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Solid-state polymer electrolytes with in-built fast interfacial transport for secondary lithium batteries

Nature Energy volume 4, pages 365–373 (2019)Cite this article

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Abstract

Solid-state electrolytes with high room-temperature ionic conductivity and fast interfacial charge transport are a requirement for practical solid-state batteries. Here, we report that cationic aluminium species initiate ring-opening polymerization of molecular ethers inside an electrochemical cell to produce solid-state polymer electrolytes (SPEs), which retain conformal interfacial contact with all cell components. SPEs exhibit high ionic conductivity at room temperature (>1 mS cm−1), low interfacial resistances, uniform lithium deposition and high Li plating/striping efficiencies (>98% after 300 charge–discharge cycles). Applications of SPEs in Li–S, Li–LiFePO4 and Li–LiNi0.6Mn0.2Co0.2O2 batteries further demonstrate that high Coulombic efficiency (>99%) and long life (>700 cycles) can be achieved with an in situ SPE design. Our study therefore provides a promising direction for creating solid electrolytes that meet both the bulk and interfacial conductivity requirements for practical solid polymer batteries.

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Fig. 1: Preparation of SPEs.
Fig. 2: Kinetics and electrochemical characteristics of SPEs with different concentrations of Al(OTf)3.
Fig. 3: Electrochemical stability of the poly-DOL electrolyte.
Fig. 4: Characterization of SEI formed on Li cycled in liquid DOL and SPE electrolytes.
Fig. 5: Li electrodeposit morphology in the liquid electrolyte and poly-DOL SPEs.
Fig. 6: Full cell demonstration of electrochemical cells using an Li metal anode and poly-DOL SPEs.

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Data availability

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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Acknowledgements

This work was supported by the Department of Energy Basic Energy Sciences programme through award DE-SC0016082. Electron microscopy and XPS analysis were performed in facilities supported by the Cornell Center for Materials Research with funding from the NSF MRSEC programme (DMR-1719875). Q.Z. thanks B. Abel and H. Johnson from the Coates Research Group for fruitful discussions about DOL polymerization.

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Authors and Affiliations

  1. Robert Frederick Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY, USA

    Qing Zhao, Xiaotun Liu, Sanjuna Stalin, Kasim Khan & Lynden A. Archer

  2. Department of Materials Science and Engineering, Cornell University, Ithaca, NY, USA

    Lynden A. Archer

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  1. Qing Zhao
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Contributions

Q.Z. and L.A.A. conceived and designed the experiments. Q.Z. prepared and characterized the polymer electrolyte, as well as electrochemical performance. X.L. and Q.Z. performed thermal and rheology studies of SPEs. Q.Z., X.L. and L.A.A. wrote the original draft. Q.Z. and L.A.A. further wrote and revised the manuscript. All authors contributed to the data analysis. L.A.A. directed the research.

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Correspondence to Lynden A. Archer.

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Supplementary Figures 1–20, Supplementary Table 1, Supplementary References

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Zhao, Q., Liu, X., Stalin, S. et al. Solid-state polymer electrolytes with in-built fast interfacial transport for secondary lithium batteries. Nat Energy 4, 365–373 (2019). https://doi.org/10.1038/s41560-019-0349-7

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