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; Gerbrand Ceder

doi:10.1038/s41467-024-45030-7

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

Nat Commun. 2024 Jan 29;15(1):858. doi: 10.1038/s41467-024-45030-7.

Authors

Mouhamad S Diallo^#¹, Tan Shi¹, Yaqian Zhang¹, Xinxing Peng¹, Imtiaz Shozib², Yan Wang³, Lincoln J Miara³, Mary C Scott^{1

4}, Qingsong Howard Tu^#^{5

6}, Gerbrand Ceder^{7

8}

Affiliations

¹ Department of Materials Science and Engineering, University of California, Berkeley, CA, 94720, USA.
² Department of Mechanical Engineering, Rochester Institute of Technology, Rochester, NY, 14623, USA.
³ Advanced Materials Lab, Samsung Advanced Institute of Technology-America, Samsung Semiconductor Inc., Cambridge, MA, 02138, USA.
⁴ National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA, 94720, USA.
⁵ Department of Mechanical Engineering, Rochester Institute of Technology, Rochester, NY, 14623, USA. howard.tu@rit.edu.
⁶ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA. howard.tu@rit.edu.
⁷ Department of Materials Science and Engineering, University of California, Berkeley, CA, 94720, USA. gceder@berkeley.edu.
⁸ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA. gceder@berkeley.edu.

^# Contributed equally.

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 [Formula: see text] 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.

Abstract

Grants and funding