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A Guideline to Mitigate Interfacial Degradation Processes in Solid‐State Batteries Caused by Cross Diffusion.

Authors :
Din, Mir Mehraj Ud
Ladenstein, Lukas
Ring, Joseph
Knez, Daniel
Smetaczek, Stefan
Kubicek, Markus
Sadeqi‐Moqadam, Mohsen
Ganschow, Steffen
Salagre, Elena
Michel, Enrique G.
Lode, Stefanie
Kothleitner, Gerald
Dugulan, Iulian
Smith, Jeffrey G.
Limbeck, Andreas
Fleig, Jürgen
Siegel, Donald J.
Redhammer, Günther J.
Rettenwander, Daniel
Source :
Advanced Functional Materials; 10/13/2023, Vol. 33 Issue 42, p1-13, 13p
Publication Year :
2023

Abstract

Diffusion of transition metals across the cathode–electrolyte interface is identified as a key challenge for the practical realization of solid‐state batteries. This is related to the formation of highly resistive interphases impeding the charge transport across the materials. Herein, the hypothesis that formation of interphases is associated with the incorporation of Co into the Li7La3Zr2O12 lattice representing the starting point of a cascade of degradation processes is investigated. It is shown that Co incorporates into the garnet structure preferably four‐fold coordinated as Co2+ or Co3+ depending on oxygen fugacity. The solubility limit of Co is determined to be around 0.16 per formula unit, whereby concentrations beyond this limit causes a cubic‐to‐tetragonal phase transition. Moreover, the temperature‐dependent Co diffusion coefficient is determined, for example, D700 °C = 9.46 × 10−14 cm2 s−1 and an activation energy Ea = 1.65 eV, suggesting that detrimental cross diffusion will take place at any relevant process condition. Additionally, the optimal protective Al2O3 coating thickness for relevant temperatures is studied, which allows to create a process diagram to mitigate any degradation with a minimum compromise on electrochemical performance. This study provides a tool to optimize processing conditions toward developing high energy density solid‐state batteries. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
1616301X
Volume :
33
Issue :
42
Database :
Complementary Index
Journal :
Advanced Functional Materials
Publication Type :
Academic Journal
Accession number :
173013777
Full Text :
https://doi.org/10.1002/adfm.202303680