Abstract
State-of-the-art oxides and sulfides with high Li-ion conductivity and good electrochemical stability are among the most promising candidates for solid-state electrolytes in secondary batteries. Yet emerging halides offer promising alternatives because of their intrinsic low Li+ migration energy barriers, high electrochemical oxidative stability, and beneficial mechanical properties. Mechanochemical synthesis has enabled the characterization of LiAlX4 compounds to be extended and the iodide, LiAlI4, to be synthesized for the first time (monoclinic P21/c, Z = 4; a = 8.0846(1) Å; b = 7.4369(1) Å; c = 14.8890(2) Å; β = 93.0457(8)°). Of the tetrahaloaluminates, LiAlBr4 exhibited the highest ionic conductivity at room temperature (0.033 mS cm–1), while LiAlCl4 showed a conductivity of 0.17 mS cm–1 at 333 K, coupled with the highest thermal and oxidative stability. Modeling of the diffusion pathways suggests that the Li-ion transport mechanism in each tetrahaloaluminate is closely related and mediated by both halide polarizability and concerted complex anion motions.
Highlights
State-of-the-art oxides and sulfides with high Liion conductivity and good electrochemical stability are among the most promising candidates for solid-state electrolytes in secondary batteries
Oxide- and sulfide-based materials have been the main focus of research because of the remarkable ionic conductivity that can be achieved at room temperature
It should be noted that the ionic conductivity for LiAlCl4 measured here is 1 order of magnitude higher than that reported by Weppner and Huggins.[18]
Summary
State-of-the-art oxides and sulfides with high Liion conductivity and good electrochemical stability are among the most promising candidates for solid-state electrolytes in secondary batteries.
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