Dilute Electrolytes with Fluorine‐Free Ether Solvents for 4.5 V Lithium Metal Batteries

Author:

Yang Yusi1,Wang Xiaofang2,Zhu Jiacheng3,Tan Lulu1,Li Nan1,Chen Yifan1,Wang Linlin1,Liu Ziqiang4,Yao Xiayin4,Wang Xuefeng3,Ji Xiao5,Zhu Yujie1ORCID

Affiliation:

1. School of Chemistry Beihang University Beijing 100191 P.R. China

2. School of Physics Hubei University Wuhan Hubei 430062 P.R. China

3. Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences College of Materials Science and Opto-Electronic Technology University of Chinese Academy of Sciences Beijing 100190 P.R. China

4. Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo 315201 P.R. China

5. School of Optical and Electronic Information Huazhong University of Science and Technology Wuhan Hubei 430074 P.R. China

Abstract

AbstractThe limited oxidation stability of ether solvents has posed significant challenges for their applications in high‐voltage lithium metal batteries (LMBs). To tackle this issue, the prevailing strategy either adopts a high concentration of fluorinated salts or relies on highly fluorinated solvents, which will significantly increase the manufacturing cost and create severe environmental hazards. Herein, an alternative and sustainable salt engineering approach is proposed to enable the utilization of dilute electrolytes consisting of fluorine (F)‐free ethers in high‐voltage LMBs. The proposed 0.8 M electrolyte supports stable lithium plating‐stripping with a high Coulombic efficiency of 99.47 % and effectively mitigates the metal dissolution, phase transition, and gas release issues of the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode upon charging to high voltages. Consequently, the 4.5 V high‐loading Li||NCM 811 cell shows a capacity retention of 75.2 % after 300 cycles. Multimodal experimental characterizations coupled with theoretical investigations demonstrate that the boron‐containing salt plays a pivotal role in forming the passivation layers on both anode and cathode. The present simple and cost‐effective electrolyte design strategy offers a promising and alternative avenue for using commercially mature, environmentally benign, and low‐cost F‐free ethers in high‐voltage LMBs.

Funder

National Natural Science Foundation of China

Key Technologies Research and Development Program

Natural Science Foundation of Beijing Municipality

Publisher

Wiley

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