Supramolecular Perylene Bisimide-Polysulfide Gel Networks as Nanostructured Redox Mediators in Dissolved Polysulfide Lithium–Sulfur Batteries,Chemistry of Materials

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Supramolecular Perylene Bisimide-Polysulfide Gel Networks as Nanostructured Redox Mediators in Dissolved Polysulfide Lithium–Sulfur Batteries
Chemistry of Materials ( IF 7.2 ) Pub Date : 2015-09-29 00:00:00 , DOI: 10.1021/acs.chemmater.5b02955
Peter D. Frischmann ₁ , Laura C. H. Gerber ₁ , Sean E. Doris _{1,

2} , Erica Y. Tsai ₁ , Frank Y. Fan ₃ , Xiaohui Qu ₄ , Anubhav Jain ₄ , Kristin A. Persson ₄ , Yet-Ming Chiang ₃ , Brett A. Helms ₁

Affiliation

Here we report a new redox-active perylene bisimide (PBI)-polysulfide (PS) gel that overcomes electronic charge-transport bottlenecks common to lithium–sulfur (Li–S) hybrid redox flow batteries designed for long-duration grid-scale energy storage applications. PBI was identified as a supramolecular redox mediator for soluble lithium polysulfides from a library of 85 polycyclic aromatic hydrocarbons by using a high-throughput computational platform; furthermore, these theoretical predictions were validated electrochemically. Challenging conventional wisdom, we found that π-stacked PBI assemblies were stable even in their reduced state through secondary interactions between PBI nanofibers and Li₂S_n, which resulted in a redox-active, flowable 3-D gel network. The influence of supramolecular charge-transporting PBI-PS gel networks on Li–S battery performance was investigated in depth and revealed enhanced sulfur utilization and rate performance (C/4 and C/8) at a sulfur loading of 4 mg cm^–2 and energy density of 44 Wh L^–1 in the absence of conductive carbon additives.

中文翻译：

超分子Per双酰亚胺-聚硫化物凝胶网络作为溶解多硫化锂-硫电池中的纳米结构氧化还原介体

在这里，我们报告了一种新型的氧化还原活性per双酰亚胺（PBI）-聚硫化物（PS）凝胶，该凝胶克服了锂-硫（Li-S）混合氧化还原液流电池常见的电子电荷传输瓶颈，该电池设计用于长时间电网规模的储能应用程序。通过使用高通量计算平台，从85种多环芳香烃的文库中，PBI被确定为可溶性多硫化锂的超分子氧化还原介体；此外，这些理论预测得到了电化学验证。挑战传统观点，我们发现，π堆积的PBI组装件即使通过PBI纳米纤维与Li ₂ S _n之间的二次相互作用，即使在还原状态下也能保持稳定。，从而形成了具有氧化还原活性的可流动3-D凝胶网络。李-S的电池性能的超分子电荷输送PBI-PS凝胶网络的影响在深度进行了研究，以4mg cm的硫负载透露增强硫利用率和速率性能（C / 4和C / 8）^-2和在没有导电碳添加剂的情况下，能量密度为44 Wh L ^–1。

更新日期：2015-09-29

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