture features nanocrystalline inorganic domains providing grain-boundary strengthening, while polymer-integrated outer layers incorporate distributed nanocrystals as crack arresters, preventing fracture propagation through synergistic stress redistribution. This crack pinning strategy maintains structural integrity under ∼200% volumetric expansion, preserving continuous wide-temperature lithium-ion transport. Paired with NCM811 cathodes, 1-Ah pouch cells exhibit long cycle life, retaining >80% capacity from −20 °C to 70 °C over extended cycling, substantially exceeding existing silicon technologies. These findings establish crack pinning as a transformative approach for thermally-robust silicon batteries, enabling next-generation energy storage across diverse environmental conditions.

Graphical abstract: Crack pinning enables stable cycling of micro-sized silicon anodes for wide-temperature lithium-ion batteries

Supplementary files

Article information

Article type
Paper
Submitted
30 May 2025
Accepted
01 Jul 2025
First published
04 Jul 2025

Energy Environ. Sci., 2025, Advance Article

Crack pinning enables stable cycling of micro-sized silicon anodes for wide-temperature lithium-ion batteries

K. Hu, J. Zhang, X. Yu, J. Wang and X. Hu, Energy Environ. Sci., 2025, Advance Article , DOI: 10.1039/D5EE02997J

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