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Among them, Iron\u2010Chromium RFBs (Fe\u2010Cr RFBs), which utilize aqueous\u2010based electrolytes, effectively address critical challenges in renewable energy integration while offering unparalleled safety, low\u2010cost scalability and environmental compatibility. Potassium hexacyanochromate (K\n                    <jats:sub>3<\/jats:sub>\n                    [Cr(CN)\n                    <jats:sub>6<\/jats:sub>\n                    ]) has emerged as a promising negolyte material in Fe\u2010Cr RFBs due to its favorable electrochemical properties. However, enhancing its long\u2010term stability and elucidating its structural transformations remain crucial for optimized performance. Investigations into ligand exchange mechanism reveal connections to detrimental side reactions, notably hydrogen evolution reaction (HER) and hexacyanochromate instability, highlighting pathways for targeted improvement. Density functional theory (DFT) calculations illuminate the effects of ligand exchange dynamics and structural variations on redox stability, providing mechanistic insights into electrolyte behavior. By strategically incorporating sodium hydroxide with sodium cyanide as supporting electrolytes, our study demonstrates significantly improved stability of the redox couple, achieving a stable cycling performance over 250 cycles with an energy density of 13.91\u00a0Wh L\n                    <jats:sup>\u22121<\/jats:sup>\n                    and energy efficiencies exceeding 76%\u201377%. This research provides valuable insights into the degradation pathways of hexacyanochromate\u2010based negolyte and emphasizes the importance of optimized electrolyte design for advancing sustainable energy storage technologies.\n                  <\/jats:p>","DOI":"10.1002\/anie.202507119","type":"journal-article","created":{"date-parts":[[2025,7,2]],"date-time":"2025-07-02T03:25:23Z","timestamp":1751426723000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":17,"title":["Elucidating Ligand Exchange Dynamics of Hexacyanochromate\u2010Based Redox Mediators in Aqueous Iron\u2010Chromium Redox Flow Batteries"],"prefix":"10.1002","volume":"64","author":[{"given":"Ji\u2010Eun","family":"Jang","sequence":"first","affiliation":[{"name":"School of Energy and Chemical Engineering Ulsan National Institute of Science and Technology  Ulsan 44919 Republic of 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