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Naji, M. |
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Motta, Antonella |
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Aletan, Dirar |
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Mohamed, Tarek |
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Ertürk, Emre |
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Taccardi, Nicola |
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Kononenko, Denys |
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Petrov, R. H. | Madrid |
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Alshaaer, Mazen | Brussels |
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Bih, L. |
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Casati, R. |
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Muller, Hermance |
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Kočí, Jan | Prague |
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Šuljagić, Marija |
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Kalteremidou, Kalliopi-Artemi | Brussels |
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Azam, Siraj |
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Ospanova, Alyiya |
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Blanpain, Bart |
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Ali, M. A. |
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Popa, V. |
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Rančić, M. |
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Ollier, Nadège |
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Azevedo, Nuno Monteiro |
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Landes, Michael |
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Rignanese, Gian-Marco |
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Naik, Kaustubh G.
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (4/4 displayed)
- 2024Dendrite Growth—Microstructure—Stress—Interrelations in Garnet Solid‐State Electrolytecitations
- 2024Operando Investigation on the Role of Densification and Chemo‐Mechanics on Solid‐State Cathodescitations
- 2024Mechanical Milling – Induced Microstructure Changes in Argyrodite LPSCl Solid‐State Electrolyte Critically Affect Electrochemical Stabilitycitations
- 2023Tuned Reactivity at the Lithium Metal–Argyrodite Solid State Electrolyte Interphasecitations
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article
Mechanical Milling – Induced Microstructure Changes in Argyrodite LPSCl Solid‐State Electrolyte Critically Affect Electrochemical Stability
Abstract
<jats:title>Abstract</jats:title><jats:p>Microstructure of argyrodite solid‐state electrolyte (SSE) critically affects lithium metal electrodeposition/dissolution. While the stability of unmodified SSE is mediocre, once optimized state‐of‐the‐art electrochemical performance is achieved (symmetric cells, full cells with NMC811) without secondary interlayers or functionalized current collectors. Planetary mechanical milling in wet media (m‐xylene) is employed to alter commercial Li<jats:sub>6</jats:sub>PS<jats:sub>5</jats:sub>Cl (LPSCl) powder. Quantitative stereology demonstrates how milling progressively refines grain and pore size/distribution in the SSE compact, increases its density, and geometrically smoothens the SSE‐Li interface. Mechanical indentation demonstrates that these changes lead to reduced site‐to‐site variation in the compact's hardness. Milled microstructures promote uniform early‐stage electrodeposition on foil collectors and stabilize solid electrolyte interphase (SEI) reactivity. Analysis of half‐cells with bilayer electrolytes demonstrates the importance of microstructure directly contacting current collector, with interface roughness due to pore and grain size distribution being key. For the first time, short‐circuiting Li metal dendrite is directly identified, employing 1.5 mm diameter “mini” symmetrical cell and cryogenic focused ion beam (cryo‐FIB) electron microscopy. The branching sheet‐like dendrite traverses intergranularly, filling the interparticle voids and forming an SEI around it. Mesoscale modeling reveals the relationship between Li‐SSE interface morphology and the onset of electrochemical instability, based on underlying reaction current distribution.</jats:p>