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关键的知识空白，使下一代高能量密度固态电池的工程。具体而言，该项目将解决原子，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已知导致灾难性故障（如电池中的破裂或短路）的局部压力的发展。这些新知识将直接为强大的战略提供信息，为消费电子产品和电动汽车设计最安全和最高性能的电池。跨学科和综合研究方法将培养和教育学生在国家的最先进的实验力学，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教授。通过这种方式，学生将能够为世界一流的材料科学和工程工作人员做出贡献，以加速先进材料的发现，开发和部署。该提案的研究目标是进行有针对性的纳米压痕研究，旨在填补关键的知识空白，这将直接告知策略，以优化固态电解质的化学，成分和加工，以稳定关键界面并最大限度地提高设备性能。这些结果将通过设计固态电解质来实现，以提供应力导向的短程分子重排，其减轻由不均匀锂离子转移动力学引起的有害应变和相称应力。此外，这种能力将被设计为在广泛的电池相关操作条件下尽可能有效地操作。实验观察到的应力松弛机制的转变的统计分析将使新的小规模变形机制的地图表示为关键操作变量，电化学循环和温度的函数的建设。这些独特的地图将提供非常需要的洞察界面缺陷的物理尺寸能够产生灾难性的设备故障的固态电解质的断裂。通过这种方式，这些地图将直接为能够支持纯金属锂阳极的无应力平面沉积的工程稳定界面的策略和指导方针提供信息。该奖项反映了NSF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.