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    Multivalent Cation Incorporated into Manganese-Iron Based NASICON Cathodes for High Voltage Sodium-Ion Batteries
    (Wiley-V C H Verlag Gmbh, 2024) Zeng, Jingyao; Gao, Jinqiang; Jian, Weishun; Wang, Haoji; Li, Wenyuan; Hong, Ningyun; Zhang, Baichao
    Na4Mn1.5Fe1.5(PO4)(2)P2O7 (NMFPP), with its low cost and high energy density, is essential for accelerating the commercialization of sodium-ion batteries. However, its practical application is limited by serious voltage hysteresis and detrimental Jahn-Teller distortions. Herein, a high operating voltage and superior stable Nb-doped NMFPP with fewer intrinsic anti-site defects are elaborately designed by the reconstruction of the crystal lattice and electronic distribution. By introducing higher charge density Nb & horbar;O bonds, the lengths of Mn-O bonds are shortened, enhancing lattice stability. As a result, the lattice volume contracted during Na+ extraction/insertion is decreased with niobium-modified Na-4(Mn0.5Fe0.5)(2.94)Nb-0.06(PO4)(2)P2O7, mitigating lattice distortion from the Jahn-Teller effect and increasing the capacity retention after 1000 cycles from 57.5% to 82.3%. More importantly, the delayed effect of Mn2+ involvement in redox reactions is significantly reduced, raising the average operating voltage from 3.32 to 3.64 V and increasing the overall energy density by 13%. This study opens new avenues to develop advanced sodium-ion battery cathode materials with high energy density and long calendar life for energy storage.