Journal
ADVANCED ENERGY MATERIALS
Volume 12, Issue 3, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202102825
Keywords
electrochemical-mechanical interactions; filament propagation; grain boundaries; lithium metal anodes; mesoscale mechanisms; solid-state batteries
Categories
Funding
- National Science Foundation [2041499, 1727863, 1847029]
- Alfred P. Sloan Foundation through a Scialog: Advanced Energy Storage award
- DOE Office of Science [DE-AC02-06CH11357]
- Directorate For Engineering
- Div Of Civil, Mechanical, & Manufact Inn [1727863] Funding Source: National Science Foundation
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [2041499] Funding Source: National Science Foundation
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This study provides comprehensive insights into the mechanical and electrochemical interactions at the mesoscale level in solid-state batteries, revealing the impact of grain boundaries on electrodeposition morphology and mechanical stability of the solid-state electrolyte. Furthermore, it delineates a crack formation and void filling mechanism triggered by the heterogeneous nature of electrochemical-mechanical interactions at the GB-electrode junction.
Solid-state batteries (SSBs), utilizing a lithium metal anode, promise to deliver enhanced energy and power densities compared to conventional lithium-ion batteries. Penetration of lithium filaments through the solid-state electrolytes (SSEs) during electrodeposition poses major constraints on the safety and rate performance of SSBs. While microstructural attributes, especially grain boundaries (GBs) within the SSEs are considered preferential metal propagation pathways, the underlying mechanisms are not fully understood yet. Here, a comprehensive insight is presented into the mechanistic interactions at the mesoscale including the electrochemical-mechanical response of the GB-electrode junction and competing ion transport dynamics in the SSE. Depending on the GB transport characteristics, a highly non-uniform electrodeposition morphology consisting of either cavities or protrusions at the GB-electrode interface is identified. Mechanical stability analysis reveals localized strain ramps in the GB regions that can lead to brittle fracture of the SSE. For ionically less conductive GBs compared to the grains, a crack formation and void filling mechanism, triggered by the heterogeneous nature of electrochemical-mechanical interactions is delineated at the GB-electrode junction. Concurrently, in situ X-ray tomography of pristine and failed Li7La3Zr2O12 (LLZO) SSE samples confirm the presence of filamentous lithium penetration and validity of the proposed mesoscale failure mechanisms.
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