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Title: A Stable, Low Permeable TEMPO Catholyte for Aqueous Total Organic Redox Flow Batteries

Journal Article · · Advanced Energy Materials

We report aqueous organic redox flow batteries (AORFBs) are highly attractive for large-scale energy storage because of their nonflammability, low cost, and sustainability. (2,2,6,6-Tetramethylpiperidin-1-yl)oxyl (TEMPO) derivatives, a class of redox active molecules bearing air-stable free nitroxyl radicals and high redox potential (>0.8 V vs NHE), has been identified as promising catholytes for AORFBs. However, reported TEMPO based molecules are either permeable through ion exchange membranes or not chemically stable enough for long-term energy storage. Herein, a new TEMPO derivative functionalized with a dual-ammonium dicationic group, N1, N1, N1, N3, N3, 2, 2, 6, 6-nonamethyl-N3-(piperidinyloxy)propane-1,3-bis(ammonium) dichloride (N2-TEMPO) as a stable, low permeable catholyte for AORFBs is reported. Ultraviolet–visible (UV–vis) and proton nuclear magnetic resonance (1H-NMR) spectroscopic studies reveal its exceptional stability and ultra-low permeability (1.49 × 10-12 cm2 s-1). Coupled with 1,1'-bis[3-(trimethylammonio)propyl]-4,4'-bipyridinium tetrachloride ((NPr)2V) as an anolyte, a 1.35 V N2-TEMPO/(NPr)2V AORFB with 0.5 m electrolytes (9.05 Wh L-1) delivers a high power density of 114 mW cm-2 and 100% capacity retention for 400 cycles at 60 mA cm-2. At 1.0 m electrolyte concentrations, the N2-TEMPO/(NPr)2V AORFB achieves an energy density of 18.1 Wh L-1 and capacity retention of 90% for 400 cycles at 60 mA cm-2.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE; National Science Foundation (NSF); Utah Science Technology and Research initiative (USTAR); China CSC
Grant/Contract Number:
AC05-76RL01830; 1847674; 502995; 1429195
OSTI ID:
1968560
Report Number(s):
PNNL-SA-169500
Journal Information:
Advanced Energy Materials, Vol. 12, Issue 8; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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