• Reactive Zn and Al electrodes enable electrochemical extraction of Sr from molten salts despite Sr's more negative reduction potential than Li.
• Sr extraction products are Zn13Sr and Al4Sr intermetallic compounds, with no Li codeposition, confirmed by DFT calculations.
• Zn electrode achieves ~54% coulombic efficiency for Sr extraction, with depolarization values of 0.864 V (Zn) and 0.485 V (Al), indicating stronger Zn–Sr interaction.
• This method facilitates purification and reuse of molten salts in pyroprocessing, reducing nuclear waste volume.
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