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In Situ Self-Adaptive Structure Evolution Under Volume Fluctuation Toward High-Performance Silicon-Based Anode
DOI:10.1002/adma.202517989.png)
Abstract
En 中文
Alloy-type anodes have become the most promising candidates for the next-generation energy-dense lithium-ion batteries, but structural collapse caused by intrinsic volume fluctuation is the key bottleneck to their practical applications. Herein, an innovative self-adaptive structural evolution strategy toward electrochemically stable Si-based alloy-type anode is proposed, which breaks the conventional ideas that pursue the immutability of the initial structure. Particularly, interconnected commercial Si nanoparticles are covalently coated by amorphous homogeneous composite SiOx/C (h-SiOx/C) layer, forming a “pea-like” core–shell structure. After charge–discharge cycling, as-designed Si@h-SiOx/C evolves into a more stable micro-sized “spherical-like” particle with Si always well protected by h-SiOx/C layer. Furthermore, inner SEI microdomains and cavities are also formed, which can provide rapid transport pathways for Li+ and accommodation space for volume expansion, respectively. Accordingly, Si@h-SiOx/C displays excellent performances in both half and full pouch cells. 3D reconstruction, in situ optical microscopy and finite element simulations have been conducted to deeply analyze the structural self-adaptive mechanism. This work provides new insights into optimizing Si-based alloy anodes via dynamically self-adaptive regulation, replacing conventional static structural design paradigms.
Keywords:
3D reconstruction
finite element simulations
lithium-ion batteries
self-adaptive structure evolution
silicon-based anode
Journal
IF:
26.8
Papers:
3.4W
Citations:
46.0W

