Effect of solid-electrolyte pellet density on failure of solid-state batteries

Mouhamad S. Diallo, Tan Shi, Yaqian Zhang, Xinxing Peng, Imtiaz Shozib, Yan Wang, Lincoln J. Miara, Mary C. Scott, Qingsong Howard Tu () and Gerbrand Ceder ()
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Mouhamad S. Diallo: University of California
Tan Shi: University of California
Yaqian Zhang: University of California
Xinxing Peng: University of California
Imtiaz Shozib: Rochester Institute of Technology
Yan Wang: Samsung Semiconductor Inc.
Lincoln J. Miara: Samsung Semiconductor Inc.
Mary C. Scott: University of California
Qingsong Howard Tu: Rochester Institute of Technology
Gerbrand Ceder: University of California

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Despite the potentially higher energy density and improved safety of solid-state batteries (SSBs) relative to Li-ion batteries, failure due to Li-filament penetration of the solid electrolyte and subsequent short circuit remains a critical issue. Herein, we show that Li-filament growth is suppressed in solid-electrolyte pellets with a relative density beyond ~95%. Below this threshold value, however, the battery shorts more easily as the density increases due to faster Li-filament growth within the percolating pores in the pellet. The microstructural properties (e.g., pore size, connectivity, porosity, and tortuosity) of $$75\%{{{{{\rm{L}}}}}}{{{{{{\rm{i}}}}}}}_{2}{{{{{\rm{S}}}}}}-25\%{{{{{{\rm{P}}}}}}}_{2}{{{{{{\rm{S}}}}}}}_{5}$$ 75 % L i 2 S − 25 % P 2 S 5 with various relative densities are quantified using focused ion beam–scanning electron microscopy tomography and permeability tests. Furthermore, modeling results provide details on the Li-filament growth inside pores ranging from 0.2 to 2 μm in size. Our findings improve the understanding of the failure modes of SSBs and provide guidelines for the design of dendrite-free SSBs.

Date: 2024
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DOI: 10.1038/s41467-024-45030-7

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