The urgent need for safer batteries is leading research to all-solid-state lithium-based cells. To achieve energy density comparable to liquid electrolyte-based cells, ultrathin and lightweight solid electrolytes with high ionic conductivity are desired. However, solid electrolytes with comparable thicknesses to commercial polymer electrolyte separators (~10 μm) used in liquid electrolytes remain challenging to make because of the increased risk of short-circuiting the battery. Here, we report on a polymer–polymer solid-state electrolyte design, demonstrated with an 8.6-μm-thick nanoporous polyimide (PI) film filled with polyethylene oxide/lithium bis(trifluoromethanesulfonyl)imide (PEO/LiTFSI) that can be used as a safe solid polymer electrolyte. The PI film is nonflammable and mechanically strong, preventing batteries from short-circuiting even after more than 1,000 h of cycling, and the vertical channels enhance the ionic conductivity (2.3 × 10−4 S cm−1 at 30 °C) of the infused polymer electrolyte. All-solid-state lithium-ion batteries fabricated with PI/PEO/LiTFSI solid electrolyte show good cycling performance (200 cycles at C/2 rate) at 60 °C and withstand abuse tests such as bending, cutting and nail penetration.
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The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.
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The work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy under the Battery Materials Research (BMR) programme and Battery 500 Consortium programme. Z.L. and L.-Q.C. also acknowledge the support from the Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE), under the Award (DE-EE0007803).
The authors declare no competing interests.
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Supplementary Methods, Supplementary Figs. 1–24 and Supplementary Table 1
Flame test of PP/PE/PP separator
Flame test of PEO/LiTFSI SPE
Flame test of PI film
Nail penetration test of LFP/PI/PEO/LiTFSI/Li pouch cell
Phase evolution of Li deposition with PI/PEO/LiTFSI/PEO/Al2O3
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Wan, J., Xie, J., Kong, X. et al. Ultrathin, flexible, solid polymer composite electrolyte enabled with aligned nanoporous host for lithium batteries. Nat. Nanotechnol. 14, 705–711 (2019). https://doi.org/10.1038/s41565-019-0465-3
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