Collaborative Research: CDS&E: Computational Exploration of Electrically Conductive Metal-Organic Frameworks as Cathode Materials in Lithium-Sulfur Batteries

锂硫电池（LSBs）由锂金属阳极和地球上丰富的硫阴极组成，作为一种很有前途的储能材料而备受关注。迄今为止，一些挑战和技术障碍阻碍了lsdb的发展。在这个合作项目中，Farnaz Shakib教授（新泽西理工学院）和Mohammad Momeni教授（密苏里大学堪萨斯城分校）将研究导电金属有机框架（EC-MOFs）作为lsb正极材料的设计和应用。ec - mof是一种新型的纳米多孔材料，具有极高的表面积和分层结构，可以承受电池运行过程中的机械变形。该项目将通过采用新颖的计算技术来设计和研究一种新型材料作为阴极的功能，从而推动科学的发展。这将导致设计出更高效的清洁能源。在这个项目中，研究生将被训练成未来STEM的熟练劳动力。本科和K-12水平的学生将通过全天研讨会和暑期学校学习计算化学的基础知识，这将有助于他们在STEM领域的成长。尽管对锂硫电池（LSBs）进行了深入的研究，但寻找一种具有高导电性的多孔阴极材料，以防止硫在阳极上来回穿梭，仍然是一个紧迫的挑战。该项目将研究Pi（Pi）的独特结构和电子特性——层状二维导电金属有机框架（EC-MOFs）作为lsb的最佳正极材料。除了电导率的明显优势外，ec - mof的分层结构可以承受极端变形而不会发生机械坍塌。同时，它们的多孔特性允许在阴极中有效地封装活性硫材料，从而增强其溶解到电解质溶液中的阻力（穿梭效应）。该项目的主要目标是探索ec - mof几乎无限的化学空间，以引入理想的候选阴极材料。由于对成千上万的ec - mof作为潜在阴极材料进行逐个分析是不切实际的，因此本研究遵循两个主要目标：(i)使用自动晶体结构创建工具创建一个全面且可扩展的ec - mof数据库，随后将进行高通量筛选，发现具有所需结构和电学性能的ec - mof；（ii）通过高级分子动力学模拟研究硫（S8）及其锂-多硫化物衍生物在电极-电解质界面的封装和可能的运输。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。

Lithium-sulfur batteries (LSBs) consisting of a lithium metal anode and an earth-abundant sulfur cathode have attracted much attention as a promising candidate for energy storage. To date, several challenges and technical hurdles prevent the development of LSBs. In this collaborative project, Professors Farnaz Shakib (New Jersey Institute of Technology) and Mohammad Momeni (University of Missouri–Kansas City) will investigate the design and application of electrically-conductive metal-organic frameworks (EC-MOFs) as cathode materials for LSBs. EC-MOFs are a new class of nanoporous materials with exceptionally high surface area and layered structures that can tolerate mechanical deformations during battery operation. This project will advance science by employing novel computational techniques to design and investigate the functionality of a new class of materials as cathodes. This will lead to the design of more efficient clean energy resources. During this project, graduate students will be trained as the skilled workforce for the future of STEM. Undergraduate and K-12 level students will learn the fundamentals of computational chemistry through full-day workshops and Summer Schools, which will help their growth in STEM fields.Despite intensive research on lithium-sulfur batteries (LSBs), finding a porous cathode material with a high electrical conductivity that can prevent sulfur shuttling to the anode is still a pressing challenge. The project will address the unique structural and electronic properties of Pi(𝜋)-stacked layered 2D electrically conductive metal-organic frameworks (EC-MOFs) as optimal cathode materials in LSBs. Apart from the apparent advantage of electrical conductivity, the layered architecture of EC-MOFs can endure extreme deformations without mechanical collapse. At the same time, their porous nature allows for efficient encapsulation of the active sulfur material in the cathode providing enhanced resistance toward its dissolution into the electrolyte solution (the shuttling effect). The primary goal of this project is to probe the virtually unlimited chemical space of EC-MOFs to introduce ideal candidates as cathode materials. Since a case-by-case analysis of thousands of EC-MOFs as potential cathode materials is impractical, this research follows two main objectives: (i) creating a comprehensive and expandable database of EC-MOFs with an automated crystal structure creation tool which will be followed by high-throughput screening discovery of EC-MOFs with desired structural and electrical properties; and (ii) investigating sulfur (S8) and its lithium-polysulfide derivatives’ encapsulation and possible transport at the electrode-electrolyte interface from advancedmolecular dynamics simulations.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.