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001019580 0247_ $$2datacite_doi$$a10.34734/FZJ-2023-05515
001019580 037__ $$aFZJ-2023-05515
001019580 1001_ $$0P:(DE-Juel1)180575$$aYang, Aikai$$b0$$eCorresponding author$$ufzj
001019580 245__ $$aNa5YSi4O12-type Na+ superionic conductors for solid-state batteries$$f - 2023-09-22
001019580 260__ $$aJülich$$bForschungszentrum Jülich GmbH Zentralbibliothek, Verlag$$c2023
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001019580 4900_ $$aSchriften des Forschungszentrums Jülich Reihe Energie & Umwelt / Energy & Environment$$v618
001019580 502__ $$aDissertation, RWTH Aachen University, 2023$$bDissertation$$cRWTH Aachen University$$d2023$$o2023-09-22
001019580 520__ $$aThe development of high-performance solid-state batteries (SSBs) has gained increasing attention in recent years as a promising alternative to conventional liquid electrolyte batteries. In this context, the Na5YSi4O12- type (NYS) Na+ superionic conductors have emerged as potential electrolyte candidates due to their high Na+ ionic conductivity and stability in solid-state Na batteries (SSSBs). This thesis investigates the synthesis, characterization, and electrochemical properties of NYS-type Na+ superionic conductors, focusing on their applicability in large-scale fabrication as well as in SSBs and the development of novel compositions with higher ionic conductivity. The background of the work is introduced in the first two chapters, followed by an explanation of the preparation and characterization methods applied. The results and discussion are divided into three main parts: First, tape-casting of thin NYS sheets using aqueous slurries has been developed. The microstructure, crystal structure, electrochemical performance and mechanical properties of the as-prepared NYS tapes have been investigated. After sintering, the obtained NYS tapes had high crystalline purity, dense microstructure (relative density > 90%), and favorable mechanical properties (hardness H of 2 GPa andYoung’s modulus E of 45 GPa). The NYS tapes showed a total ionic conductivity of 1.0 mS cm‒1 at room temperature (RT), a low total activation energy of 0.30 eV, and a wide electrochemical stability window of  over 8 V. The critical current density (CCD) of NYS tape against Na metal electrodes reached 2.2 mA cm‒ 2 and the galvanostatic cycling time was over 280 h at 0.8 mA cm‒2 and 0.8 mAh cm‒2. This work not only highlights the potential of the scarcely studied silicate-based NYS ionic conductor as a functional separator but also presents a cost-efficient and eco-friendly continuous fabrication using the aqueous tape casting technique, thus is expected to boost the practical application of NYS as a solid-state electrolyte (SSE) in SSSBs.
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