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| Book/Dissertation / PhD Thesis | FZJ-2024-01469 |
2024
Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag
Jülich
ISBN: 978-3-95806-737-0
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Please use a persistent id in citations: doi:10.34734/FZJ-2024-01469
Abstract: Ceramic solid-state batteries (SSBs) are attracting significant attention worldwide as an alternative to lithium-ion batteries (LIBs). As the organic electrolyte is replaced by a ceramic electrolyte, unprecedented cell-level safety, a greatly extended operating temperature range and a potentially high energy density are expected. Li-ion conductive oxide ceramics such as the garnet type Li7La3Zr2O12 (LLZO) are promising solid electrolytes for future lithium SSBs because they have sufficient ionic conductivity up to 1 mS cm−1 at room temperature that can be tuned by doping elements, can be processed in air, have a wide electrochemical stability window, and have a high stability to Li metal, enabling the use of Li metal anodes. The garnet material is usually obtained in form of powders. Therefore, a sintering step is required to densify the powder and achieve good contact at the various interfaces, which is critical for adequate electrochemical performance. However, the high sintering temperatures, which can exceed 1000 °C for garnet materials, lead to the interdiffusion of elements at the interface and the formation of undesirable secondary phases. In particular, most common cathode materials such as layered LiCoO2 (LCO) and LiNi1−x−yMnxCoyO2 (NMC) or spinel LiMn2O4 (LMO) are known to react with LLZO at temperatures as low as 400 °C to 600 °C to form resistive secondary phases that drastically degrade battery performance. Material degradation during processing could be avoided by kinetically controlling the sintering process and drastically shortening the sintering times. Apart from numerous undesirable material interactions, protracted sintering at high temperatures is also energy consuming and thus has a negative impact on production costs. New, fast, scalable, and energy-efficient sintering technologies need to be explored to demonstrate viable manufacturing routes for oxide-ceramic batteries. The objective of this work was to investigate the suitability of radiation-based sintering processes for sintering garnet-based battery components. Radiation-based sintering (photonic sintering) such as rapid thermal processing (RTP) and laser sintering are non-contact processes that combine extremely high heating rates with short exposure times to selectively sinter the surface of a sample. The light sources can range from high-power lamps and flash lamps to lasers. Radiation-based sintering and annealing processes are commercialized and well-established for inorganic thin films, but have not been investigated for ceramic garnetbased battery components, yet.
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