Designing lithium halide solid electrolytes

Qidi Wang, Yunan Zhou, Xuelong Wang, Hao Guo, Shuiping Gong, Zhenpeng Yao, Fangting Wu, Jianlin Wang, Swapna Ganapathy, Xuedong Bai, Baohua Li, Chenglong Zhao (), Jürgen Janek () and Marnix Wagemaker ()
Additional contact information
Qidi Wang: Delft University of Technology
Yunan Zhou: Tsinghua University
Xuelong Wang: Chemistry Division, Brookhaven National Laboratory
Hao Guo: China Institute of Atomic Energy
Shuiping Gong: Shanghai Jiao Tong University
Zhenpeng Yao: Shanghai Jiao Tong University
Fangting Wu: Tsinghua University
Jianlin Wang: State Key Laboratory for Surface Physics, Institute of Physics, Chinese Academy of Sciences
Swapna Ganapathy: Delft University of Technology
Xuedong Bai: State Key Laboratory for Surface Physics, Institute of Physics, Chinese Academy of Sciences
Baohua Li: Tsinghua University
Chenglong Zhao: Delft University of Technology
Jürgen Janek: Justus-Liebig-University Giessen
Marnix Wagemaker: Delft University of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract All-solid-state lithium batteries have attracted widespread attention for next-generation energy storage, potentially providing enhanced safety and cycling stability. The performance of such batteries relies on solid electrolyte materials; hence many structures/phases are being investigated with increasing compositional complexity. Among the various solid electrolytes, lithium halides show promising ionic conductivity and cathode compatibility, however, there are no effective guidelines when moving toward complex compositions that go beyond ab-initio modeling. Here, we show that ionic potential, the ratio of charge number and ion radius, can effectively capture the key interactions within halide materials, making it possible to guide the design of the representative crystal structures. This is demonstrated by the preparation of a family of complex layered halides that combine an enhanced conductivity with a favorable isometric morphology, induced by the high configurational entropy. This work provides insights into the characteristics of complex halide phases and presents a methodology for designing solid materials.

Date: 2024
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DOI: 10.1038/s41467-024-45258-3

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