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An intermediate temperature garnet-type solid electrolyte-based molten lithium battery for grid energy storage

Abstract

Batteries are an attractive grid energy storage technology, but a reliable battery system with the functionalities required for a grid such as high power capability, high safety and low cost remains elusive. Here, we report a solid electrolyte-based molten lithium battery constructed with a molten lithium anode, a molten Sn–Pb or Bi–Pb alloy cathode and a garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) solid electrolyte tube. We show that the assembled Li||LLZTO||Sn–Pb and Li||LLZTO||Bi–Pb cells can stably cycle at an intermediate temperature of 240 °C for about one month at current densities of 50 mA cm−2 and 100 mA cm−2 respectively, with almost no capacity decay and an average Coulombic efficiency of 99.98%. Furthermore, the cells demonstrate high power capability with current densities up to 300 mA cm−2 (90 mW cm−2) for Li||LLZTO||Sn–Pb and 500 mA cm−2 (175 mW cm−2) for Li||LLZTO||Bi–Pb. Our design offers prospects for grid energy storage with intermediate temperature operations, high safety margin and low capital and maintenance costs.

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Fig. 1: Schematic and optical image of the Li||LLZTO||liquid cathode battery.
Fig. 2: Electrochemical performance of a Li||LLZTO||Sn–Pb cell operating at 240 °C.
Fig. 3: Electrochemical performance of a Li||LLZTO||Bi–Pb cell operating at 240 °C.
Fig. 4: Freezing and thawing test of the Li||LLZTO||Sn–Pb cell and the Li||LLZTO||Bi–Pb cell.
Fig. 5

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Acknowledgements

Y.C. acknowledges support from the Joint Center for Energy Storage Research, a battery hub under the US Department of Energy. H.W. acknowledges support from the National Basic Research of China (Grants 2015CB932500), National Natural Science Foundations of China (grants 51661135025 and 51522207). C.A.W. acknowledges support from the National Natural Science Foundations of China (grant 51572145).

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Authors

Contributions

Y.J., K.L., H.W. and Y.C. conceived the idea. Y.J. and K.L. designed the battery cells and conducted the electrochemical measurements. J.L. and Z.H. conducted SEM and XRD characterization. H.W. and Y.C. supervised the project. Y.J., K.L. D.Z., C.A.W., H.W. and Y.C. contributed to writing the manuscript. Y.J. and K.L. contributed equally to this work. All authors discussed the results and commented on the manuscript.

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Correspondence to Hui Wu or Yi Cui.

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The authors declare no competing interests.

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Supplementary Information

Supplementary Figures 1–19 and Supplementary Tables 1–3

Supplementary Video 1

Vibration and impact experiment of the LLZTO tube

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Jin, Y., Liu, K., Lang, J. et al. An intermediate temperature garnet-type solid electrolyte-based molten lithium battery for grid energy storage. Nat Energy 3, 732–738 (2018). https://doi.org/10.1038/s41560-018-0198-9

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