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

Abstract

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.

Authors:

Ji, Yunlong  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-1124-4209"

Goulet, Marc-Antoni  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-9146-6759"

Pollack, Daniel A.  ^[1];

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• Search DOE PAGES for ORCID "0000-0003-3909-5118"

Kwabi, David G.  ^[1];

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• Search DOE PAGES for ORCID "0000-0003-3649-1270"

Jin, Shijian  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-9450-9606"

De Porcellinis, Diana  ^[1];

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• Search DOE PAGES for ORCID "0000-0003-2503-0305"

Kerr, Emily F.  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-5750-1514"

Gordan, Roy G.  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-5980-268X"

Aziz, Michael J.  ^[1]

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• Search DOE PAGES for ORCID "0000-0001-9657-9456"

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+ Show Author Affiliations

1. Harvard Univ., Cambridge, MA (United States)

Publication Date:

Wed Feb 06 00:00:00 EST 2019

Research Org.:

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 Org.:

USDOE; National Science Foundation (NSF); Innovation Fund Denmark; Massachusetts Clean Energy Technology Center

OSTI Identifier:

1661884

Alternate Identifier(s):

OSTI ID: 1493638

Grant/Contract Number:  

AC05-76RL01830; 428977

Resource Type:

Accepted Manuscript

Journal Name:

Advanced Energy Materials

Additional Journal Information:

Journal Volume: 9; Journal Issue: 12; Journal ID: ISSN 1614-6832

Publisher:

Wiley

Country of Publication:

United States

Language:

English

Subject:

25 ENERGY STORAGE; energy storage; long lifetime; quinone; redox‐flow batteries