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Nitrate (NO3−) removal by photochemical-reduction has received extensive attention. However, the low selectivity of NO3− reduction to N2 hinders the application of this technology. In this study, a novel Cu@Fe-Cu-CuFe2O4−x photocatalyst was prepared by modifying CuFe2O4 with KBH4 and Cu(II), and used to selectively reduce NO3− to N2 with a two-step reduction process. In step (1), with Cu@Fe-Cu-CuFe2O4−x/ultraviolet (UV) system, 91.0% NO3− was reduced to 52.3% NO2− and 39.4% N2 within 60 min. The rapid removal of NO3− was due to the synergistic effect of oxygen vacancies, Fe-Cu corrosion cell, and CuFe2O4 photocatalysis. In step (2), H2C2O4 and H2O2 were introduced into the effluent of step (1) to promote CO2·− formation via Fe(II) and Fe(III) catalysis and UV radiation, which boosted the selective reduction of NO2− to N2. When H2C2O4 and H2O2 dosages were both 4.0 mmol·L−1 and the reaction time was 30 min, the removal efficiency of NO2− achieved 100% and the selectivity of N2 was 83.0%. Overall, the two-step reduction process achieved 95.0% NO3− removal efficiency and 90.1% N2 selectivity with initial NO3− concentration of 30 mg·N·L−1. In addition, the denitrification mechanism of the two-step reduction process was tentatively proposed.
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