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

交通运输占美国能源相关温室气体排放量的28%。目前，只有1%的交通运输部门使用电力。先进的储能系统是电动汽车快速普及的必要条件。能量密集电池对于交通运输和电网应用的脱碳至关重要。用锂金属代替传统的石墨负极材料可能为提高锂离子电池的能量密度提供一条途径。然而，锂金属电池的消费副作用限制了其循环寿命和充电时间。最近，人们对使用锂金属阳极的固体电解质重新产生了兴趣。固体电解质可以作为不需要的物理和化学分解的屏障，导致不稳定的电沉积（例如枝晶和长丝生长）。本研究旨在探讨化学力学对所有固态电池电沉积稳定性的影响。该项目旨在为高中生、本科生和研究生提供多样化的研究和教育机会。通过一系列组织开展教育推广活动，旨在将研究成果传播到更大的普林斯顿、费城和西拉斐特社区。这项研究的基本性质是为了揭示下一代能量密集固态电池的固体-固体界面上锂电极动力学的性质。界面动力学在软界面（固体-气体和固体-液体）中被很好地理解，在许多电化学能量转换和存储应用中很常见。这些接口很容易与一系列不同的电分析和材料表征探针访问。对于固体-固体界面的电极动力学知之甚少，其中基本的电荷转移机制可能受到化学-机械过程的影响。该项目旨在通过结合先进的原位同步加速器技术、电化学和中尺度建模，了解埋藏的固体-固体界面上电荷转移反应的本质。本项目将探索锂金属/石榴石型Li7La3Zr2O12 （LLZO）固体离子导体的电解质结构。同步加速器特性数据将通过普渡大学托管的开源NanoHub平台提供。对锂电极动力学的深入了解将有助于安全，能量密集和持久的储能系统的设备和材料设计策略。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

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.