Exploration and Optimization of Thiol-containing Conductive Polymer and Covalent Organic Frameworks as Cathode Materials in Lithium-Sulfur Batteries: Synthesis, Operando Analysis, and Simulation

含硫醇导电聚合物和共价有机骨架作为锂硫电池正极材料的探索和优化：合成、操作分析和模拟

• 批准号: 441211139
• 负责人: Professor Dr. Joachim Dzubiella
• 金额: --
• 依托单位: Institut für Chemie
• 依托单位国家: 德国
• 项目类别: Priority Programmes
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/441211139?language=en
• 关键词: Exploration; Optimization; Thiol; containing; Conductive

Lithium-sulfur (Li-S) batteries hold promise for future energy storage, with polymers like poly(4-(thiophene-3-yl) benzenethiol) (PTBT) playing key roles. However, achieving high sulfur loading and maintaining optimal conductivity present challenges. Covalent organic frameworks (COFs) provide potential solutions, offering porous structures for sulfur storage and transport. Despite promising initial studies, fundamental issues such as electrochemical interactions between sulfur and COFs and the impact of pore structures on sulfur loading remain unexplored. In addition to the scientific challenges, practical aspects such as scalability, compatibility with industrial processes, and degradation mechanisms during transition to industrially relevant cell formats need addressing. Advanced characterization technologies and operando methods offer deeper understanding of electrochemical mechanisms in electrode materials, though COFs have had limited exposure to multi-method modeling studies. The proposed research combines experimental and theoretical investigations to optimize PTBT and thiol-functionalized COFs (SH-COFs) as cathode materials, aiming to enhance the efficiency, stability, and energy density of Li-S batteries. The work program includes experimental investigations, comprehensive operando analysis, and mechanistic studies using simulations and theoretical calculations. The program involves optimizing the up-scale synthesis of PTBT-based sulfur cathodes for pouch cell application, creating SH-COFs with controllable pore size and -SH groups, performing multimodal operando analysis of Li-S cells (both coin cells and pouch cells), and attaining a theoretical understanding of thiol-containing COF-based sulfur hosts. Techniques like X-ray imaging will track active material distributions, while spectroscopic methods will study the release of polysulfide species into the electrolyte during cell cycling. A mechanistic study of thiol-containing COFs, based on multiscale simulations and theoretical modeling, will provide a microscopic understanding of these materials. Molecular structure, dynamics, and the impact of varied solvent compositions and pore sizes will be investigated.

锂硫（Li-S）电池有望成为未来的能源存储，其中聚（4-（噻吩-3-基）苯乙撑）（PTBT）等聚合物发挥着关键作用。然而，实现高硫负载和保持最佳电导率存在挑战。共价有机框架（COF）提供了潜在的解决方案，为硫的储存和运输提供了多孔结构。尽管有希望的初步研究，基本问题，如硫和COFs之间的电化学相互作用和孔结构对硫负载的影响仍然没有探索。除了科学上的挑战，实际方面，如可扩展性，与工业过程的兼容性，以及在过渡到工业相关的细胞格式的降解机制需要解决。先进的表征技术和操作方法提供了更深入的了解电极材料的电化学机制，虽然COFs有有限的曝光多方法建模研究。该研究将实验和理论研究相结合，以优化PTBT和硫醇官能化COFs（SH-COFs）作为阴极材料，旨在提高Li-S电池的效率，稳定性和能量密度。工作计划包括实验研究，全面的operando分析，以及使用模拟和理论计算的机理研究。该计划涉及优化用于袋式电池应用的PTBT基硫阴极的大规模合成，创建具有可控孔径和-SH基团的SH-COF，对Li-S电池（硬币电池和袋式电池）进行多模式操作分析，并获得对含硫醇的COF基硫主体的理论理解。X射线成像等技术将跟踪活性材料的分布，而光谱方法将研究电池循环过程中多硫化物物质向电解质中的释放。基于多尺度模拟和理论建模的含巯基COFs的机理研究将提供对这些材料的微观理解。分子结构，动力学，以及不同的溶剂组合物和孔径的影响将进行研究。