A Guideline to Mitigate Interfacial Degradation Processes in Solid‐State Batteries Caused by Cross Diffusion
[1]
- Department of Material Science and Engineering NTNU Norwegian University of Science and Technology Trondheim 7034 Norway, Christian Doppler Laboratory for Solid‐State Batteries NTNU Norwegian University of Science and Technology Trondheim 7034 Norway, Institute of Chemistry and Technology of Materials Graz University of Technology Graz 8010 Austria
- Institute of Chemistry and Technology of Materials Graz University of Technology Graz 8010 Austria
- Institute of Chemical Technologies and Analytics TU Wien Wien 1060 Austria
- Institute of Electron Microscopy and Nanoanalysis and Graz Centre for Electron Microscopy Graz University of Technology Graz 8010 Austria, Leibniz‐Institut für Kristallzüchtung 12489 Berlin Germany
- Department of Material Science and Engineering NTNU Norwegian University of Science and Technology Trondheim 7034 Norway
- Institute of Electron Microscopy and Nanoanalysis and Graz Centre for Electron Microscopy Graz University of Technology Graz 8010 Austria
- Departamento de Física de la Materia Condensada Facultad de Ciencias Universidad Autónoma de Madrid Madrid E‐28049 Spain, Condensed Matter Physics Center (IFIMAC) Universidad Autónoma de Madrid Madrid E‐28049 Spain
- Department of Geoscience and Petroleum Norwegian University of Science and Technology Trondheim 7031 Norway
- Fundamental Aspects Mat and Energy Group Delft University of Technology Mekelweg 15 Delft 2629 JB the Netherlands
- Mechanical Engineering Department University of Michigan Ann Arbor MI 48109 USA, Walker Department of Mechanical Engineering Texas Materials Institute Oden Institute for Computational Engineering and Sciences, and Joint Center for Energy Storage Research University of Texas at Austin Austin TX 78712‐1591 USA
- Department of Chemistry and Physics of Materials University of Salzburg Salzburg 5020 Austria
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 Li 7 La 3 Zr 2 O 12 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 Co 2+ or Co 3+ 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, D 700 °C = 9.46 × 10 −14 cm 2 s −1 and an activation energy E a = 1.65 eV, suggesting that detrimental cross diffusion will take place at any relevant process condition. Additionally, the optimal protective Al 2 O 3 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.
- Sponsoring Organization:
- USDOE
- OSTI ID:
- 1985533
- Alternate ID(s):
- OSTI ID: 1995297
- Journal Information:
- Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 42 Vol. 33; ISSN 1616-301X
- Publisher:
- Wiley Blackwell (John Wiley & Sons)Copyright Statement
- Country of Publication:
- Germany
- Language:
- English
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