2019
DOI: 10.1021/jacs.9b07345
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Mechanism-Based Design of a High-Potential Catholyte Enables a 3.2 V All-Organic Nonaqueous Redox Flow Battery

Abstract: Nonaqueous redox flow batteries (RFBs) represent a promising technology for grid-scale energy storage. A key challenge for the field is identifying molecules that undergo reversible redox reactions at the extreme potentials required to leverage the large potential window of organic solvents. In this Article, we use a combination of computations, chemical synthesis, and mechanistic analysis to develop thioether-substituted cyclopropenium derivatives as high potential electrolytes for nonaqueous RFBs. These mole… Show more

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Cited by 125 publications
(142 citation statements)
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“…Subsequently, other organic redox-active molecules were successfully demonstrated in the redox flow batteries, employing both aqueous [67][68][69] and non-aqueous electrolytes, showing the great promises. [70,71] Analogous liquid-state organic electrodes were also explored in rechargeable non-flow battery systems, which contain solid electrolyte membranes that physically separate the two electrodes. The alkali metal biphenyl complexes were successfully utilized as the liquid-state anode with their low redox potential close to that of the elemental alkali metal electrode.…”
Section: Recent Paradigm Shifts In Utilizing Redox-active Organic Commentioning
confidence: 99%
“…Subsequently, other organic redox-active molecules were successfully demonstrated in the redox flow batteries, employing both aqueous [67][68][69] and non-aqueous electrolytes, showing the great promises. [70,71] Analogous liquid-state organic electrodes were also explored in rechargeable non-flow battery systems, which contain solid electrolyte membranes that physically separate the two electrodes. The alkali metal biphenyl complexes were successfully utilized as the liquid-state anode with their low redox potential close to that of the elemental alkali metal electrode.…”
Section: Recent Paradigm Shifts In Utilizing Redox-active Organic Commentioning
confidence: 99%
“…In addition to preventing cross contamination, symmetric ORFBs can access three different oxidation states of the electrolyte within the same compartment, resulting in a charged to one polarity or to the opposite polarity via one-electron cycles in opposite directions. To date, only three examples of symmetric ORFBs have been reported, (Figure 1, green box), [31][32][33] and these either possess a high OCV with low cyclability (Figure 1, example iv), or a better reliability (max 100 cycles) but a small OCV (Figure 1 (Cyclability = capacity (Q) retention >90% after n cycles) with their electrolyte couples: (i), 28 (ii), 29 (iii), 30 (iv), 31 (v) 32 and (vi) 33 .…”
Section: Toc Graphicsmentioning
confidence: 99%
“…These values are higher than other known anolytes, 29,42,43 and about four times higher than recent catholytes studied, which is an advantage for our DMQA + . [28][29][30]43,44 The electron transfer rate constants (k 0 ) were determined using the Nicholson method (Equation S2, Figures S5-6), 45 where the k 0 = 2.5(5) × 10 -3 cm s -1 for C + /C • redox couple is almost similar to that of the C •++ /C + redox pair k 0 = 2.3(1) × 10 -3 cm s -1 and both are comparable to recent electrolytes developed for RFB. 28,30 The persistent oxidized and reduced species of C + , and their fast and identical electronic kinetics, suggest that this electrolyte is suitable for ORFB application.…”
Section: Toc Graphicsmentioning
confidence: 99%
“…Whereas viologens and their progeny are promising as active species in redox flow batteries (RFBs), [9][10][11] their organoboron analogues have yet to be explored for similar applications. Viologens have been extensively explored as nonaqueous electrolytes, highlighted by results from Sanford and co-workers, [12] who have shown such compounds to be viable catholytes.…”
Section: Introductionmentioning
confidence: 99%
“…Such systems tend to have limited stability and/or solubilities on top of incomplete discharge through each redox event. [11,18] To summarize, a catholyte for nonaqueous redox flow batteries should have a highly negative reduction potential, a low molecular mass per electron transferred, and good solubility in all redox states. Sanford and co-workers have shown the viability of using diquat and viologens as catholytes in RFBs.…”
Section: Introductionmentioning
confidence: 99%