Abstract

Na3(VOPO4)2F (NVOPF) has emerged as a promising cathode candidate for commercial Na-ion batteries, ascribed to its elevated theoretical energy density and robust structure during the extraction/insertion of two Na+ ions. However, the intrinsic poor electronic conductivity and unscalable materials-preparation technologies make it unexpected to stand out in large-scale energy storage systems. In this study, a spray-drying process technology is implemented to synthesize Na3(VOPO4)2F@carbon nanotubes (NVOPF@CNTs) composite through the reduction of V5+ driven by methanol at room temperature, in which the shortened Na-ion transfer path and the rapid electron mobility are facilitated by the CNTs. The resulting NVOPF@CNTs electrode exhibits exceptional capabilities, including a high discharge capacity (122.1 mA h g−1 at 1 C= 120 mA h g−1), outstanding rate performance (103.1 mA h g−1 at 100 C), and an extended lifespan (71.8 % capacity retention after 6000 cycles at 20 C). Additionally, the Na3(VOPO4)2F//NaTi2(PO4)3 full battery system demonstrates impressive high-power output capabilities (93.3 mA h g−1, 20 C), versatile current switching adaptability, and robust cycling performance (75.3 % of 98.5 mA h g−1 for the initial capacity after 3000 cycles). The study underscores the potential of improving the preparation of vanadium-based phosphate materials to enhance the practical application of Na-ion batteries.

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