Membrane–Electrolyte System Approach to Understanding Ionic Conductivity and Crossover in Alkaline Flow Cells

George, Thomas Y.; Thomas, Isabelle C.; Haya, Naphtal O.; Deneen, John P.; Wang, Cliffton; Aziz, Michael J.

doi:10.1021/acsami.3c14173

ACS Appl. Mater. Interfaces

2023

DOI: 10.1021/acsami.3c14173

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Membrane–Electrolyte System Approach to Understanding Ionic Conductivity and Crossover in Alkaline Flow Cells

Thomas Y. George,

Isabelle C. Thomas,

Naphtal O. Haya

et al.

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2024

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Cited by 2 publications

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“…Since the semipermeable membrane is used in separating the positive and negative electrolytes of RFB, crossover problems have consistently been a significant challenge. The crossover of active species (metallic ion) used to be a challenge in all-iron RFB systems. − To overcome the easy crossover issue of single ions, metal-ligand complexes instead of metal ions are suggested as active materials . Some studies have indicated that the crossover of large-volume metal-ligand complexes is negligible, which uses the Donnan effect and the size exclusion effect. , However, our previous research has revealed that the crossover of free ligands from the negative electrolyte poses another challenging problem .…”

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confidence: 99%

Sulfonated-Ligand Engineering Enables a Stable Alkaline All-Iron Ion Redox Flow Battery

Yang,

Jiang,

Wang

et al. 2024

ACS Energy Lett.

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Alkaline all-iron ion redox flow batteries (RFBs) are considered promising devices for large-scale energy storage due to their remarkable resistance to dendrite formation and the hydrogen evolution reaction. However, the decomposition of negative complexes and ligand crossover issues have limited their stable operation. Herein, we have developed a tetrasulfonated ethylenediamine derivative ligand (EDTS) to chelate with iron ions to serve as the negative active species (Fe(EDTS)). Benefiting from its stable hexa-coordinated structure, the Fe(EDTS) chelate exhibits unprecedented stability during long-term cycling. Additionally, the EDTS ligand with high charge density and large volume effectively mitigates crossover through size exclusion and Donnan effects. Paired with the Fe(CN) 6 electrolyte, the Fe(CN) 6 /Fe(EDTS) RFB demonstrates a formal cell voltage of 1.25 V, a high energy density of 25.04 Ah L −1 , and an unprecedented durability among reported capacity-symmetric all-iron RFBs, achieving a Coulombic efficiency of 99.93% and capacity retention of 96.08% after 3000 cycles.

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Sulfonated-Ligand Engineering Enables a Stable Alkaline All-Iron Ion Redox Flow Battery

Yang,

Jiang,

Wang

et al. 2024

ACS Energy Lett.

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Protocol for Evaluating Anion Exchange Membranes for Nonaqueous Redox Flow Batteries

Tami,

Mazumder,

Cook

et al. 2024

ACS Appl. Mater. Interfaces

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Nonaqueous redox flow batteries often suffer from reduced battery lifetime and decreased coulombic efficiency due to crossover of the redox-active species through the membrane. One method to mitigate this undesired crossover is to judiciously choose a membrane based on several criteria: swelling and structural integrity, size and charge of redox active species, and ionic conductivity. Most research to date has focused on reducing crossover by synthesizing modified redox-active molecules and/or new membranes. However, no standard protocol exists to compare membranes and a comprehensive study comparing membranes has yet to be done. To address both these limitations, we evaluate herein 26 commercial anion exchange membranes (AEMs) to assess their compatibility with common nonaqueous solvents and their resistance to crossover by using neutral and cationic redox-active molecules. Ultimately, we found that all the evaluated AEMs perform poorly in organic solvents due to uncontrolled swelling, low ionic conductivity, and/or high crossover rates. We believe that this method, and the generated data, will be useful to evaluate and compare the performance of all AEMs�commercial and newly synthesized�and should be implemented as a standard protocol for future research.

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Membrane–Electrolyte System Approach to Understanding Ionic Conductivity and Crossover in Alkaline Flow Cells

Cited by 2 publications

References 78 publications

Sulfonated-Ligand Engineering Enables a Stable Alkaline All-Iron Ion Redox Flow Battery

Sulfonated-Ligand Engineering Enables a Stable Alkaline All-Iron Ion Redox Flow Battery

Protocol for Evaluating Anion Exchange Membranes for Nonaqueous Redox Flow Batteries

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