Microscale mechanical property variations of Al-substituted LLZO: insights from compression testing and molecular dynamics simulations

Ceramic solid electrolytes based on LLZO (Li₇La₃Zr₂O₁₂) are promising candidates for all-solid-state batteries due to their high ionic conductivity and good apparent stability vs. lithium metal, however they are prone to mechanical failure. Lithium metal intrusions, alongside cell stack pressure, transition polycrystalline solid electrolyte grains into a compressed state that promotes crack propagation and fracture. Here this work examines the mechanical response of Al-substituted LLZO to compressive forces by measuring ultimate strength under pillar compression with a flat punch tip. Failure modes characterized by in situ scanning electron microscopy show diverse splitting patterns arising from internal porosity, grain boundaries, and slip planes. Large correlated variations in compressive strength (0.93–2.63 GPa) and Young's modulus (72.1–150.97 GPa) are observed across microscale regions of the solid electrolyte. Molecular dynamics simulations of LLZO with different porosities describe the variation of compressive strength and Young's modulus, and enable a microscale porosity model to be fit accounting for Young's modulus reduction across the solid electrolyte. Overall, the results indicate the importance of microscale mechanical testing of ceramic solid electrolytes to identify preferential sites for mechanical degradation and Li intrusion, and ensure the robust design of all-solid-state lithium metal batteries.. Authors: Moon, Jaron V. [Univ. of Utah, Salt Lake City, UT (United States)] (ORCID:0000000302060448); Sakir, Md Takmil [Utah State Univ., Logan, UT (United States)]; Go, Wooseok [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]; Xie, Rui [Univ. of Utah, Salt Lake City, UT (United States)]; Tucker, Michael C. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]. DOE Contract: AC02-05CH11231. Subjects: 25 ENERGY STORAGE; lithium lanthanum zirconium oxide (LLZO); mechanical properties testing; molecular dynamics (MD); nanoindentation; solid-state lithium metal battery