High entropy liquid electrolytes for lithium batteries

Qidi Wang, Chenglong Zhao (), Jianlin Wang, Zhenpeng Yao, Shuwei Wang, Sai Govind Hari Kumar, Swapna Ganapathy, Stephen Eustace, Xuedong Bai, Baohua Li and Marnix Wagemaker ()
Additional contact information
Qidi Wang: Delft University of Technology
Chenglong Zhao: Delft University of Technology
Jianlin Wang: State Key Laboratory for Surface Physics, Institute of Physics, Chinese Academy of Sciences
Zhenpeng Yao: Shanghai Jiao Tong University
Shuwei Wang: Tsinghua University
Sai Govind Hari Kumar: University of Toronto
Swapna Ganapathy: Delft University of Technology
Stephen Eustace: Delft University of Technology
Xuedong Bai: State Key Laboratory for Surface Physics, Institute of Physics, Chinese Academy of Sciences
Baohua Li: Tsinghua University
Marnix Wagemaker: Delft University of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract High-entropy alloys/compounds have large configurational entropy by introducing multiple components, showing improved functional properties that exceed those of conventional materials. However, how increasing entropy impacts the thermodynamic/kinetic properties in liquids that are ambiguous. Here we show this strategy in liquid electrolytes for rechargeable lithium batteries, demonstrating the substantial impact of raising the entropy of electrolytes by introducing multiple salts. Unlike all liquid electrolytes so far reported, the participation of several anionic groups in this electrolyte induces a larger diversity in solvation structures, unexpectedly decreasing solvation strengths between lithium ions and solvents/anions, facilitating lithium-ion diffusivity and the formation of stable interphase passivation layers. In comparison to the single-salt electrolytes, a low-concentration dimethyl ether electrolyte with four salts shows an enhanced cycling stability and rate capability. These findings, rationalized by the fundamental relationship between entropy-dominated solvation structures and ion transport, bring forward high-entropy electrolytes as a composition-rich and unexplored space for lithium batteries and beyond.

Date: 2023
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DOI: 10.1038/s41467-023-36075-1

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