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Addressing the Scalable Manufacturing Considerations of All-Solid-State Batteries

Abstract

All-solid-state batteries (ASSBs) are viewed as promising next-generation energy storage devices due to their enhanced safety, which results from replacing organic liquid electrolytes with non-flammable solid-state electrolytes (SSEs). However, ASSBs are still in the development stage, and further efforts are required before they can be commercialized. While energy density, power density, and cycle life are frequently mentioned challenges for real-world applications, the progress on scalable manufacturing of ASSBs is often overlooked. Recognizing this, the thesis aims to address practical manufacturing considerations for ASSBs, including layer fabrication, material selection, and cell integration.In the field of layer fabrication, most studies have emphasized only electrochemical performance, neglecting the uniformity of the films. The relationship between manufacturing parameters and the physical properties of SSE films was analyzed using machine learning (ML), revealing that both ionic conductivity and film uniformity are crucial for quality evaluation. To underscore the importance of material selection for scalable manufacturing, the stability of sulfide and chloride SSEs in ambient air and dry rooms was assessed, as dry rooms are often utilized in the scalable manufacturing of Li batteries. The degradation mechanisms of different SSEs were investigated, and their recoverability after degradation was evaluated. Lastly, all materials were integrated into all-solid-state pouch cells (ASSPCs) and operated using newly designed isostatic pouch cell holders (IPCHs), which provide cycling pressure with improved uniformity and accuracy compared to conventional uniaxial pouch cell holders (UPCHs). IPCHs significantly increased the utilization and capacity retention of ASSPCs and are lighter than UPCHs. The research potential of IPCHs was demonstrated by establishing an accurate relationship between electrochemical performance and cycling pressure. Collectively, these findings contribute significantly to the advancement and understanding of the complexities involved in the development and scalability of ASSBs.

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