A stable quasi-solid electrolyte improves the safe operation of highly efficient lithium-metal pouch cells in harsh environments

Zhi Chang; Huijun Yang; Xingyu Zhu; Ping He; Haoshen Zhou

doi:10.1038/s41467-022-29118-6

A stable quasi-solid electrolyte improves the safe operation of highly efficient lithium-metal pouch cells in harsh environments

Nat Commun. 2022 Mar 21;13(1):1510. doi: 10.1038/s41467-022-29118-6.

Authors

Zhi Chang¹, Huijun Yang^{1

2}, Xingyu Zhu^{1

2}, Ping He³, Haoshen Zhou^{4

5

6}

Affiliations

¹ Energy Technology Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1, Umezono, Tsukuba, 305-8568, Japan.
² Graduate School of System and Information Engineering, University of Tsukuba, 1-1-1, Tennoudai, Tsukuba, 305-8573, Japan.
³ Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, P. R. China.
⁴ Energy Technology Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1, Umezono, Tsukuba, 305-8568, Japan. hszhou@nju.edu.cn.
⁵ Graduate School of System and Information Engineering, University of Tsukuba, 1-1-1, Tennoudai, Tsukuba, 305-8573, Japan. hszhou@nju.edu.cn.
⁶ Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, P. R. China. hszhou@nju.edu.cn.

Abstract

Nanoconfined/sub-nanoconfined solvent molecules tend to undergo dramatic changes in their properties and behaviours. In this work, we find that unlike typical bulk liquid electrolytes, electrolytes confined in a sub-nanoscale environment (inside channels of a 6.5 Å metal-organic framework, defined as a quasi-solid electrolyte) exhibits unusual properties and behaviours: higher boiling points, highly aggregated configurations, decent lithium-ion conductivities, extended electrochemical voltage windows (approximately 5.4 volts versus Li/Li⁺) and nonflammability at high temperatures. We incorporate this interesting electrolyte into lithium-metal batteries (LMBs) and find that LMBs cycled in the quasi-solid electrolyte demonstrate an electrolyte interphase-free (CEI-free) cathode and dendrite-free Li-metal surface. Moreover, high-voltage LiNi_0.8Co_0.1Mn_0.1O₂//Li (NCM-811//Li with a high NCM-811 mass loading of 20 mg cm^-2) pouch cells assemble with the quasi-solid electrolyte deliver highly stable electrochemical performances even at a high working temperature of 90 °C (171 mAh g^-1 after 300 cycles, 89% capacity retention; 164 mAh g^-1 after 100 cycles even after being damaged). This strategy for fabricating nonflammable and ultrastable quasi-solid electrolytes is promising for the development of safe and high-energy-density LIBs/LMBs for powering electronic devices under various practical working conditions.