Nitrate is a common groundwater contaminant and poses health and environmental threats. Reductive denitrification of nitrate by zero-valent iron was investigated in unbuffered solutions at 20 °C. Nitrate was effectively removed at low initial solution pH. The reaction was accompanied by the production and then disappearance of a small quantity of nitrite, suggesting that nitrite was the intermediate and subsequently further reduced. A rapid rise in solution pH was also observed during the reaction. At the initial pH of 4, a reduction of 90% in nitrate concentration from 60 to 7.0 mg/L at 60 min was observed. The extent of nitrate removal decreased with increasing solution pH within the tested range of 3 - 6, suggesting that the reaction was an acid-driven process. The extent of nitrate removal also increased with Fe dosage over the range of 5 - 20 g/L, as higher Fe dosages provided more reactive surfaces. It is proposed that protons participate in the nitrate reduction by Fe0 via an initial reduction of protons to reduced hydrogen species followed by a subsequent reaction with nitrate. The hydrolysis of Fe corrosion products (e.g., ferrous ions) produces protons, in particular, near the surfaces of Fe, which drives the reaction to continue.
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