Dual Regulation Strategy to Construct Robust and High-Conductivity Na3V2(PO4)2O2F for Ultra-Long-Life Sodium-Ion Full Cells
The polyanionic compound Na3V2(PO4)2O2F (NVPOF) possesses a stable three-dimensional framework, high theoretical specific capacity, and favorable operating voltage, yet its sluggish Na+ diffusion kinetics and low electronic conductivity impede industrial application. This study proposes a dual regulation strategy combining carbon coating and heat treatment temperature to synergistically enhance crystallinity and electrochemical performance. NVPOF@C-400 and NVPOF@C-600 were synthesized via in-situ dopamine hydrochloride coating followed by heat treatment at 400 °C and 600 °C, respectively. Carbon coating at 600 °C significantly improved crystallinity and increased electronic conductivity by three orders of magnitude through the carbon layer's conductive network. The ~4.5 nm carbon layer effectively suppressed abnormal grain growth and secondary crystallization aggregation at high temperatures, maintaining uniform particle size of approximately 0.36 μm, which shortens Na+ diffusion pathways and prevents ion transport obstruction. Consequently, NVPOF@C-600 delivered a high discharge capacity of 102.5 mAh g−1 at 20 C and retained 96.5% capacity after 10,000 cycles. In a full-cell configuration with hard carbon (HC), NVPOF@C-600//HC achieved an impressive 89.3% capacity retention after 9,000 cycles. This work provides critical insights for practical implementation of high-performance NVPOF cathodes in sodium-ion batteries.