Abstract:

While conventional graphite anodes (372 mAh g-1) struggle to meet the ever-increasing energy density demands of electric vehicles, silicon-based materials emerge as promising alternatives with exceptional theoretical capacity (4200 mAh g-1). However, the implementation of silicon anodes in lithium-ion batteries has been hindered by persistent structural degradation and interfacial instability arising from severe volume fluctuations during (de)lithiation cycles. Herein, this study presents an innovative layer-stacked SiOx (LS-SiOx) architecture, featuring an interconnected, void-rich microstructure that strategically accommodates mechanical strain while maintaining structural integrity over extended cycling. By adjusting oxygen content through controlled hydrogen ion adsorption on precursors before thermal processing, an optimal balance between capacity retention and cycle stability is achieved. Furthermore, carbon nanotube-encapsulated LS-SiOx@CNT composites spontaneously formed through binder-mediated assembly demonstrate enhanced initial coulombic efficiency and deliver superior capacity retention, demonstrating a specific capacity of 800 mAh g-1 after 300 cycles. This synthetic strategy provides new insights into developing durable high-capacity anodes, establishing a scalable design paradigm for high-energy-density lithium-ion batteries.

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