A Long Cycle‐Life High‐Voltage Spinel Lithium‐Ion Battery Electrode Achieved by Site‐Selective Doping

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....

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2020-06, Vol.59 (26), p.10594-10602
Main Authors: Liang, Gemeng, Wu, Zhibin, Didier, Christophe, Zhang, Wenchao, Cuan, Jing, Li, Baohua, Ko, Kuan‐Yu, Hung, Po‐Yang, Lu, Cheng‐Zhang, Chen, Yuanzhen, Leniec, Grzegorz, Kaczmarek, Sławomir Maksymilian, Johannessen, Bernt, Thomsen, Lars, Peterson, Vanessa K., Pang, Wei Kong, Guo, Zaiping
Format: Article
Language:English
Subjects:
Doping
Durability
Electrochemical analysis
Electrochemistry
Electrode materials
Electrodes
high energy density
Lithium
Lithium-ion batteries
long cycle life
Magnesium
Manganese
site-selective doping
Spinel
spinel cathodes
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Summary: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 Fd3‾ 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. Magnesium is selectively doped onto both tetrahedral (8a) and octahedral (16c) sites in Fd3‾ m LiNi0.5Mn1.5O4. The Mg stabilizes the structure against structural deformation and suppresses unfavorable two‐phase reactions during cycling, thus contributing to an excellent extended‐long‐term electrochemical performance.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202001454