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调控配位化学以加速用于超稳定钠离子电池的聚阴离子阴极的钠转移动力学

Regulation of Coordination Chemistry To Accelerate Na Transfer Kinetics of Polyanionic Cathodes for Ultrastable Sodium-Ion Batteries.

作者信息

Zhang Tianshu, Zhang Pengcheng, Liu Jie, Zhang Lifang, Zheng Yiwei, Shen Xiaowei, Qian Yijun, Zhou Xi, Zhou Jinqiu, Qian Tao, Yan Chenglin

机构信息

College of Energy, Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou 215006, China.

Suzhou Industrial Park Monash Research Institute of Science and Technology, Suzhou 215000, P. R. China.

出版信息

Nano Lett. 2025 Feb 12;25(6):2150-2158. doi: 10.1021/acs.nanolett.4c04913. Epub 2025 Feb 3.

DOI:10.1021/acs.nanolett.4c04913
PMID:39898532
Abstract

Alluaudite-type iron-based sulfate structure (NaFe(SO)) has attracted wide attention due to its high working voltage and low cost. However, their practical application is hindered by challenges such as limited reversible capacity and sluggish transfer kinetics. Herein, we proposed an anion substitution strategy to optimize iron-based sulfate cathode materials. The electrochemical characterization and theoretical calculations confirmed a reduction in the migration barrier of Na ions in various pathways. Besides, fluorine weakened the electron density of the crystal plane, thereby impeding the continuous side reaction of the electrolyte. As expected, the NFSF cathode can exhibit a capacity of 121.5 mAh g at 12 mA g and keep a high retention of 78.8% after 1000 cycles at 600 mA g. In addition, the NFSF-based cathode and hard carbon (HC)-based anode were assembled into a laboratory-scale pouch cell to demonstrate the electrochemical performance and practical applications.

摘要

阿硫铁钠型铁基硫酸盐结构(NaFe(SO))因其高工作电压和低成本而备受关注。然而,其实际应用受到诸如可逆容量有限和迁移动力学迟缓等挑战的阻碍。在此,我们提出了一种阴离子取代策略来优化铁基硫酸盐阴极材料。电化学表征和理论计算证实了钠离子在各种路径中的迁移势垒降低。此外,氟削弱了晶面的电子密度,从而抑制了电解质的持续副反应。正如预期的那样,NFSF阴极在12 mA g下可表现出121.5 mAh g的容量,在600 mA g下循环1000次后仍保持78.8%的高保留率。此外,将基于NFSF的阴极和基于硬碳(HC)的阳极组装成实验室规模的软包电池,以展示其电化学性能和实际应用。

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