Engineering All-Solid Metal-Sulfur Batteries: Transport, Speciation, and Kinetics in Sulfur Copolymer Composite Cathodes

金属硫可充电电池是替代用于电动运输的锂离子电池的潜在成本效益解决方案。锂硫电池和镁硫电池的能量密度可以超过锂离子电池，但仅在低电解质与硫的比率下。然而，很难用低水平的液体电解质来设计高性能的硫电池。此外，优选消除挥发性电池组件以提高安全性。在这个项目中，研究人员将研究基于共聚硫阴极的固态金属硫电池。将研究硫共聚物阴极的化学和形态对离子传输、硫形态和反应速率的影响。还将探索使用固体共聚物夹层来防止硫物质溶解到本体聚合物电解质中。这项研究将从事研究生和本科圣母院的学生和访问本科生从路易斯安那州泽维尔大学，以促进培训和保留研究人员在电化学工程领域。此外，化学科学和工程的下一代研究人员的数量，多样性和培训将通过课后丰富编程的发展得到加强。这一基础工程科学研究将是变革性的，因为它有助于理解当地环境对固态硫和聚（硫化物）电化学性能的影响。元素硫和有机单体的共聚将被利用来容易地调节硫阴极环境，包括富硫和富离子域的尺寸和形态、离子溶剂化组分与聚（硫化物）的相互作用以及电荷转移动力学。光谱电化学技术将用于研究硫/（多）硫化物的形态和反应途径。另外，将研究用于活性阳离子传输和固态多硫化物排斥的共聚物夹层。该奖项反映了NSF的法定使命，并已被认为是值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估的支持。

Metal-sulfur rechargeable batteries are a potentially cost-effective solution for replacement of Li-ion batteries for use in electric transportation. The energy density of lithium-sulfur and magnesium-sulfur batteries can exceed that of Li-ion, but only at low electrolyte-to-sulfur ratios. However, it is difficult to engineer sulfur batteries for high performance with low levels of liquid electrolyte. In addition, elimination of volatile battery components to improve safety is preferred. In this project, the investigator will investigate solid-state metal-sulfur batteries based on copolymerized sulfur cathodes. The influence of the chemistry and morphology of the sulfur copolymer cathode on the ion transport, sulfur speciation, and reaction rates will be investigated. The use of a solid copolymer interlayer to prevent the dissolution of sulfur species into the bulk polymer electrolyte will also be explored. This research will engage graduate and undergraduate Notre Dame students and visiting undergraduates from the Xavier University of Louisiana to promote the training and retention of researchers in the field of electrochemical engineering. Additionally, the number, diversity, and training of the next generation of researchers in the chemical sciences and engineering will be enhanced by development of afterschool enrichment programming.This fundamental engineering science research will be transformative for its contributions to the understanding of the effects of local environment on sulfur and poly(sulfide) electrochemical properties in the solid-state. Copolymerization of elemental sulfur and organic monomers will be leveraged to facilely tune the sulfur cathode environment, including the size and morphology of sulfur-rich and ion-rich domains, the interactions of ion-solvating components with poly(sulfide)s, and charge-transfer kinetics. Spectroelectrochemical techniques will be used to investigate sulfur/(poly)sulfide speciation and reaction pathways. Separately, copolymer interlayers for active cation transport and polysulfide rejection in the solid-state will be investigated. Ion transport in both the cathode and interlayer nanostructured solid-state environments will be probed.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.