Mediating anion-cation interactions to improve aqueous flow battery electrolytes AITranslate
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The limited solubility of electrolyte active materials has impeded the development of energy dense aqueous redox flow batteries. Here, we report on the solubilizing effect urea has on metal-organic complexes chelated by aminopolycarboxylate ligands. Upon addition of urea, solubility enhancements of up to 60% or 125% are observed for chromium ethylenediaminetetraacetate (CrEDTA) and chromium 1,3-propylenediaminetetraacetate (CrPDTA) salts, respectively, resulting in maximum solubilities of e.g., 1.5 м for KCrPDTA and 2.2 м for NaCrEDTA. We investigate the mechanism behind enhanced solubility of aminopolycarboxylate chelates, revealing strong hydrogen bonding between urea and anions, resulting in eutectic-like destabilization of the solid phase. We study the impact of urea on the electrochemical performance of near neutral pH flow batteries and demonstrate 50% higher anolyte capacities, up to 40 Ah L−1, than previously reported for this promising class of materials. In capacity balanced full cells, using ferrocyanide catholytes, we observe excellent Coulombic efficiencies >99.6% and voltage efficiencies >78% at average discharge voltages of ca. 1.5 V when cycling at 100 mA cm−2. Peak discharge power densities of >400 mW cm−2 further highlight the potential of our facile and cost-effective approach. Finally, we discuss avenues for future work to further exploit the solubilizing effect described herein. Graphical abstract Download : Download high-res image (61KB) Download : Download full-size image
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DOI:https://doi.org/10.1016/j.apmt.2022.101512
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The limited solubility of electrolyte active materials has impeded the development of energy dense aqueous redox flow batteries. Here, we report on the solubilizing effect urea has on metal-organic complexes chelated by aminopolycarboxylate ligands. Upon addition of urea, solubility enhancements of up to 60% or 125% are observed for chromium ethylenediaminetetraacetate (CrEDTA) and chromium 1,3-propylenediaminetetraacetate (CrPDTA) salts, respectively, resulting in maximum solubilities of e.g., 1.5 м for KCrPDTA and 2.2 м for NaCrEDTA. We investigate the mechanism behind enhanced solubility of aminopolycarboxylate chelates, revealing strong hydrogen bonding between urea and anions, resulting in eutectic-like destabilization of the solid phase. We study the impact of urea on the electrochemical performance of near neutral pH flow batteries and demonstrate 50% higher anolyte capacities, up to 40 Ah L−1, than previously reported for this promising class of materials. In capacity balanced full cells, using ferrocyanide catholytes, we observe excellent Coulombic efficiencies >99.6% and voltage efficiencies >78% at average discharge voltages of ca. 1.5 V when cycling at 100 mA cm−2. Peak discharge power densities of >400 mW cm−2 further highlight the potential of our facile and cost-effective approach. Finally, we discuss avenues for future work to further exploit the solubilizing effect described herein. Graphical abstract Download : Download high-res image (61KB) Download : Download full-size image
quote
| GB/T 7714-2015 | [1] David Reber, Jonathan R. Thurston, Maximilian Becker, et al. Applied Materials Today, 2022(28). DOI:10.1016/j.apmt.2022.101512. |
| MLA | [1] David Reber, et al., Applied Materials Today, no. 28, 2022, https://doi.org/10.1016/j.apmt.2022.101512. |
| APA | [1] David Reber, Jonathan R. Thurston, Maximilian Becker, Gregory F. Pach, Marc E. Wagoner, Brian H. Robb, Scott E. Waters, & Michael P. Marshak. (2022). Applied Materials Today(28). https://doi.org/10.1016/j.apmt.2022.101512 |
| IEEE | [1] David Reber, Jonathan R. Thurston, Maximilian Becker, Gregory F. Pach, Marc E. Wagoner, Brian H. Robb, Scott E. Waters, and Michael P. Marshak, Applied Materials Today, no. 28, 2022, doi: 10.1016/j.apmt.2022.101512. |
