In situ electrochemical recomposition of decomposed redox-active species in aqueous organic flow batteries

Yan Jing; Evan Wenbo Zhao; Marc-Antoni Goulet; Meisam Bahari; Eric M Fell; Shijian Jin; Ali Davoodi; Erlendur Jónsson; Min Wu; Clare P Grey; Roy G Gordon; Michael J Aziz

doi:10.1038/s41557-022-00967-4

In situ electrochemical recomposition of decomposed redox-active species in aqueous organic flow batteries

Nat Chem. 2022 Oct;14(10):1103-1109. doi: 10.1038/s41557-022-00967-4. Epub 2022 Jun 16.

Authors

Yan Jing^#¹, Evan Wenbo Zhao^#^{2

3}, Marc-Antoni Goulet^#^{4

5}, Meisam Bahari⁴, Eric M Fell⁴, Shijian Jin⁴, Ali Davoodi^{4

6

7}, Erlendur Jónsson², Min Wu⁴, Clare P Grey⁸, Roy G Gordon^{9

10}, Michael J Aziz¹¹

Affiliations

¹ Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA.
² Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK.
³ Magnetic Resonance Research Center, Institute for Molecules and Materials, Radboud University Nijmegen, Nijmegen, the Netherlands.
⁴ John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
⁵ Department of Chemical and Materials Engineering, Concordia University, Montreal, Quebec, Canada.
⁶ Materials and Metallurgical Engineering Department, Faculty of Engineering, Ferdowsi University of Mashhad (FUM), Mashhad, Iran.
⁷ Sichuan University-Pittsburgh Institute, Sichuan University, Chengdu, China.
⁸ Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK. cpg27@cam.ac.uk.
⁹ Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA. gordon@chemistry.harvard.edu.
¹⁰ John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA. gordon@chemistry.harvard.edu.
¹¹ John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA. maziz@harvard.edu.

^# Contributed equally.

PMID: 35710986
DOI: 10.1038/s41557-022-00967-4

Abstract

Aqueous organic redox flow batteries offer a safe and potentially inexpensive solution to the problem of storing massive amounts of electricity produced from intermittent renewables. However, molecular decomposition represents a major barrier to commercialization-and although structural modifications can improve stability, it comes at the expense of synthetic cost and molecular weight. Now, utilizing 2,6-dihydroxy-anthraquinone (DHAQ) without further structural modification, we demonstrate that the regeneration of the original molecule after decomposition represents a viable route to achieve low-cost, long-lifetime aqueous organic redox flow batteries. We used in situ (online) NMR and electron paramagnetic resonance, and complementary electrochemical analyses to show that the decomposition compound 2,6-dihydroxy-anthrone (DHA) and its tautomer, 2,6-dihydroxy-anthranol (DHAL) can be recomposed to DHAQ electrochemically through two steps: oxidation of DHA(L)^2- to the dimer (DHA)₂^4- by one-electron transfer followed by oxidation of (DHA)₂^4- to DHAQ^2- by three-electron transfer per DHAQ molecule. This electrochemical regeneration process also rejuvenates the positive electrolyte-rebalancing the states of charge of both electrolytes without introducing extra ions.

Publication types

Research Support, Non-U.S. Gov't
Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

Anthralin*
Electrolytes / chemistry
Ions
Mitoxantrone*
Oxidation-Reduction

Substances

Electrolytes
Ions
Mitoxantrone
Anthralin