Collaborative Research: Unraveling the role of chemo-mechanics in all solid state batteries

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Transportation accounts for 28% of energy-related greenhouse gas emissions in the United States. Currently, only 1% of the transportation sector employs electricity. Advanced energy storage systems are necessary for rapid adoption of electric vehicles. Energy dense batteries are paramount for decarbonization of transportation and grid applications. Replacing traditional graphite anode materials with lithium metal may provide a pathway for increasing the energy density of a lithium-ion battery. However, lithium metal batteries suffer from consumptive side effects which limits its cycle lifetime and charge time. Recently, there has been renewed interest in using a solid electrolyte with lithium metal anodes. A solid electrolyte can act as a barrier for unwanted physical and chemical decomposition that leads to unstable electrodeposition (e.g. dendrite and filament growth). This proposal intends to explore the role chemo-mechanics has on electrodeposition stability in all solid-state batteries. This project aims to engage high school, undergraduates, and graduate students in a diverse array of research and educational opportunities. Educational outreach through a range of organizations will aim to disseminate the research findings to the greater Princeton, Philadelphia, and West Lafayette communities.The fundamental nature of this research seeks to uncover the nature of lithium electrode kinetics at solid-solid interfaces for next generation energy dense solid-state batteries. Interface kinetics are well understood at soft interfaces (solid-gas and solid-liquid) common in many electrochemical energy conversion and storage applications. These interfaces are readily accessible with a range of different electroanalytical and materials characterization probes. Less is known regarding electrode kinetics at solid-solid interfaces where fundamental charge-transfer mechanisms can be affected by chemo-mechanical processes. This project aims to understand the nature of charge-transfer reactions at buried solid-solid interfaces via combining advanced in situ synchrotron techniques, electrochemistry, and meso-scale modeling. The project will explore lithium metal/garnet-type Li7La3Zr2O12 (LLZO) solid ion conductor electrolyte configurations. Synchrontron characterization data will be made available via the open source NanoHub platform hosted by Purdue University. Advanced understanding of lithium electrode kinetics will aid in device and materials design strategies for safe, energy-dense, and long lasting energy storage systems.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.