Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes

Porz, Lukas; Swamy, Tushar; Sheldon, Brian W.; Rettenwander, Daniel; Frömling, Till; Thaman, Henry L.; Berendts, Stefan; Uecker, Reinhard; Carter, W. Craig; Chiang, Yet‐Ming

doi:10.1002/aenm.201701003

Title: Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes

Journal Article · Thu Jul 06 00:00:00 EDT 2017 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201701003· OSTI ID:1400633

Porz, Lukas ^[1];

^[2]; Sheldon, Brian W. ^[3]; Rettenwander, Daniel ^[4]; Frömling, Till ^[5]; Thaman, Henry L. ^[4]; Berendts, Stefan ^[6]; Uecker, Reinhard ^[7]; Carter, W. Craig ^[4]; Chiang, Yet‐Ming ^[4]

Department of Material Science and Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA, Institute of Materials Science Technische Universität Darmstadt Darmstadt 64287 Germany
Department of Mechanical Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA
School of Engineering Brown University Providence RI 02912 USA
Department of Material Science and Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA
Institute of Material Science Technische Universität Darmstadt 64287 Darmstadt Germany
Department of Chemistry Technische Universität Berlin 10623 Berlin Germany
Leibniz Institute for Crystal Growth (IKZ) 12489 Berlin Germany

Abstract Li deposition is observed and measured on a solid electrolyte in the vicinity of a metallic current collector. Four types of ion‐conducting, inorganic solid electrolytes are tested: Amorphous 70/30 mol% Li ₂ S‐P ₂ S ₅ , polycrystalline β‐Li ₃ PS ₄ , and polycrystalline and single‐crystalline Li ₆ La ₃ ZrTaO ₁₂ garnet. The nature of lithium plating depends on the proximity of the current collector to defects such as surface cracks and on the current density. Lithium plating penetrates/infiltrates at defects, but only above a critical current density. Eventually, infiltration results in a short circuit between the current collector and the Li‐source (anode). These results do not depend on the electrolytes shear modulus and are thus not consistent with the Monroe–Newman model for “dendrites.” The observations suggest that Li‐plating in pre‐existing flaws produces crack‐tip stresses which drive crack propagation, and an electrochemomechanical model of plating‐induced Li infiltration is proposed. Lithium short‐circuits through solid electrolytes occurs through a fundamentally different process than through liquid electrolytes. The onset of Li infiltration depends on solid‐state electrolyte surface morphology, in particular the defect size and density.

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Sponsoring Organization:: USDOE

OSTI ID:: 1400633

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Vol. 7 Journal Issue: 20; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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