Development of high-voltage bipolar redox-active organic molecules through the electronic coupling of catholyte and anolyte structures

Tracy, Jacob S.; Horst, Elena S.; Roytman, Vladislav A.; Toste, F. Dean

doi:10.1039/D2SC03450F

Title: Development of high-voltage bipolar redox-active organic molecules through the electronic coupling of catholyte and anolyte structures

Journal Article · Wed Sep 21 00:00:00 EDT 2022 · Chemical Science

DOI:https://doi.org/10.1039/D2SC03450F· OSTI ID:1885199

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Chemical Science Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, CA 94720-1460, USA, Department of Chemistry, University of California, Berkeley, CA 94720-1460, USA, Joint Center for Energy Storage Research (JCESR), 9700 South Cass Avenue, Argonne, Illinois, 60439, USA
Department of Chemistry, University of California, Berkeley, CA 94720-1460, USA, Joint Center for Energy Storage Research (JCESR), 9700 South Cass Avenue, Argonne, Illinois, 60439, USA
Department of Chemistry, University of California, Berkeley, CA 94720-1460, USA

All-organic non-aqueous redox flow batteries (O-NRFBs) are a promising technology for grid-scale energy storage. However, most examples of high-voltage (>2 V) O-NRFBs rely upon the use of distinct anolytes and catholytes separated by a membrane or porous separator which can result in crossover of redox active material from one side of the battery to the other. The resulting electrolyte mixing leads to irreversible reductions in energy density and capacity. A potentially attractive solution to overcome this crossover issue is the implementation of symmetric flow batteries where a single bipolar molecule functions as both an anolyte and a catholyte. Herein, we report the development of a new class of bipolar redox active materials for use in such symmetric flow batteries through the electronic coupling of phenothiazine catholytes and phthalimide anolytes. Such a strategy results in hybrid molecules possessing higher cell voltages than what could be obtained together by their uncoupled building blocks. Performance in flow batteries is demonstrated for two members of this new class of molecules, with the highest performing candidate featuring a ΔE of 2.31 V and demonstrating 93.6% average coulombic efficiency, 86.8% energy efficiency, and 68.6% capacity retention over the course of 275 charge–discharge cycles and 5 cell polarity reversals. Finally, the superior performance of symmetric O-NRFBs is experimentally confirmed by comparing these results to an asymmetric flow battery constructed with a distinct phenothiazine catholyte and a distinct phthalimide anolyte on opposing sides of the cell.

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

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1885199

Alternate ID(s):: OSTI ID: 1902925

Journal Information:: Chemical Science, Journal Name: Chemical Science Vol. 13 Journal Issue: 36; ISSN 2041-6520

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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