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Manganese charge redistribution induced by high-entropy charge compensation mechanism for aqueous potassium-ion batteries
Energy Storage Materials ( IF 18.9 ) Pub Date : 2024-01-26 , DOI: 10.1016/j.ensm.2024.103221
Bingqiu Liu , Qi Zhang , Lingyu Zhang , Xue Yong , Lu Li , Chungang Wang

In aqueous batteries, Mn-based electrodes suffer from uncontrollable dissolution and Jahn-Teller distortion caused by the formation of Mn3+ during the charging process, resulting in poor cycling stability. Herein, the high-entropy charge compensation mechanism is applied to Mn-based cathode to induce manganese charge redistribution during charge/discharge process. Experimental characterization proves that Mn2+ in cathode has not been oxidized to the conventional Mn3+ upon charging but is in the valence state between +2 and +3 through the high-entropy charge compensation mechanism, while the suppressed Jahn-Teller distortion leads to a solid-solution reaction. Furthermore, the theoretical calculations reveal the robust and insoluble structure of the electrode and the fast K-ion diffusion in the crystal structure. With these advantages, the high-entropy cathode exhibits outstanding cycling performance over 2000 cycles in diluent electrolyte. This work provides a new strategy for Mn-based electrodes in aqueous batteries, which undergo dissolution and Jahn-Teller distortion.



中文翻译:

水系钾离子电池高熵电荷补偿机制引起的锰电荷再分布

在水系电池中,锰基电极在充电过程中会因Mn 3+的形成而导致无法控制的溶解和Jahn-Teller变形,从而导致循环稳定性差。在此,将高熵电荷补偿机制应用于锰基阴极,以在充电/放电过程中诱导锰电荷重新分布。实验表征证明,充电时正极中的Mn 2+并未被氧化为传统的Mn 3+,而是通过高熵电荷补偿机制处于+2至+3价态,同时抑制Jahn-Teller畸变导致至固溶反应。此外,理论计算揭示了电极的坚固且不溶的结构以及晶体结构中的快速钾离子扩散。凭借这些优点,高熵正极在稀释电解质中表现出超过2000次循环的出色循环性能。这项工作为水系电池中的锰基电极提供了一种新策略,该电极会发生溶解和 Jahn-Teller 畸变。

更新日期:2024-01-29
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