Suppressing the Jahn–Teller Effect in Mn-Based Layered Oxide Cathode toward Long-Life Potassium-Ion Batteries

Xiao Zhitong; Xia Fanjie; Xu LinhanWang XuanpengMeng JiashenWang HongZhang XiaoGeng LishanWu JinsongMai Liqiang

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Suppressing the Jahn–Teller Effect in Mn-Based Layered Oxide Cathode toward Long-Life Potassium-Ion Batteries

机译：Suppressing the Jahn–Teller Effect in Mn-Based Layered Oxide Cathode toward Long-Life Potassium-Ion Batteries

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Mn-based layered oxides are one of the most appealing cathodes for potassium-ion batteries (PIBs) because of their high theoretical capacity. However, the Jahn-Teller effect of Mn3+ induces detrimental structural disorder and irreversible phase transition, leading to inferior cycling stability. Herein, an efficient strategy to suppress the Jahn-Teller effect in Mn-based layered oxides by regulating the Mn average valence is demonstrated. To verify this strategy, Ti4+ and Mg2+ ions are chosen and introduced into the layered oxides (K0.5Mn0.7Co0.2Fe0.1O2), which can enhance the structural stability but have opposite effects on the regulation of Mn3+/4+ valence. The K0.5Mn0.6Co0.2Fe0.1Mg0.1O2 with a higher Mn valence (4+) exhibits long-term cycling stability as a PIB cathode compared to the K0.5Mn0.6Co0.2Fe0.1Ti0.1O2 with a lower Mn valence (3.667+). Meanwhile, the detrimental phase transition from P3 to O3 caused by Jahn-Teller effect is completely suppressed, and is replaced by a highly reversible single-phase solid solution reaction for K0.5Mn0.6Co0.2Fe0.1Mg0.1O2. The enhanced cycling stability and single-phase reaction are attributed to the suppressed Jahn-Teller effect via Mn valence regulation, confirmed by first-principles calculations. Therefore, this discovery paves the way for the development of advanced layered cathodes for the next-generation high-performance PIBs.

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《Advanced functional materials》 |2022年第14期|2108244.1-2108244.9|共9页
作者
Xiao Zhitong; Xia Fanjie; Xu LinhanWang XuanpengMeng JiashenWang HongZhang XiaoGeng LishanWu JinsongMai Liqiang;
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Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China;

Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China|Wuhan Univ Technol, Nanostruct Res Ctr NRC, Wuhan 430070, Peoples R China;

Xiamen Univ, Collaborat Innovat Centpotassiumer Optoelect Semi, Dept Phys, Xiamen 361005, Peoples R ChinaWuhan Univ Technol, Sch Sci, Dept Phys Sci & Technol, Wuhan 430070, Peoples R China|Xianhu Hydrogen Valley, Adv Energy Sci & Technol Guangdong Lab, Foshan Xianhu Lab, Foshan 528200, Peoples R ChinaWuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China|Xianhu Hydrogen Valley, Adv Energy Sci & Technol Guangdong Lab, Foshan Xianhu Lab, Foshan 528200, Peoples R China;

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Jahn-Teller effect; long-term cycling stability; Mn-based layered cathodes; potassium-ion batteries; valence regulating;

Suppressing the Jahn–Teller Effect in Mn-Based Layered Oxide Cathode toward Long-Life Potassium-Ion Batteries

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