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

Journal Article · · Nature Chemistry
 [1];  [2];  [3];  [3];  [3];  [3];  [4];  [2];  [3];  [2];  [3];  [3]
  1. Harvard Univ., Cambridge, MA (United States); Harvard SEAS
  2. Univ. of Cambridge (United Kingdom)
  3. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences
  4. Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences; Ferdowsi University of Mashhad (FUM), Mashhad (Iran)
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Aqueous organic redox flow batteries (AORFBs) offer a safe and potentially inexpensive solution to the problem of storing massive amounts of electricity produced from intermittent renewables. However, molecular decomposition is the major barrier preventing AORFBs from being commercialized. Structural modifications can improve molecular stability at the expense of increased synthetic cost and molecular weight. Utilizing 2,6-dihydroxy-anthraquinone (DHAQ), without further structural modification, we demonstrate that electrochemical regeneration could be a viable route to achieve low-cost, long-lifetime AORFBs. In situ (online) NMR and EPR and complementary electrochemical analyses reveal that decomposition compounds i.e., 2,6-dihydroxy-anthrone (DHA) and its tautomer, 2,6-dihydroxy-anthranol (DHAL), can be converted back to DHAQ in two steps: first DHA(L)2- are oxidized to the dimer (DHA)24- at - 0.32 V vs. SHE by one-electron transfer; subsequently, the (DHA)24- is oxidized to DHAQ2- at +0.57 V vs. SHE by three-electron transfer. Electrochemical regeneration rejuvenates not only DHAQ2-, but also the positive electrolyte – rebalancing the states of charge of both electrolytes without introducing extra ions. We demonstrate the repeated capacity recovery with DHAQ | potassium ferro-/ferricyanide flow battery in basic conditions, and show the approach is also effective for anthraquinone-2,7-disulfonate in acid. Electrochemical regeneration strategies may extend the useful lifetime of many water-soluble organic molecules with anthraquinone core structures in electrochemical cells.
Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC05-76RL01830
OSTI ID:
1905990
Journal Information:
Nature Chemistry, Journal Name: Nature Chemistry Journal Issue: 10 Vol. 14; ISSN 1755-4330
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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25 ENERGY STORAGE