A long cycle-life high-voltage spinel lithium-ion battery electrode achieved by site-selective doping

Spinel LiNi₀.₅ Mn₁.₅ O₄ (LNMO) is a promising cathode candidate for the next-generation high energy-density lithium-ion batteries (LIBs). Unfortunately, the application of LNMO is hindered by its poor cycle stability. Now, site-selectively doped LNMO electrode is prepared with exceptional durability. In this work, Mg is selectively doped onto both tetrahedral (8a) and octahedral (16c) sites in the Fd 3‾ m structure. This site-selective doping not only suppresses unfavorable two-phase reactions and stabilizes the LNMO structure against structural deformation, but also mitigates the dissolution of Mn during cycling. Mg-doped LNMOs exhibit extraordinarily stable electrochemical performance in both half-cells and prototype full-batteries with novel TiNb2 O7 counter-electrodes. This work pioneers an atomic-doping engineering strategy for electrode materials that could be extended to other energy materials to create high-performance devices.Gemeng Liang, Zhibin Wu, Christophe Didier, Wenchao Zhang, Jing Cuan, Baohua Li, Kuan-Yu Ko, Po-Yang Hung, Cheng-Zhang Lu, Yuanzhen Chen, Grzegorz Leniec, Sławomir Maksymilian Kaczmarek, Bernt Johannessen, Lars Thomsen, Vanessa K. Peterson, Wei Kong Pang, and Zaiping Gu