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Phase formation, hydration behavior, and pressure response of sulfide and thiophosphate solid electrolytes
Phase formation, hydration behavior, and pressure response of sulfide and thiophosphate solid electrolytes
Rechargeable lithium ion batteries (LIB) have become an essential part of our daily lives in recent decades, powering mobile phones, laptops, cordless power tools, and even automobiles. While LIB technology currently dominates the battery market for these mobile applications, its physicochemical power and energy density limit will be reached soon. The use of a solid electrolyte instead of a liquid electrolyte in LIBs promises higher energy density, safer operation, and faster charging. Although the benefits of an all-solid-state battery (ASSB) are enormous, certain prerequisites for solid electrolyte application must be met in order for ASSBs to be technologically and commercially competitive. Ionic conductivity is arguably the most important performance indicator of a solid electrolyte. This thesis introduces the concept of LIBs and ASSBs, as well as fundamentals of battery performance and ion conduction in solids, an overview of material classes with a focus on sulfide- and thiophosphate-based solid electrolytes. Furthermore, the techniques used to characterize the solid electrolytes presented in this thesis are introduced. This work presents several design strategies for improving the ionic conductivity of solid electrolytes based on sulfides and thiophosphates. Bottom-up and top-down post-synthetic modification approaches, thermally and chemically induced phase transitions, and microstructure modifications cover a wide range of length scales.
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Schneider, Christian
2023
English
Universitätsbibliothek der Ludwig-Maximilians-Universität München
Schneider, Christian (2023): Phase formation, hydration behavior, and pressure response of sulfide and thiophosphate solid electrolytes. Dissertation, LMU München: Faculty of Chemistry and Pharmacy
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Abstract

Rechargeable lithium ion batteries (LIB) have become an essential part of our daily lives in recent decades, powering mobile phones, laptops, cordless power tools, and even automobiles. While LIB technology currently dominates the battery market for these mobile applications, its physicochemical power and energy density limit will be reached soon. The use of a solid electrolyte instead of a liquid electrolyte in LIBs promises higher energy density, safer operation, and faster charging. Although the benefits of an all-solid-state battery (ASSB) are enormous, certain prerequisites for solid electrolyte application must be met in order for ASSBs to be technologically and commercially competitive. Ionic conductivity is arguably the most important performance indicator of a solid electrolyte. This thesis introduces the concept of LIBs and ASSBs, as well as fundamentals of battery performance and ion conduction in solids, an overview of material classes with a focus on sulfide- and thiophosphate-based solid electrolytes. Furthermore, the techniques used to characterize the solid electrolytes presented in this thesis are introduced. This work presents several design strategies for improving the ionic conductivity of solid electrolytes based on sulfides and thiophosphates. Bottom-up and top-down post-synthetic modification approaches, thermally and chemically induced phase transitions, and microstructure modifications cover a wide range of length scales.