Ion-exchange (IX) is common for separating NO
3− from drinking water. From both cost and environmental perspectives, the IX regeneration brine must be recycled, via nitrate reduction to N
2(g). Nano zero-valent iron (nZVI) reduces nitrate efficiently to ammonia, under brine
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Ion-exchange (IX) is common for separating NO
3− from drinking water. From both cost and environmental perspectives, the IX regeneration brine must be recycled, via nitrate reduction to N
2(g). Nano zero-valent iron (nZVI) reduces nitrate efficiently to ammonia, under brine conditions. However, to be sustainable, the formed ammonia should be oxidized. Accordingly, a new process was developed, comprising IX separation, nZVI-based nitrate removal from the IX regeneration brine, followed by indirect ammonia electro-oxidation. The aim was to convert nitrate to N
2(g) while allowing repeated usage of the NaCl brine for multiple IX cycles. All process steps were experimentally examined and shown to be feasible: nitrate was efficiently separated using IX, which was subsequently regenerated with the treated/recovered NaCl brine. The nitrate released to the brine reacted with nZVI, generating ammonia and Fe(II). Fresh nZVI particles were reproduced from the resulting brine, which contained Fe(II), Na
+, Cl
− and ammonia. The ammonia in the nZVI production procedure filtrate was indirectly electro-oxidized to N
2(g) at the inherent high Cl
− concentration, which prepared the brine for the next IX regeneration cycle. The dominant reaction between nZVI and NO
3− was described best (Wilcoxon test) by 4Fe
(s) + 10H
+ + NO
3− → 4Fe
2+ + NH
4+ + 3H
2O, and proceeded at >5 mmol·L
−1·min
−1 at room temperature and 3 < pH < 5.
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