Overcoming chemical incompatibility: Co-Firing of high-energy all ceramic cathodes for garnet-based solid-state batteries
Kun Joong Kim a, Steffen Weinmann a, Jennifer Rupp a b, Lucie Quincke a, Samuel Merk b
a Department of Chemistry, Technical University of Munich, Chair of Solid-State Electrolyte Chemistry, Germany
b TUMint. Energy Research GmbH, Lichtenbergstr. 4, Garching 85747, Germany
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
Advances in Li-Metal All-Solid-State Batteries: Processing, Manufacturing, and Integration - #AdvanceSSB
Sevilla, Spain, 2025 March 3rd - 7th
Organizer: Juan Carlos Gonzalez-Rosillo
Invited Speaker, Kun Joong Kim, presentation 070
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.070
Publication date: 16th December 2024

High-temperature sintering of composite cathodes triggers lithium loss and secondary phase formation, one of the major challenges in oxide-based solid-state batteries. However, the interdiffusion during sintering in the different partial pressures of lithium and oxygen remains poorly understood. Here, we study the reaction mechanism for the formation of impurity phases during the co-firing of Li-garnet (Li7La3Zr2O12) and LiCoO2 at high temperature and propose an alternative processing strategy that enables the production of impurity-free all-oxide composite cathodes. By using Li-rich atmospheres, the secondary phase of LaCoO3 is avoided and the composite cathodes exhibit >95% relative density. The electrical resistance of the composite cathode is increased by 3-4 orders of magnitude. Electronic conductivity of over 1 mS cm-1 is achieved at room temperature. An unprecedented areal discharge capacity of 3.48 mAh cm-2 is realised at current densities of 0.25 mA cm-2, demonstrating the high performance of the cathodes. Our results encourage further demonstration of all oxide solid state battery prototypes in combination with thin oxide electrolytes and lithium metal anodes.

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