A Long-Lifetime All-Organic Aqueous Flow Battery Utilizing TMAP-TEMPO Radical

Qing, Guangyan; Goulet, Marc‐Antoni; Tong, Liuchuan; Liu, Yazhi; Ji, Yunlong; Wu, Liang; Gordon, Roy G.; Aziz, Michael J.; Yang, Zhengjin

doi:10.1016/j.chempr.2019.04.021

Cited by 251 publications

(260 citation statements)

References 25 publications

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“…The total capacity loss during cell cycling might be caused by chemical degradation or crossover of viologens. The permeability of BHOE‐Vi, BHOP‐Vi, and BTMAP‐Vi across the DSV membrane was measured according to previous reports (Figure e and Figure S13 in the Supporting Information) . Permeability measurements suggest that the membrane permeability of hydroxylated viologens decreased with an increase in molecule size and was sharply reduced for BTMAP‐Vi owing to coulombic charge repulsion between charged substituent with the membrane (Figure S14 in the Supporting Information).…”

Section: Figurementioning

confidence: 84%

Screening Viologen Derivatives for Neutral Aqueous Organic Redox Flow Batteries

Qing¹,

Li²,

Zuo³

et al. 2020

ChemSusChem

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Viologen derivatives have been developeda sn egative electrolyte for neutrala queous organic redox flow batteries (AOFBs), but the structure-performancer elationship remains unclear. Here, it was investigated how the structure of viologens impacts their electrochemical behavior and thereby the battery performance, by taking hydroxylated viologensa se xamples. Calculations of frontierm olecular orbitale nergy and molecular configuration promise to be an effective tool in predicting potential, kinetics, and stability,a nd may be broadly applicable. Specifically,amodified viologen derivative, BHOP-Vi, was provedt ob et he most favorable structure, enablingaconcentrated 2 m battery to exhibit ap owerd ensity of 110.87 mW cm À2 and an excellent capacityr etention rate of 99.953 %h À1 .Renewable energy plays an indispensable role in replacing fossil fuel energy and provides ap ossible solution for as ustainable future. [1] However,t he large-scale adoption of renewable energy,s uch as solar and wind energy,i si mpeded by their intermittent and fluctuating features. The fluctuation in renewable energy supply can be solved by electrochemical energystoraget echnology,w hich stores electricity in electrochemically active materials and provides stable electricity output when needed. [2] As an emerging energy-storage technology,a queous organic redoxf low batteries (AOFBs) exploit the reversible redox reaction of low-cost organic compounds dissolved in aqueous solutions. [3] AOFBs that operate under neutral conditions do not involveh ighly basic or acidic solutionsa nd are therefore safe to handle and have fewer requirementso nb attery components. [4] The electrolyte solutionso faneutralA OFB flow along opposite sides of an ion-selective membrane and are circulated between cell stacksa nd externalt anks. The tanks can be as large as possible to provide long-duration energy supply,a nd the powerc apability can be independently tuned. Powerc apability and cycle lifetime of an eutral AOFB can be effectively tailoredb ye ngineering the chemical structure of redox-active organic electrolytes.Viologens, the characteristicn egative electrolytes (negolytes) for neutral AOFBs, have attracted increasingr esearch interests because of their diverse structure and straightforward chemical modification. The simplest viologen,m ethyl viologen,i sc ommerciallya vailablea nd can also be readily synthesized on a large scale with high yield by reacting bipyridine with either methyli odide or chloroacetic acid. [5] When paired with 4-OH-TEMPO [TEMPO = (2,2,6,6-tetramethylpiperidin-1-yl)oxyl],i tc an deliver ab attery capacity of 13.4 Ah L À1 and ac apacity loss rate of 3.6 %p er day.T his high capacity loss rate is owing to the dimerization of the intermediate, the cationic viologen radical. [6] To prevent the dimerization, Aziz and co-workers took advantage of coulombic repulsion, [7] and after adding quaternary ammonium groups to the viologen core they reporteda much lower capacity loss rate of 0.03 %p er day for the BTMAP-Vi/BTMAP-Fc cell ...

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Section: Figurementioning

confidence: 84%

Screening Viologen Derivatives for Neutral Aqueous Organic Redox Flow Batteries

Qing¹,

Li²,

Zuo³

et al. 2020

ChemSusChem

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“…Different molecular engineering strategies have been reported to increase the solubility of anthraquinones in aqueous solution . Anthraquinones with different water‐solubilizing groups require aqueous solution with distinct acidity for optimal solubility; acidic units, such as alcohol, phosphonic acid, and carboxylic acid, require alkaline solvents for the deprotonation of the substituents for high water solubility, whereas sulfonated anthraquinone requires highly acidic H 2 SO 4 solution for high solubility .…”

Section: Resultsmentioning

confidence: 99%

“…Several classes of organic active materials have been extensively investigated in organic RFBs, including (but not limited to): quinone, viologen, 2,2,6,6‐tetramethylpiperidine‐1‐oxyl (TEMPO), phenothiazine, and metallocene compounds . Our group has successfully demonstrated the PEGylation (PEG=poly(ethylene glycol)) strategy in organic RFBs using viologen and phenothiazine as the redox active materials .…”

Section: Introductionmentioning

confidence: 99%

A pH‐Neutral, Aqueous Redox Flow Battery with a 3600‐Cycle Lifetime: Micellization‐Enabled High Stability and Crossover Suppression

et al. 2020

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Redox‐flow batteries (RFBs) are a highly promising large‐scale energy storage technology for mitigating the intermittent nature of renewable energy sources. Here, the design and implementation of a micellization strategy in an anthraquinone‐based, pH‐neutral, nontoxic, and metal‐free aqueous RFB is reported. The micellization strategy (1) improves stability by protecting the redox‐active anthraquinone core with a hydrophilic poly(ethylene glycol) shell and (2) increases the overall size to mitigate the crossover issue through a physical blocking mechanism. Paired with a well‐established potassium ferrocyanide catholyte, the micelle‐based RFB displayed an excellent capacity retention of 90.7 % after 3600 charge/discharge cycles (28.3 days), corresponding to a capacity retention of 99.67 % per day and 99.998 % per cycle. The mechanistic studies of redox‐active materials were also conducted and indicated the absence of side reactions commonly observed in other anthraquinone‐based RFBs. The outstanding performance of the RFB demonstrates the effectiveness of the micellization strategy for enhancing the performance of organic material‐based aqueous RFBs.

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“…In addition to quinone derivatives, other families of redox molecules have also been studied, such as polyaniline (PANI), polythiophene, viologen derivatives, 2,2,6,6‐tetramethylpiperidine‐1‐oxyl (TEMPO), alkoxybenzene‐based molecules . Profiting from the possibility to modulate the physical chemical properties of organic molecules and the stability of inorganic compounds, organometallic mediators appear to be good candidates for redox flow battery systems.…”

Section: Introductionmentioning

confidence: 99%

Recent Advances in the Development of Organic and Organometallic Redox Shuttles for Lithium‐Ion Redox Flow Batteries

et al. 2020

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In recent years, redox flow batteries (RFBs) and derivatives have attracted wide attention from academia to the industrial world because of their ability to accelerate large‐grid energy storage. Although vanadium‐based RFBs are commercially available, they possess a low energy and power density, which might limit their use on an industrial scale. Therefore, there is scope to improve the performance of RFBs, and this is still an open field for research and development. Herein, a combination between a conventional Li‐ion battery and a redox flow battery results in a significant improvement in terms of energy and power density alongside better safety and lower cost. Currently, Li‐ion redox flow batteries are becoming a well‐established subdomain in the field of flow batteries. Accordingly, the design of novel redox mediators with controllable physical chemical characteristics is crucial for the application of this technology to industrial applications. This Review summarizes the recent works devoted to the development of novel redox mediators in Li‐ion redox flow batteries.

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A Long-Lifetime All-Organic Aqueous Flow Battery Utilizing TMAP-TEMPO Radical

Cited by 251 publications

References 25 publications

Screening Viologen Derivatives for Neutral Aqueous Organic Redox Flow Batteries

Screening Viologen Derivatives for Neutral Aqueous Organic Redox Flow Batteries

A pH‐Neutral, Aqueous Redox Flow Battery with a 3600‐Cycle Lifetime: Micellization‐Enabled High Stability and Crossover Suppression

Recent Advances in the Development of Organic and Organometallic Redox Shuttles for Lithium‐Ion Redox Flow Batteries

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