ERI: Interphase Evolution and Electrochemical Behavior for Highly Reversible Zinc Metal Anodes

尽管锂离子电池已广泛用于从电动车辆到可再生电力的电网存储的广泛应用，但锂和过渡金属（例如钴）资源的高成本和有限的国内供应使得有必要开发水性可再充电锌金属电池作为"超越锂"的补充技术。然而，在锌金属阳极和电解质之间的区域上发生不希望的反应，这损害了水性锌电池的寿命和耐久性。为了提高电池寿命，在设计阶段之前，重要的是要了解阳极和电极之间的面积、相间区域和锌金属阳极的电化学性能之间的关系。在这个工程研究启动（ERI）项目中，PI和他的研究小组将研究这种中间相的演变及其对电池运行期间锌阳极性能的影响。该项目将提供关键的科学知识，以开发先进的水性电池，以保持和推进美国电池技术的领先地位。多学科的研究项目将提供充分的教育和推广机会，高中，本科，硕士。和博士这个ERI研究项目旨在推进由SEI缺陷和电子可接近厚度驱动的水性固体电解质界面（SEI）演变的基础知识。基于含吡唑的水性电解质的实验和建模方法的紧密结合将用于研究影响SEI形成的关键因素，并确认SEI的缺陷和厚度的影响。该研究项目的其他独特元素包括1）使用表面表征来识别锌阳极SEI的形态和化学组成作为水溶液pH值、温度和电池循环时间的函数，2）除了SEI形态和化学信息之外，还使用电化学阻抗谱和密度泛函理论（DFT）计算来确定通过SEI的Zn2+阳离子传输的机制，3）使用扫描电子显微镜、纳米压痕和耦合的电化学-机械多物理场建模框架来识别锌金属枝晶形成/生长和SEI的机械降解对循环历史的依赖性，以及4）使用DFT计算结合在前三个任务中获得的SEI的电化学-机械信息来识别水性SEI形成/演化的有利反应途径。通过该项目，PI将促进新的研究伙伴关系（包括与内部和外部合作者），并扩展研究小组在理论建模和高级表征方面的能力。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。

Although lithium-ion batteries have been widely used for a wide range of applications ranging from electric vehicles to grid storage of renewable electricity, the high cost and limited domestic supply of lithium and transition metal (e.g. cobalt) resources necessitate the development of aqueous rechargeable zinc metal batteries as a “beyond-lithium” complementary technology. However, unwanted reactions occur on the region between zinc metal anode and electrolytes, which compromises the lifetime and durability of aqueous zinc batteries. To improve the cell lifetime, it is important to understand the relationship between the area between the anode and the electrode, the interphase region, and the electrochemical performance of zinc metal anode prior to the design stages. In this Engineering Research Initiation (ERI) project, the PI and his research group will study the evolution of this interphase and its effect on the zinc anode performance during cell operation. The project will provide critical scientific knowledge to develop advanced aqueous batteries for maintaining and advancing US battery technology leadership. The multidisciplinary research project will provide ample educational and outreach opportunities for high school, undergraduate, M.S. and Ph.D. students, including those from underrepresented groups in STEM.This ERI research project seeks to advance fundamental knowledge of the aqueous solid electrolyte interphase (SEI) evolution driven by SEI defects and an electron approachable thickness. A close integration of experimental and modeling approaches based on pyrazole-based containing aqueous electrolytes will be used to study key factors that impact SEI formation and to confirm the effect of the SEI’s defects and thickness. Other unique elements of the research project include 1) identifying the morphology and chemical compositions of zinc anode SEI as a function of aqueous pH value, temperature and cell cycling time using surface characterizations, 2) determining the mechanism of Zn2+ cation transport through the SEI using electrochemical impedance spectroscopy and density functional theory (DFT) calculations in addition to SEI morphology and chemical information, 3) identifying the dependence of zinc metallic dendrite formation/growth and mechanical degradation of the SEI on the cycling history using scanning electron microscopy, nanoindentation and a coupled electrochemical-mechanical multiphysics modeling framework, and 4) identifying the favorable reaction pathways of aqueous SEI formation/evolution using DFT calculations combined with the electro−chemo−mechanical information of the SEI obtained in the first three tasks. Through this project, the PI will catalyze new research partnerships (both with internal and external collaborators) and extend the research group’s capabilities in both theoretical modeling and advanced characterization.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.