Designing Bidirectionally Functional Polymer Electrolytes for Stable Solid Lithium Metal Batteries

The development of high energy density lithium metal batteries has been retarded by the uncontrolled lithium dendrite formation and unstable Ni‐rich cathode–electrolyte interface (CEI). Herein, the bidirectionally functional polymer electrolytes (BDFPE) are designed via direct UV solidification of f...

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Bibliographic Details
Published in:Advanced energy materials 2023-03, Vol.13 (11), p.n/a
Main Authors: Ma, Qiang, Fu, Sha, Wu, An‐Jun, Deng, Qi, Li, Wei‐Dong, Yue, Dan, Zhang, Bing, Wu, Xiong‐Wei, Wang, Zhen‐Ling, Guo, Yu‐Guo
Format: Article
Language:English
Subjects:
Additives
Anodes
Cathodes
Cycles
Electrodes
electrode–electrolyte interface
Electrolytes
Electrolytic cells
functional polymer electrolytes
Interfaces
Lithium
Lithium batteries
lithium metal anodes
lithium metal batteries
Molten salt electrolytes
nickel‐rich cathodes
Polymers
Solid electrolytes
Solidification
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Summary:The development of high energy density lithium metal batteries has been retarded by the uncontrolled lithium dendrite formation and unstable Ni‐rich cathode–electrolyte interface (CEI). Herein, the bidirectionally functional polymer electrolytes (BDFPE) are designed via direct UV solidification of functional polymer species on electrode surfaces to simultaneously handle the interface issues faced by anodes and cathodes. By constructing the BDFPE, a smooth and dendrite‐free lithium deposition is enabled for Li||Li symmetry cells after 1800 h ultralong cycling at 1 mA cm−2 and 1 mAh cm−2, which are attributed to the fast ion conductivity (5.84 × 10−4 S cm−1), high Li+ transfer number (0.69) of BDFPE and low interfacial resistance between electrode and solid electrolytes. Furthermore, Li||LiNi0.6Co0.2Mn0.2O2 batteries demonstrate a favorable cycling and rate capability, and a stable and phosphate‐based CEI layer is constructed in situ. DFT studies reveal that the functional additives FEC and TEP participate in the interface formation. The finding provides a promising design strategy to accommodate the anode and cathode interfaces for high energy density lithium metal batteries. Bidirectionally functional polymer electrolytes are designed directly via UV solidification of functional species on electrode surfaces to simultaneously handle the interface issues faced by the anode and cathode. Meanwhile, a stable solid electrolyte interphase and phosphate‐based cathode–electrolyte interface layer is constructed. The finding provides a promising design strategy to accommodate the anode and cathode interfaces for high energy density solid lithium metal batteries.
ISSN:1614-6832
1614-6840
DOI:10.1002/aenm.202203892