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

金属硫可充电电池是一种潜在的经济有效的解决方案，可以替代用于电动交通的锂离子电池。锂硫和镁硫电池的能量密度可以超过锂离子，但只能在低电解液与硫的比例下。然而，在液体电解液水平较低的情况下，很难设计出高性能的硫电池。此外，首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。研究了硫共聚物阴极的化学和形态对离子迁移、硫形态和反应速率的影响。还将探索使用固体共聚中间层来防止硫物种溶解到本体聚合物电解质中。这项研究将邀请路易斯安那州泽维尔大学的圣母大学研究生和本科生以及来访的本科生参与，以促进电化学工程领域研究人员的培训和留住。此外，通过课外浓缩计划的发展，下一代化学科学和工程研究人员的数量、多样性和培训将得到加强。这项基础工程科学研究将对理解局部环境对硫磺和多硫化物在固体中的电化学性质的影响做出贡献，从而具有变革性。元素硫和有机单体的共聚将被用来方便地调节硫的阴极环境，包括富硫和富离子区域的大小和形态，离子溶剂组分与多硫化物S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，还将研究在固体中用于活性阳离子传输和多硫化物抑制的共聚物界面层。将探索离子在阴极和层间纳米结构固态环境中的传输。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。

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.