ELECTROLYTE AND INTERFACE DESIGNATION FOR HIGH-PERFORMANCE SOLID-STATE LITHIUM METAL BATTERIES

Abstract

The demand for advanced battery technology is intensifying as electric energy becomes the foundation of modern technologies, such as smart devices, transportation, and artificial intelligence. Batteries play a crucial role in meeting our increasing energy demands and transitioning towards cleaner and more sustainable energy sources. However, range anxiety and safety concerns still hinder the widespread application of battery technology.Current Li-ion batteries, based on graphite anode, have revolutionized battery technology but are nearing the energy density limits. This necessitates the development of metal batteries, employing lithium metal as anode which eliminates host materials that do not contribute to capacity, thereby offering 10 times higher specific capacity. Recent research on lithium metal batteries has seen a significant surge, with growing knowledge transitioning from Li+ intercalation chemistry (graphite) to Li metal plating/stripping. The electrolyte, which was previously regarded as an inert material and acting as a Li+ ion transportation mediator, has gradually attracted researchers’ attention due to its significant impact on the solid electrolyte interphase (SEI) and the Li metal plating/stripping behaviors. Compared to the traditional liquid electrolytes, solid-state lithium metal batteries (SSLMB) have been regarded as the holy grail, the future of electric vehicles (EVs), due to their high safety and potential for higher energy density. However, there are notable knowledge gaps between liquid electrolytes and solid-state electrolytes (SSEs). The transition from liquid-solid contact to solid-solid contact poses new challenges to the SSLMB. As a result, the development of SSLMB is strongly hindered by interface challenges, including not only the Li/SSE interfaces and SSE/cathode interfaces but also SSE/SSE interfaces. In this dissertation, I detailed our efforts to highlight the role of electrolytes and interfaces and establish our understanding and fundamental criteria for them. Building on this understanding, we propose effective and facile engineering solutions that significantly enhance batterie metrics to meet real-world application demand. Rather than simply introducing new compositions or new designations, we are dedicated to introducing our understanding and mechanism behind it, we hope the scientific understanding, the practical solution, and the applicability to various systems can further guide and inspire the electrolyte and interface designation for next-generation battery technology.