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Do More with Less: Breaking the Performance Dilemma of NASICON Cathode via Minimal Quadruple Doping
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DOI：10.1002/adfm.202600083.png)
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Abstract
En 中文
NASICON-type Na3V2(PO4)3, featuring multielectron reactions, is a prospective cathode for SIBs, but suffers from inferior conductivity and structural degradation with compromised rate/cyclic stability. Overcoming the enduring capacity-stability trade-off remains a pivotal challenge in the advancement of high-performance cathodes. Herein, we break the performance dilemma of Na3V2(PO4)3 cathode through strategic minimal quadruple doping (Mn, Al, Ni, and Cr; total 8 at%) at its V-site. As-prepared QD-NVP exhibits a reversible solid-solution-triphasic reaction mechanism across successive V2+/V3+/V4+/V5+ redox processes, accompanied by low voltage polarization and small lattice stress. Theoretical calculation and in/ex situ characterizations reveal that the minimal quadruple doping endows QD-NVP with stable [QD-VO6] octahedra, expanded channels, weakened Na+-O interactions, and high V-site spin polarization, simultaneously boosting the ion/electron conductivity, the structure stability, and the vanadium utilization. Consequently, the QD-NVP cathode achieves concurrent high capacity (179 mA h g−1 at 0.1C), exceptional rate capability (115 mA h g−1@80C), and excellent cycling stability (97.2% retention over 4200 cycles@50C), surpassing those of the best-performing V-polyanionic cathodes reported to date. Moreover, the superior battery performance of QD-NVP-assembled full/symmetric cells further highlights its potential multi-scenario applications. This work provides an innovative perspective by doing more with less to develop a high-performance NASICON cathode for next-generation SIBs.
Keywords:
cathode
NASICON
quadruple doping
sodium ion batteries
sodium vanadium phosphate
Journal
IF:
19
Papers:
3.4W
Citations:
32.1W