Dendrite Growth�Microstructure�Stress�Interrelations in Garnet Solid-State Electrolyte

Raj, V and Naik, KG and Vishnugopi, BS and Rana, AK and Manning, AS and Mahapatra, SR and Varun, KR and Singh, V and Nigam, A and McBrayer, JD and Mukherjee, PP and Aetukuri, NPB and Mitlin, D (2024) Dendrite Growth�Microstructure�Stress�Interrelations in Garnet Solid-State Electrolyte. In: Advanced Energy Materials .

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Abstract

This study illustrates how the microstructure of garnet solid-state electrolytes (SSE) affects the stress-state and dendrite growth. Tantalum-doped lithium lanthanum zirconium oxide (LLZTO, Li6.4La3Zr1.4Ta0.6O12) is synthesized by powder processing and sintering (AS), or with the incorporation of intermediate-stage high-energy milling (M). The M compact displays higher density (91.5 vs 82.5 of theoretical), and per quantitative stereology, lower average grain size (5.4 ± 2.6 vs 21.3 ± 11.1 µm) and lower AFM-derived RMS surface roughness contacting the Li metal (45 vs 161 nm). These differences enable symmetric M cells to electrochemically cycle at constant capacity (0.1 mAh cm�2) with enhanced critical current density (CCD) of 1.4 versus 0.3 mA cm�2. It is demonstrated that LLZTO grain size distribution and internal porosity critically affect electrical short-circuit failure, indicating the importance of electronic properties. Lithium dendrites propagate intergranularly through regions where LLZTO grains are smaller than the bulk average (7.4 ± 3.8 µm for AS in a symmetric cell, 3.1 ± 1.4 µm for M in a half-cell). Metal also accumulates in the otherwise empty pores of the sintered compact present along the dendrite path. Mechanistic modeling indicates that reaction and stress heterogeneities are interrelated, leading to current focusing and preferential plating at grain boundaries. © 2024 Wiley-VCH GmbH.

Item Type:	Journal Article
Publication:	Advanced Energy Materials
Publisher:	John Wiley and Sons Inc
Additional Information:	The copyright for this article belongs toJohn Wiley and Sons Inc.
Keywords:	Electronic properties; Garnets; Grain boundaries; Grain size and shape; Lithium compounds; Mechanical alloying; Milling (machining); Powders; Sintering; Solid electrolytes; Solid state devices; Surface roughness; Tantalum compounds; Textures; Zirconium compounds, All solid-state battery; All-solid-state battery; Chemo-mechanical; Electrochemicals; Electrochemical�mechanical; LLZO; Mechanical; Metal dendrite; Oxide electrolytes, Lanthanum compounds
Department/Centre:	Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Date Deposited:	04 Mar 2024 07:06
Last Modified:	04 Mar 2024 07:06
URI:	https://eprints.iisc.ac.in/id/eprint/84202

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