锰
歧化
镍
雅恩-泰勒效应
阴极
离子
电化学
材料科学
无机化学
化学
氧化还原
相(物质)
电极
冶金
物理化学
催化作用
有机化学
生物化学
作者
Peiyu Hou,Mengyang Dong,Zezhou Lin,Zhong-Xi Sun,Maoguo Gong,Feng Li,Xijin Xu
出处
期刊:ACS Sustainable Chemistry & Engineering
[American Chemical Society]
日期:2023-06-27
卷期号:11 (29): 10785-10794
被引量:2
标识
DOI:10.1021/acssuschemeng.3c01854
摘要
P3-type manganese-based cathodes with high specific capacity and low cost have attracted considerable attention. But the Mn3+ with unpaired, eg* electron gives rise to the Jahn-Teller distortion and disproportionation reaction, which further leads to the rapid capacity/voltage decay. In this work, we design a compositionally graded P3-type manganese-based oxide, in which the nickel content increases linearly while the manganese fraction decreases gradually from the interior to the surface of a single particle. At the surface, the nickel/manganese solid solution phase is formed when 1/3 of manganese ions are substituted by nickel, in which all manganese ions act as +4, suggesting the lowered Jahn-Teller distortion and thus induced structural evolutions. The preferable composition of this solid solution is also expected to reduce the disproportionation of Mn3+ ions. Consequently, the stability of the Mn3+/Mn4+ redox couple in the P3-type cathode is significantly improved by building a compositionally graded structure. The graded P3-type electrode shows superior cycling stability with a capacity retention of 72.9% even after 400 cycles at 1C. These findings offer new insight into mitigating the Jahn-Teller effect and thus improving the electrochemical properties of manganese-based cathodes for advanced sodium-ion batteries.
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