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Title: A Phosphonate-Functionalized Quinone Redox Flow Battery at Near-Neutral pH with Record Capacity Retention Rate

Journal Article · · Advanced Energy Materials

A highly stable phosphonate-functionalized anthraquinone is introduced as the redox-active material in a negative potential electrolyte (negolyte) for aqueous redox flow batteries operating at nearly neutral pH. Here, the design and synthesis of 2,6-DPPEAQ, (((9,10-dioxo-9,10-dihydroanthracene-2,6-diyl)bis(oxy))bis(propane-3,1-diyl))bis(phosphonic acid), which has a high solubility at pH 9 and above, is described. Chemical stability studies demonstrate high stability at both pH 9 and 12. By pairing 2,6-DPPEAQ with a potassium ferri/ferrocyanide positive electrolyte across an inexpensive, nonfluorinated permselective polymer membrane, this near-neutral quinone flow battery exhibits an open-circuit voltage of 1.0 V and a capacity fade rate of 0.00036% per cycle and 0.014% per day, which is the lowest ever reported for any flow battery in the absence of rebalancing processes. It is further demonstrated that the negolyte pH drifts upward upon atmospheric oxygen penetration but, when oxygen is excluded, oscillates reversibly between 9 and 12 during cycling. These results enhance the suitability of aqueous-soluble redox-active organics for use in large-scale energy storage, potentially enabling massive penetration of intermittent renewable electricity.

Research Organization:
Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences (SEAS); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE; National Science Foundation (NSF); Innovation Fund Denmark; Massachusetts Clean Energy Technology Center
Grant/Contract Number:
AC05-76RL01830; 428977
OSTI ID:
1661884
Alternate ID(s):
OSTI ID: 1493638
Journal Information:
Advanced Energy Materials, Vol. 9, Issue 12; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 166 works
Citation information provided by
Web of Science

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Cited By (5)

A pH‐Neutral, Metal‐Free Aqueous Organic Redox Flow Battery Employing an Ammonium Anthraquinone Anolyte journal September 2019
A pH‐Neutral, Metal‐Free Aqueous Organic Redox Flow Battery Employing an Ammonium Anthraquinone Anolyte journal November 2019
In situ NMR metrology reveals reaction mechanisms in redox flow batteries journal March 2020
Structure reorganization-controlled electron transfer of bipyridine derivatives as organic redox couples journal January 2019
Investigating the Effects of Primary Amine Linkers with Different Carbon Chain Lengths on the Acid Dissociation Constant (p K a) for Covalently Immobilized Anthraquinone at the Electrode Surface Using Linear and Non-Linear Fittings journal January 2019

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