Revealing the Multiple Influences of Zr Substitution on the Structural and Electrochemical Behavior of High Nickel LiNi₀.₈Co₀.₁Mn₀.₁O₂ Cathode Material
2021
Wu, Kang | Jiao, Jianyue | Li, Na | Wang, Min | Jia, Guofeng | Lee, Yu Lin | Dang, Rongbin | Deng, Xin | Xiao, Xiaoling | Wu, Zhijian
Layered O3-phase LiNi₀.₈Co₀.₁Mn₀.₁O₂ (NCM811) material has shown great potential for lithium-ion batteries (LIBs). However, capacity attenuation and irreversible phase transitions have been serious challenges for high nickel materials, which greatly affect their electrochemical performances and large-scale storage applications for LIBs. Therefore, this study explores a collaborative strategy to optimize the electrochemical behavior of NCM811 by introducing non-electrochemical activity Zr with high valence and strong binding energy of Zr-O into the Li layers. The enhancement of the electrochemical performances results from diversified influences of Zr doping: the strong binding energy of Zr-O can stabilize the structure and inhibit side reactions and irreversible phase transitions; substituting high valence Zr⁴⁺ into Li sites offers a wider channel for Li⁺ intercalation/extraction during the process of charge/discharge. Furthermore, Li/Ni mixing can be effectively regulated with appropriate amounts of Zr⁴⁺ ions as partial substitutes for Li⁺ ions and suitable Li/Ni mixing is beneficial to the thermal and structural stability of the materials. It is an impactful way to select the appropriate substitute element to promote electrochemical performance, and the method could also be applied to other high nickel layered cathode materials.
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