Abstract
In-situ polymerized electrolytes significantly enhance the interfacial compatibility of lithium metal batteries (LMBs). Typically, in-situ polymerized 1,3-dioxolane (PDOL) exhibits low interfacial resistance, yet still suffers from low ionic conductivity and a narrow electrochemical stability window (ESW). Here, an ultra-stable PDOL-based polymer electrolyte is developed by incorporating plasticizers of tetramethylene sulfone (TMS) and fluorinated ethylene carbonate (FEC) into the 3D cross-linked network, achieving a significant enhancement in the transport capacity and efficiency of Li-ion. The ionic conductivity reaches 3.63×10−4 S cm−1 even at room temperature, and the transference number (\(t_{{\rm Li}^{+}}\)) is even higher at 0.85. Furthermore, the ESW of this electrolyte can be increased to 4.5 V with the addition of TMS, which forms a thin and robust antioxidant cathode-electrolyte interface (CEI) on the surface of high-voltage LiCoO2. FEC generates an inorganic-rich solid-electrolyte interface (SEI) on the Li anode, which effectively inhibits the growth of lithium dendrites. Benefiting from the aforementioned advantages, the high-voltage lithium metal battery demonstrates outstanding long-cycle stability, with 93.2% capacity retention after 200 cycles. This work offers a straightforward and accessible method for the practical implementation of high energy density in-situ polymerized solid-state LMBs.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (52202327), and Science and Technology Commission of Shanghai Municipality (22ZR1471300).
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Supporting information The supporting information is available online at chem.scichina.com and link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.
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Supporting Information: In-situ construction of PDOL electrolyte with dual-reinforced stable interface for high-voltage lithium metal batteries
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Wu, Y., Bai, Y., Dong, W. et al. In-situ construction of PDOL electrolyte with dual-reinforced stable interface for high-voltage lithium metal batteries. Sci. China Chem. 67, 1664–1671 (2024). https://doi.org/10.1007/s11426-023-1953-2
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DOI: https://doi.org/10.1007/s11426-023-1953-2