Near Neutral pH Redox Flow Battery with Low Permeability and Long-Lifetime Phosphonated Viologen Active Species

Jin, Shijian; Fell, Eric M.; Vina-Lopez, Lucia; Jing, Yan; Michalak, P. Winston; Gordon, Roy G.; Aziz, Michael J.

doi:10.1002/aenm.202000100

Near Neutral pH Redox Flow Battery with Low Permeability and Long-Lifetime Phosphonated Viologen Active Species

Journal Article · Mon Apr 06 00:00:00 EDT 2020 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202000100· OSTI ID:1608418

^[1]; ^[2]; Vina-Lopez, Lucia ^[2]; ^[3]; Michalak, P. Winston ^[3]; ^[2]; ^[2]

Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences; Harvard John A. Paulson School of Engineering and Applied Sciences
Harvard Univ., Cambridge, MA (United States). John A. Paulson School of Engineering and Applied Sciences
Harvard Univ., Cambridge, MA (United States)

A highly stable phosphonate-functionalized viologen is introduced in this work as the redox-active material in a negative potential electrolyte for aqueous redox flow batteries (ARFBs) operating at nearly neutral pH. The solubility is 1.23 m and the reduction potential is the lowest of any substituted viologen utilized in a flow battery, reaching –0.462 V versus SHE at pH = 9. The negative charges in both the oxidized and the reduced states of 1,1'-bis(3-phosphonopropyl)-[4,4'-bipyridine]-1,1'-diium dibromide (BPP–Vi ) effect low permeability in cation exchange membranes and suppress a bimolecular mechanism of viologen decomposition. A flow battery pairing BPP–Vi with a ferrocyanide-based positive potential electrolyte across an inexpensive, non-fluorinated cation exchange membrane at pH = 9 exhibits an open-circuit voltage of 0.9 V and a capacity fade rate of 0.016% per day or 0.00069% per cycle. Overcharging leads to viologen decomposition, causing irreversible capacity fade. Our research introduces extremely stable, extremely low-permeating and low reduction potential redox active materials into near neutral ARFBs.

View Accepted Manuscript (DOE)

Research Organization:: Harvard Univ., Cambridge, MA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE

Contributing Organization:: Massachusetts Clean Energy Center

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1608418

Alternate ID(s):: OSTI ID: 1608377

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 20 Vol. 10; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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