GOALI: Engineering Mechanically Stable Interfaces Through Short-Range Molecular Rearrangement Driven by Inhomogeneous Li Ion Transfer Kinetics

这个基础研究项目旨在填补下一代高能量密度固态电池工程所需的关键知识空白。具体来说，该项目将研究原子、离子、分子的化学、组成和物理排列，以及原子结构和界面形态中的缺陷如何共同控制局部压力的发展，从而导致电池的灾难性故障，如破裂或短路。这一新知识将直接为设计消费电子产品和电动汽车最安全、性能最高的电池提供有力的策略。跨学科和综合的研究方法将培养和教育学生最先进的实验力学，分析建模，电化学和材料加工。此外，这些工具和技术将从学术界、工业界和美国国家实验室的独特视角进行教授。通过这种方式，学生们将为世界一流的材料科学和工程人才做好准备，加速先进材料的发现、开发和部署。本提案的研究目标是进行有针对性的纳米压痕研究，旨在填补关键知识空白，直接为优化固态电解质的化学、成分和加工策略提供信息，以稳定关键界面并最大化设备性能。这些结果将通过工程固态电解质来实现，以提供应力定向，短程分子重排，减轻由不均匀锂离子转移动力学引起的有害应变和相应的应力。此外，这种能力将被设计成在广泛的电池相关操作条件下尽可能高效地运行。对应力松弛机制中实验观察到的转变进行统计分析，将能够构建以关键操作变量、电化学循环和温度为函数表示的新型小尺度变形机制图。这些独特的地图将提供急需的洞察界面缺陷的物理尺寸，这些缺陷能够通过固态电解质的断裂产生灾难性的设备故障。通过这种方式，这些地图将直接为工程稳定界面提供策略和指导方针，这些界面能够支持无应力、平面沉积纯金属锂阳极。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。

This fundamental research project aims to fill critical knowledge gaps required to enable the engineering of next generation high energy density solid state batteries. Specifically, the project will address how the chemistry, composition and physical arrangement of atoms, ions, molecules, and defects in both the atomic structure and interface morphologies collectively control the development of localized pressure known to causes catastrophic failure such as cracking or short circuiting in a battery. This new knowledge will directly inform robust strategies to engineer the safest and highest performance batteries for consumer electronics and electric vehicles. The interdisciplinary and integrative research approach will train and educate students in state-of-art experimental mechanics, analytical modelling, electrochemistry and materials processing. Moreover, these tools and techniques will be taught from unique perspectives in academia, industry and a US national lab. In this way, the students will be well equipped to contribute to a world-class materials science and engineering workforce prepared to accelerate the discovery, development, and deployment of advanced materials. The research goal of this proposal is to perform targeted nanoindentation studies designed to fill critical knowledge gaps that will directly inform strategies to optimize the chemistry, composition and processing of solid-state electrolytes designed to stabilize critical interfaces and maximize device performance. These outcomes will be achieved by engineering solid-state electrolytes to provide stress directed, short range molecular rearrangement that mitigates the deleterious strains and commensurate stresses caused by inhomogeneous lithium-ion transfer kinetics. Moreover, this capability will be engineered to operate as efficiently as possible over a wide range of battery relevant operating conditions. Statistical analysis of experimentally observed transitions in stress relaxation mechanisms will enable the construction of novel small-scale deformation mechanism maps expressed as a function of key operational variables, electrochemical cycling, and temperature. These unique maps will provide much needed insight into the physical dimensions of interface defects capable of producing catastrophic device failure by fracture of the solid-state electrolyte. In this way, the maps will directly inform strategies and guidelines for engineering stable interfaces capable of supporting stress-free, planar deposition of a pure, metallic lithium anode.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.