化学
拉曼光谱
无定形固体
氟化物
快离子导体
离子键合
离子
电解质
吸收(声学)
卤化物
热传导
扩散
电导率
分析化学(期刊)
吸收光谱法
堆栈(抽象数据类型)
从头算
锡
化学物理
无机化学
离子电导率
密度泛函理论
对分布函数
从头算量子化学方法
化学工程
电磁屏蔽
电极
物理化学
光谱学
化学稳定性
分子动力学
作者
Juhyoun Park,Jun Pyo Son,Hae-Yong Kim,J. S. Kim,Changhoon Kim,Jihoon Jeon,Jae-Ryun Lee,Jiwon Seo,Dong‐Hwa Seo,Kyung-Wan Nam,Yoon Seok Jung
摘要
Fluoride solid electrolytes (SEs), despite their extremely low ionic conductivities, offer a promising pathway for enabling 5 V-class chemistries in all-solid-state batteries (ASSBs) owing to their exceptional oxidative stability. Herein, we report a new amorphous oxyfluoride SE, Li 1+ x TaO x F 6– x ( x = 0.0–1.0), which exhibits over 3 orders of magnitude higher Li + conductivity than crystalline LiTaF 6, reaching 1.08 × 10 –6 S cm –1 at 30 °C ( x = 1.0). Pair distribution function analysis, Raman spectroscopy, and X-ray absorption spectroscopy reveal an extended, corner-sharing chain of Ta(O/F) 6/7 polyhedra framework. Melt-quenching ab initio molecular dynamics simulations further demonstrate that this interconnected structure broadens Li + diffusion pathways. Leveraging high oxidative stability (>5 V) and improved Li + conductivity, Li 2 TaOF 5 was implemented as a shielding layer for 5 V-class LiNi 0.5 Mn 1.5 O 4 cathodes, enabling exceptional cycling performance with 85.8% capacity retention after 1000 cycles at 1.0C and 30 °C. Even under high-mass-loading (49.3 mg cm –2 ) or low-temperature (−20 °C) conditions, the modified LNMO electrodes with Li 2 TaOF 5 exhibited promising performance, achieving >5.9 mAh cm –2 with 94% retention. These findings underscore the efficacy of amorphization in advancing fluoride SEs and provide key design insights for advanced halide SEs in high-voltage ASSBs.
科研通智能强力驱动
Strongly Powered by AbleSci AI