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High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes

Author

Listed:
  • Fudong Han

    (University of Maryland)

  • Andrew S. Westover

    (Oak Ridge National Laboratory)

  • Jie Yue

    (University of Maryland)

  • Xiulin Fan

    (University of Maryland)

  • Fei Wang

    (University of Maryland)

  • Miaofang Chi

    (Oak Ridge National Laboratory)

  • Donovan N. Leonard

    (Oak Ridge National Laboratory)

  • Nancy J. Dudney

    (Oak Ridge National Laboratory)

  • Howard Wang

    (University of Maryland)

  • Chunsheng Wang

    (University of Maryland)

Abstract

Solid electrolytes (SEs) are widely considered as an ‘enabler’ of lithium anodes for high-energy batteries. However, recent reports demonstrate that the Li dendrite formation in Li7La3Zr2O12 (LLZO) and Li2S–P2S5 is actually much easier than that in liquid electrolytes of lithium batteries, by mechanisms that remain elusive. Here we illustrate the origin of the dendrite formation by monitoring the dynamic evolution of Li concentration profiles in three popular but representative SEs (LiPON, LLZO and amorphous Li3PS4) during lithium plating using time-resolved operando neutron depth profiling. Although no apparent changes in the lithium concentration in LiPON can be observed, we visualize the direct deposition of Li inside the bulk LLZO and Li3PS4. Our findings suggest the high electronic conductivity of LLZO and Li3PS4 is mostly responsible for dendrite formation in these SEs. Lowering the electronic conductivity, rather than further increasing the ionic conductivity of SEs, is therefore critical for the success of all-solid-state Li batteries.

Suggested Citation

  • Fudong Han & Andrew S. Westover & Jie Yue & Xiulin Fan & Fei Wang & Miaofang Chi & Donovan N. Leonard & Nancy J. Dudney & Howard Wang & Chunsheng Wang, 2019. "High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes," Nature Energy, Nature, vol. 4(3), pages 187-196, March.
    • Handle: RePEc:nat:natene:v:4:y:2019:i:3:d:10.1038_s41560-018-0312-z
    DOI: 10.1038/s41560-018-0312-z
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