Single-phase local-high-concentration solid polymer electrolytes for lithium-metal batteries

Weiran Zhang, Volodymyr Koverga, Sufu Liu, Jigang Zhou, Jian Wang, Panxing Bai, Sha Tan, Naveen K. Dandu, Zeyi Wang, Fu Chen, Jiale Xia, Hongli Wan, Xiyue Zhang, Haochen Yang, Brett L. Lucht, Ai-Min Li, Xiao-Qing Yang, Enyuan Hu, Srinivasa R. Raghavan (), Anh T. Ngo () and Chunsheng Wang ()
Additional contact information
Weiran Zhang: University of Maryland
Volodymyr Koverga: Materials Science Division, Argonne National Laboratory
Sufu Liu: University of Maryland
Jigang Zhou: Canadian Light Source Inc., University of Saskatchewan
Jian Wang: Canadian Light Source Inc., University of Saskatchewan
Panxing Bai: University of Maryland
Sha Tan: Chemistry Division, Brookhaven National Laboratory
Naveen K. Dandu: Materials Science Division, Argonne National Laboratory
Zeyi Wang: University of Maryland
Fu Chen: University of Maryland
Jiale Xia: University of Maryland
Hongli Wan: University of Maryland
Xiyue Zhang: University of Maryland
Haochen Yang: University of Maryland
Brett L. Lucht: University of Rhode Island
Ai-Min Li: University of Maryland
Xiao-Qing Yang: Chemistry Division, Brookhaven National Laboratory
Enyuan Hu: Chemistry Division, Brookhaven National Laboratory
Srinivasa R. Raghavan: University of Maryland
Anh T. Ngo: Materials Science Division, Argonne National Laboratory
Chunsheng Wang: University of Maryland

Nature Energy, 2024, vol. 9, issue 4, 386-400

Abstract: Abstract Solid polymers are promising electrolytes for Li-metal batteries, but they have limitations: they cannot simultaneously achieve high ionic conductivity, good mechanical strength and compatibility with high-voltage cathodes while suppressing Li dendrites. Here, we design a class of locally high-concentration solid polymer electrolytes based on polymer blends, which are termed Li-polymer in F diluter (LPIFD). The Li-polymer (polymer-in-salt) ensures continuous Li-ion conduction channels and contributes to the solid electrolyte interphase (SEI), and the F diluter (inert fluorinated polymer) adds mechanical strength. Studies reveal that a single-phase LPIFD, which is based on a miscible polymer blend, lacks phase boundaries and forms an organic-less and LiF-rich SEI, effectively suppressing lithium dendrites. The single-phase LPIFD delivers ionic conductivity of 3.0 × 10−4 S cm−1, and enables the Li anode to reach a high coulombic efficiency of 99.1% and a critical current density of 3.7 mA cm−2. Furthermore, the ability to form an F-rich cathode electrolyte interphase allows LiNi0.8Co0.1Mn0.1O2||Li cells to achieve a cycle life of 450 cycles at a high operating voltage of 4.5 V. This design will inspire efforts to commercialize polymer electrolytes for high-energy Li-metal batteries.

Date: 2024
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DOI: 10.1038/s41560-023-01443-0

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