CAS: Probing Nucleation and Growth Dynamics of Lithium Dendrites in Solid Electrolytes

非技术性锂离子电池为我们的日常生活提供动力，从便携式电子产品、电动工具到医疗设备，但由于对其安全性、可靠性和能量密度的担忧，它们在交通电气化和电网存储等更具战略重要性的应用中的应用速度较慢。将不可燃无机固体电解质与高容量锂金属负极相结合制成固态锂金属电池被认为是显著提高现有电池安全性和能量密度的一种有前途的途径。然而，在充电过程中，金属锂树枝状晶往往会在各种固体电解液中形成，导致短路风险，其机制仍然难以捉摸。在这项由美国国家科学基金会材料研究部固态与材料化学项目资助的项目中，韩福东教授和他在伦斯勒理工学院的研究小组将通过探测电池运行过程中树枝晶的形核和生长来研究固体电解液中树枝晶形成的根本原因。该项目不仅为开发先进的固体电解液提供关键的科学知识，以保持和提高美国电池技术的领先地位，而且还支持STEM教育和能源储存领域的劳动力发展。这项研究涉及在国家设施中使用先进的中子散射技术，该技术在电池设计、实时测量和数据分析方面的发展也促进了国家基础设施的发展。技术总结在材料研究部固态和材料化学项目的支持下，这项假设驱动的研究试图探索Li树枝晶在无机固体电解质中的形核和生长动力学。该项目结合了最先进的陶瓷合成技术、OPANDO中子散射测量技术和先进的数据建模和分析技术，旨在揭示固体电解质中形成的树枝晶的形核和生长途径、生长和溶解之间的竞争以及随温度变化的形状演变。这项研究为理解从传统宏观技术观察到的树枝晶是如何在开发抗树枝晶固体电解质的非常早期阶段形成的提供了前所未有的见解。利用原位小角中子散射法探测致密陶瓷中异种物质的形成，为进一步研究微观结构在宏观尺度上发生变化的电化学材料提供了可能。除了推进基础材料化学，多学科研究还为不同水平的学生提供了充足的教育和外展机会，包括那些来自代表不足的群体的学生。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

NON-TECHNICAL SUMMARYLithium-ion batteries power much of our daily lives from portable electronics, power tools, to medical devices, but their adoption in more strategically important applications such as transportation electrification and grid storage is slower due to concerns raised over their safety, reliability, and energy density. Integrating nonflammable inorganic solid electrolytes with high-capacity Li metal anodes to make solid-state lithium metal batteries are considered a promising approach to significantly improve the safety and energy density of existing batteries. However, metallic lithium dendrites tend to form in a variety of solid electrolytes during charging, causing short-circuit risk, by mechanisms that remain elusive. In this project, funded by the Solid State and Materials Chemistry program in the NSF’s Division of Materials Research, Prof. Fudong Han and his research group at Rensselaer Polytechnic Institute will study the underlying causes of dendrite formation in solid electrolytes by probing the nucleation and growth of dendrites during battery operation. The project not only provides critical scientific knowledge to develop advanced solid electrolytes for maintaining and advancing US battery technology leadership, but also supports STEM education and workforce development in the energy storage field. The research involves the utilization of advanced neutron scattering techniques at national facilities, and developments in cell design, real-time measurement, and data analysis for the technique also enhance national infrastructure development. TECHNICAL SUMMARYWith support from the Solid State and Materials Chemistry program of the Division of Materials Research, this hypothesis-driven research seeks to probe nucleation and growth dynamics of Li dendrites in inorganic solid electrolytes. Combining state-of-the-art ceramic synthesis, operando neutron scattering measurement, and advanced data modeling and analysis, this project aims to reveal the nucleation and growth pathways, competitions between growth and dissolution, and temperature-dependent shape evolutions of dendrites formed in solid electrolytes. The research provides unprecedented insights in understanding how the dendrites observed from the conventional macroscopic techniques are formed at the very early stage for development of dendrite-resistant solid electrolytes. The development of in-situ small-angle neutron scattering to probe the formation of alien species in a dense ceramic enables further electrochemical materials research where microstructure variations occur at the macroscopic scale. In addition to advancing the fundamental materials chemistry, the multi-disciplinary research also provides ample educational and outreach opportunities for students at different levels, including those from underrepresented groups.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.