Drinking water utilities are interested in upgrading their treatment facilities to enhance micropollutant removal and byproduct control. Pre-oxidation by chlorine dioxide (ClO
2) followed by coagulation-flocculation-sedimentation and advanced oxidation processes (AOPs) is one of the promising solutions. However, the chlorite (ClO
2–) formed from the ClO
2 pre-oxidation stage cannot be removed by the conventional coagulation process using aluminum sulfate. ClO
2– negatively affects the post-UV/chlorine process due to its strong radical scavenging effect, and it also enhances the formation of chlorate (ClO
3–). In this study, dosing micromolar-level ferrous iron (Fe(II)) into aluminum-based coagulants was proposed to eliminate the ClO
2– generated from ClO
2 pre-oxidation and benefit the post-UV/chlorine process in radical production and ClO
3– reduction. Results showed that the addition of 52.1-µmol/L FeSO
4 effectively eliminated the ClO
2– generated from the pre-oxidation using 1.0 mg/L (14.8 µmol/L) of ClO
2. Reduction of ClO
2– increased the degradation rate constant of a model micropollutant (carbamazepine) by 55.0% in the post-UV/chlorine process. The enhanced degradation was verified to be attributed to the increased steady-state concentrations of HO
· and ClO
· by Fe(II) addition. Moreover, Fe(II) addition also decreased the ClO
3– formation by 53.8% in the UV/chlorine process and its impact on the formation of chloro-organic byproducts was rather minor. The findings demonstrated a promising strategy to improve the drinking water quality and safety by adding low-level Fe(II) in coagulation in an advanced drinking water treatment train.
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