@article{31820, author = {Peter D Frischmann and Laura C. H Gerber and Sean E Doris and Erica Y Tsai and Frank Y Fan and Xiaohui Qu and Anubhav Jain and Kristin A Persson and Yet-Ming Chiang and Brett A Helms}, title = {Supramolecular Perylene Bisimide-Polysulfide Gel Networks as Nanostructured Redox Mediators in Dissolved Polysulfide Lithium–Sulfur Batteries}, abstract = {

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 Li2Sn, which resulted in a redoxactive, 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.

}, year = {2015}, journal = {Chemistry of Materials}, volume = {27}, pages = {6765 - 6770}, month = {10/2015}, issn = {0897-4756}, doi = {10.1021/acs.chemmater.5b02955}, language = {eng}, }