物理化学学报 >> 2026, Vol. 42 >> Issue (3): 100181.doi: 10.1016/j.actphy.2025.100181

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双层锰酸盐正极LaSr2Mn2O6.96在全固态氟离子电池中的结构与电化学行为

Vanita Vanita1, Roland Schoch2, Pascal Puphal3, Hasan Yilmaz1, Matthias Bauer2, Oliver Clemens1,*()   

  1. 1 University of Stuttgart, Institute for Materials Science, Materials Synthesis Group, Heisenbergstra?e 3, 70569 Germany
    2 Institute of Inorganic Chemistry and Center for Sustainable Systems Design (CSSD), Paderborn University, Warburger Stra?e 100, 33098 Paderborn, Germany
    3 Max-Planck-Institute, Heisenbergstr. 1, 70569 Stuttgart, Germany
  • 收稿日期:2025-06-30 修回日期:2025-08-27 录用日期:2025-09-04 发布日期:2026-01-05
  • 通讯作者: Email: oliver.clemens@imw.uni-stuttgart.de (Oliver Clemens)

Structural and electrochemical behaviour of bilayer manganite LaSr2Mn2O6.96 cathode for all-solid-state fluoride ion batteries

Vanita Vanita1, Roland Schoch2, Pascal Puphal3, Hasan Yilmaz1, Matthias Bauer2, Oliver Clemens1,*()   

  1. 1 University of Stuttgart, Institute for Materials Science, Materials Synthesis Group, Heisenbergstra?e 3, 70569 Germany
    2 Institute of Inorganic Chemistry and Center for Sustainable Systems Design (CSSD), Paderborn University, Warburger Stra?e 100, 33098 Paderborn, Germany
    3 Max-Planck-Institute, Heisenbergstr. 1, 70569 Stuttgart, Germany
  • Received:2025-06-30 Revised:2025-08-27 Accepted:2025-09-04 Published:2026-01-05
  • Contact: Email: oliver.clemens@imw.uni-stuttgart.de (Oliver Clemens)

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摘要：

本研究探讨了Ruddlesden-Popper型双层锰酸盐LaSr2Mn2O6.96作为全固态氟离子电池(FIBs)插层型正极材料的潜力。通过非原位X射线衍射分析了LaSr2Mn2O6.96在氟离子嵌入/脱嵌过程中的结构变化，发现F−的嵌入会形成三种不同的四方相。为理解这些物相的复杂行为，采用X射线吸收光谱和磁学测量手段研究了Mn氧化态及配位环境的变化。在20 kN的堆叠压力和1 V至−1 V电位区间的电化学循环中，LaSr2Mn2O6.96的比容量从初始的~30 mAh g−1持续增加至200次循环后的~68 mAh g−1，库仑效率达~99%，且未出现容量衰减迹象。这表明双层锰酸盐LaSr2Mn2O6.96有望成为循环稳定的全固态FIBs正极材料，尤其是在施加堆叠压力的条件下。

关键词: 电池, 全固态氟离子电池, 氟化, 脱氟, Ruddlesden-Popper型结构, 双层锰酸盐, 插层型正极, 电化学性能

Abstract:

In this study, we explore the potential of the Ruddlesden-Popper (RP)-type bilayer manganite LaSr2Mn2O6.96 as an intercalation-based cathode material for all-solid-state fluoride ion batteries (FIBs). Structural changes of LaSr2Mn2O6.96 during fluoride intercalation and de-intercalation were analyzed via ex situ X-ray diffraction, revealing that F− insertion induces the formation of three distinct tetragonal phases. To understand the complex behavior of these phases, we examined the changes in the Mn oxidation state and coordination environment using X-ray absorption spectroscopy and magnetic measurements. Under stack pressure (20 kN), electrochemical cycling of LaSr2Mn2O6.96 in the potential range of 1 V to −1 V exhibited a continuous increase in specific capacity from capacity of ~30 mAh g−1 to ~68 mAh g−1 over 200 cycles, with ~99% coulombic efficiency and no signs of capacity fading. This makes the bilayer manganite LaSr2Mn2O6.96 a promising candidate for a cycling stable cathode for all-solid-state FIBs, especially under the application of stack pressure.

Key words: Battery, All solid-state fluoride ion battery, Fluorination, Defluorination, Ruddlesden-Popper type structure, Bilayer manganite, Intercalation-type cathode, Electrochemical performance