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Mediating anion-cation interactions to improve aqueous flow battery electrolytes AITranslate

University of Colorado Boulder; University of Colorado Boulder;Empa-Swiss Federal Laboratories for Materials Science and Technology, Dübendorf 8600; National Renewable Energy Laboratory; University of Colorado Boulder; University of Colorado Boulder; University of Colorado Boulder; University of Colorado Boulder
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Publisher: Elsevier
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Abstract AITranslate

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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Citation Information:

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.