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

Frischmann, Peter D.; Gerber, Laura C.  H.; Doris, Sean E.; Tsai, Erica Y.; Fan, Frank Y.; Qu, Xiaohui; Jain, Anubhav; Persson, Kristin A.; Chiang, Yet-Ming; Helms, Brett A.

doi:10.1021/acs.chemmater.5b02955

Title: Supramolecular Perylene Bisimide-Polysulfide Gel Networks as Nanostructured Redox Mediators in Dissolved Polysulfide Lithium–Sulfur Batteries

Journal Article · Tue Sep 15 00:00:00 EDT 2015 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.5b02955· OSTI ID:1513783

Frischmann, Peter D. ^[1]; Gerber, Laura C. H. ^[1]; Doris, Sean E. ^[2]; Tsai, Erica Y. ^[1]; Fan, Frank Y. ^[3]; Qu, Xiaohui ^[1]; Jain, Anubhav ^[1]; Persson, Kristin A. ^[1]; Chiang, Yet-Ming ^[3]; Helms, Brett A. ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1513783

Journal Information:: Chemistry of Materials, Vol. 27, Issue 19; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 64 works

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