• A novel hydrolysis-driven synthesis creates a dual-surface functionalized micron-sized Si anode with a SiOx/C layer, avoiding corrosive etchants and toxic reagents.
• The functionalized inner pores and dual-functional SiOx/C layer synergistically alleviate volume change, minimize stress concentration, and improve electrochemical reaction kinetics.
• The optimized micron-Si anode delivers impressive lifespan (901.1 mAh g⁻1 after 500 cycles at 1 A g⁻1) and excellent rate capability (1123.0 mAh g⁻1 at 5 A g⁻1 and 850.4 mAh g⁻1 at 8 A g⁻1).
• When paired with commercial NCM811, the pouch cell demonstrates high capacity and desirable cyclic performance, highlighting practical applicability.
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