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A Long Cycle-Life High-Voltage Spinel Lithium-Ion Battery Electrode Achieved by Site-Selective Doping
Authors:Gemeng Liang  Zhibin Wu  Dr Christophe Didier  Dr Wenchao Zhang  Dr Jing Cuan  Prof Baohua Li  Kuan-Yu Ko  Po-Yang Hung  Dr Cheng-Zhang Lu  Dr Yuanzhen Chen  Dr Grzegorz Leniec  Dr Sławomir Maksymilian Kaczmarek  Dr Bernt Johannessen  Dr Lars Thomsen  Dr Vanessa K Peterson  Dr Wei Kong Pang  Prof Zaiping Guo
Institution:1. Faculty of Engineering, Institute for Superconducting & Electronic Materials, University of Wollongong, Wollongong, NSW, Australia;2. Faculty of Engineering, Institute for Superconducting & Electronic Materials, University of Wollongong, Wollongong, NSW, Australia

Australian Centre for Neutron Scattering, Australian Nuclear Science and Technology Organization, Sydney, NSW, Australia;3. Graduate School at Shenzhen, Tsinghua University, Shenzhen, 518055 P. R. China;4. Industrial Technology Research Institute, Hsinchu, Taiwan) (China;5. School of Materials Science and Engineering, Xi'an Jiaotong University, Xi'an, 710049 P. R. China;6. Faculty of Mechanical Engineering and Mechatronics, West Pomeranian University of Technology in Szczecin, Al. Piastów, 17, 70-310 Szczecin, Poland;7. Australian Synchrotron, Australian Nuclear Science and Technology Organization, 800 Blackburn Road, Clayton, Victoria, 3168 Australia

Abstract:Spinel LiNi0.5Mn1.5O4 (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 Fdurn:x-wiley:00448249:media:ange202001454:ange202001454-math-0001 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 TiNb2O7 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.
Keywords:high energy density  lithium-ion batteries  long cycle life  site-selective doping  spinel cathodes
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