High-entropy electrolytes for practical lithium metal batteries

Sang Cheol Kim, Jingyang Wang, Rong Xu, Pu Zhang, Yuelang Chen, Zhuojun Huang, Yufei Yang, Zhiao Yu, Solomon T. Oyakhire, Wenbo Zhang, Louisa C. Greenburg, Mun Sek Kim, David T. Boyle, Philaphon Sayavong, Yusheng Ye, Jian Qin, Zhenan Bao and Yi Cui ()
Additional contact information
Sang Cheol Kim: Stanford University
Jingyang Wang: Stanford University
Rong Xu: Stanford University
Pu Zhang: Stanford University
Yuelang Chen: Stanford University
Zhuojun Huang: Stanford University
Yufei Yang: Stanford University
Zhiao Yu: Stanford University
Solomon T. Oyakhire: Stanford University
Wenbo Zhang: Stanford University
Louisa C. Greenburg: Stanford University
Mun Sek Kim: Stanford University
David T. Boyle: Stanford University
Philaphon Sayavong: Stanford University
Yusheng Ye: Stanford University
Jian Qin: Stanford University
Zhenan Bao: Stanford University
Yi Cui: Stanford University

Nature Energy, 2023, vol. 8, issue 8, 814-826

Abstract: Abstract Electrolyte engineering is crucial for improving battery performance, particularly for lithium metal batteries. Recent advances in electrolytes have greatly improved cyclability by enhancing electrochemical stability at the electrode interfaces, but concurrently achieving high ionic conductivity has remained challenging. Here we report an electrolyte design strategy for enhanced lithium metal batteries by increasing the molecular diversity in electrolytes, which essentially leads to high-entropy electrolytes. We find that, in weakly solvating electrolytes, the entropy effect reduces ion clustering while preserving the characteristic anion-rich solvation structures, which is characterized by synchrotron-based X-ray scattering and molecular dynamics simulations. Electrolytes with smaller-sized clusters exhibit a twofold improvement in ionic conductivity compared with conventional weakly solvating electrolytes, enabling stable cycling at high current densities up to 2C (6.2 mA cm−2) in anode-free LiNi0.6Mn0.2Co0.2 (NMC622)||Cu pouch cells. The efficacy of the design strategy is verified by performance improvements in three disparate weakly solvating electrolyte systems.

Date: 2023
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DOI: 10.1038/s41560-023-01280-1

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