Engineering interleaved large and small Na4MnV(PO4)3@NC microspheres cathode towards high performance sodium ion batteries

The booming consumption of energy storage devices spontaneously accelerates the urgent development of robust cathode materials for sodium-ion batteries (SIBs). In view of this, the sodium superionic conductor Na4MnV(PO4)3 (NMVP), with considerable energy density of 425 Wh kg−1, has become the focus in SIB research. Despite this, the performance of NMVP is substantially compromised by Jahn-Teller distortion of Mn3+ ions in conjunction with inherently limited electronic conductivity. In order to address this limitation, this study introduces a series of N-doped carbon (NC) coated NMVP materials with interleaved large and small microsphere morphology. Of particular note, the optimized NMVP-NC2 shows the most excellent performance, maintaining a capacity of 65.7 mAh g−1 at 5C over 500 cycles. A full cell configuration employing an NMVP-NC2 cathode and a commercial hard carbon (HC) anode manifests commendable circular stability with a capacity of 80.7 mAh g−1 underneath 100 cycles at 1C, with an impressive 95.3 % capacity preservation. This distinctive architecture imparts the materials with a high tap density and a relatively low surface area, which is beneficial to the industrial employment. In addition, density functional theory (DFT) calculations indicate that the NC regulation significantly narrows the NMVP's bandgap and facilitates electron transfer, thereby accelerating electron/ion transport kinetics. The NC coating approach combined with large-scale spray drying tactic in this work offers a clear strategy to industrialize NMVP cathode towards high-performance SIBs.