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Dense garnet-type electrolyte with coarse grains for improved air stability and ionic conductivity

Zeng, Xiaomei and Martinolich, Andrew J. and See, Kimberly A. and Faber, Katherine T. (2020) Dense garnet-type electrolyte with coarse grains for improved air stability and ionic conductivity. Journal of Energy Storage, 27 . Art. No. 101128. ISSN 2352-152X. doi:10.1016/j.est.2019.101128.

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Garnet-type electrolytes with high ionic conductivity and chemical stability against lithium metal show promise as solid-state electrolytes for lithium-ion batteries. However, a high concentration of pores and grain boundaries in air-processed polycrystalline electrolytes makes them prone to dendrite formation and reaction with atmospheric moisture, leading to electrochemical and mechanical instability. In this work, we illustrate that abnormal grain growth, an often-avoided phenomenon in conventional ceramic processing, can be employed as a unique approach to obtain extraordinarily large oligo crystals for minimal grain boundaries. Here we report a straightforward approach to develop a robust Ga-doped garnet, Li_(6.25)Ga_(0.25)La_3Zr_2O_(12) (LGLZO) electrolyte with conventional solid-state sintering in air. By preparing nanopowders without agglomeration through ball milling and freeze drying, we can control the microstructure of air-sintered electrolytes for desirable properties of a high density (98% of theoretical density) and an average grain size of 460 µm. The robust air-processed LGLZO electrolytes demonstrate high ionic conductivity, stability in air, and mechanical robustness relative to other garnet electrolytes offering promise as cost- and performance-competitive solid-state electrolytes for safe lithium-ion batteries.

Item Type:Article
Related URLs:
URLURL TypeDescription
Martinolich, Andrew J.0000-0002-7866-9594
See, Kimberly A.0000-0002-0133-9693
Faber, Katherine T.0000-0001-6585-2536
Additional Information:© 2019 Elsevier. Received 26 July 2019, Revised 10 November 2019, Accepted 1 December 2019, Available online 23 December 2019. X. M. Z. and A. J. M. acknowledge postdoctoral fellowships from the Resnick Sustainability Institute at Caltech. K. A. S. and A. J. M. acknowledge financial support from Caltech and the Dow Next Generation Educator Fund. The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Funding AgencyGrant Number
Resnick Sustainability InstituteUNSPECIFIED
Dow Next Generation Educator FundUNSPECIFIED
Subject Keywords:Solid state electrolyte; Garnet; Abnormal grain growth; Freeze drying; Ionic conductivity; Fracture toughness
Record Number:CaltechAUTHORS:20191224-093208324
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Official Citation:Xiaomei Zeng, Andrew J. Martinolich, Kimberly A. See, Katherine T. Faber, Dense garnet-type electrolyte with coarse grains for improved air stability and ionic conductivity, Journal of Energy Storage, Volume 27, 2020, 101128, ISSN 2352-152X,
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100435
Deposited By: George Porter
Deposited On:24 Dec 2019 17:51
Last Modified:16 Nov 2021 17:54

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