Polyfluorinated crosslinker-based solid polymer electrolytes for long-cycling 4.5 V lithium metal batteries

Lingfei Tang, Bowen Chen, Zhonghan Zhang, Changqi Ma, Junchao Chen, Yage Huang, Fengrui Zhang, Qingyu Dong, Guoyong Xue, Daiqian Chen, Chenji Hu, Shuzhou Li, Zheng Liu, Yanbin Shen, Qi Chen () and Liwei Chen ()
Additional contact information
Lingfei Tang: University of Science and Technology of China
Bowen Chen: University of Science and Technology of China
Zhonghan Zhang: CINTRA CNRS/NTU/THALES, UMI 3288
Changqi Ma: University of Science and Technology of China
Junchao Chen: Shanghai Jiao Tong University
Yage Huang: Shanghai Jiao Tong University
Fengrui Zhang: i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences
Qingyu Dong: i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences
Guoyong Xue: Shanghai Jiao Tong University
Daiqian Chen: i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences
Chenji Hu: Shanghai Jiao Tong University
Shuzhou Li: Nanyang Technological University
Zheng Liu: CINTRA CNRS/NTU/THALES, UMI 3288
Yanbin Shen: University of Science and Technology of China
Qi Chen: University of Science and Technology of China
Liwei Chen: i-Lab, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Solid polymer electrolytes (SPEs), which are favorable to form intimate interfacial contacts with electrodes, are promising electrolyte of choice for long-cycling lithium metal batteries (LMBs). However, typical SPEs with easily oxidized oxygen-bearing polar groups exhibit narrow electrochemical stability window (ESW), making it impractical to increase specific capacity and energy density of SPE based LMBs with charging cut-off voltage of 4.5 V or higher. Here, we apply a polyfluorinated crosslinker to enhance oxidation resistance of SPEs. The crosslinked network facilitates transmission of the inductive electron-withdrawing effect of polyfluorinated segments. As a result, polyfluorinated crosslinked SPE exhibits a wide ESW, and the Li|SPE|LiNi0.5Co0.2Mn0.3O2 cell with a cutoff voltage of 4.5 V delivers a high discharge specific capacity of ~164.19 mAh g−1 at 0.5 C and capacity retention of ~90% after 200 cycles. This work opens a direction in developing SPEs for long-cycling high-voltage LMBs by using polyfluorinated crosslinking strategy.

Date: 2023
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DOI: 10.1038/s41467-023-37997-6

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