Degradation of carbamazepine in reverse osmosis concentrate of the secondary effluent by electrochlorination and its reaction mechanism

• The E-Cl system exhibited excellent performance for removal of EPs in ROC . • Bicarbonate and humic acid reduced CBZ removal. • ClO• and Cl 2 • - were major contributors to CBZ degradation in E-Cl. • C13-C14 double bond of CBZ was attacked by ClO•, Cl 2 • - and HO•. • The final oxidation products of CBZ had no or low toxicity. Reverse osmosis concentrate (ROC) from the secondary effluent in municipal wastewater reclamation contains emerging pollutants (EPs) that require further treatment, as these EPs may otherwise pose risks to human health and ecological balance. Since ROC has relatively high salinity, Electrochlorination (E-Cl) could exactly be a promising technology for its EPs removal. However, a comprehensive and systematic investigation has yet to be carried out. In this study, targeted at E-Cl process for the ROC treatment, a series of conscientiously designed experiments were conducted to evaluate the removal performance of carbamazepine (CBZ), investigate the effects of operating conditions and water matrix on the CBZ removal, and reveal its reaction mechanisms. An excellent CBZ removal efficiency of 99.8 % was achieved within 30 min at 2 mA cm −2 in 5 mM NaCl solution. Among water matrix components, SO 4 2- , NO 3 – , PO 4 3- and NH 4 + showed minimal effects, whereas HCO 3 – and humic acid had significant influences on the CBZ removal. The roles of ClO• and Cl 2 • - radicals in the E-Cl process were clarified through quenching experiments combined with electron paramagnetic resonance and radical probe tests. The steady-state concentrations of ClO• (88.95 × 10 -14 M) and Cl 2 • - (493.02 × 10 -14 M) were much higher than those of HO• (6.91 × 10 -14 M). Both ClO• and Cl 2 • - played key roles in CBZ degradation in the E-Cl process. Probable degradation pathways of CBZ were proposed based on the intermediates identification and density function theory (DFT) calculations. This study demonstrates the potential of E-Cl systems for effective EPs removal in ROC, providing mechanistic insights for practical applications.

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Publication Details

Journal
Separation and Purification Technology
Published
2025-04-08
DOI
https://doi.org/10.1016/j.seppur.2025.132952
Primary Topic
Advanced oxidation water treatment
Type
article
Field-Weighted Citation Impact
0.00

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article

Degradation of carbamazepine in reverse osmosis concentrate of the secondary effluent by electrochlorination and its reaction mechanism

Peiying Liu, Liping Duan, Yonghui Song, Liangjie Wang et al.
Separation and Purification Technology
Advanced oxidation water treatment
article

Degradation of carbamazepine in reverse osmosis concentrate of the secondary effluent by electrochlorination and its reaction mechanism

Peiying Liu, Liping Duan, Yonghui Song, Liangjie Wang, Xianghua Wen, Feng Qian, Pingzhou Duan, Haiyang He
article en

Abstract

• The E-Cl system exhibited excellent performance for removal of EPs in ROC . • Bicarbonate and humic acid reduced CBZ removal. • ClO• and Cl 2 • - were major contributors to CBZ degradation in E-Cl. • C13-C14 double bond of CBZ was attacked by ClO•, Cl 2 • - and HO•. • The final oxidation products of CBZ had no or low toxicity. Reverse osmosis concentrate (ROC) from the secondary effluent in municipal wastewater reclamation contains emerging pollutants (EPs) that require further treatment, as these EPs may otherwise pose risks to human health and ecological balance. Since ROC has relatively high salinity, Electrochlorination (E-Cl) could exactly be a promising technology for its EPs removal. However, a comprehensive and systematic investigation has yet to be carried out. In this study, targeted at E-Cl process for the ROC treatment, a series of conscientiously designed experiments were conducted to evaluate the removal performance of carbamazepine (CBZ), investigate the effects of operating conditions and water matrix on the CBZ removal, and reveal its reaction mechanisms. An excellent CBZ removal efficiency of 99.8 % was achieved within 30 min at 2 mA cm −2 in 5 mM NaCl solution. Among water matrix components, SO 4 2- , NO 3 – , PO 4 3- and NH 4 + showed minimal effects, whereas HCO 3 – and humic acid had significant influences on the CBZ removal. The roles of ClO• and Cl 2 • - radicals in the E-Cl process were clarified through quenching experiments combined with electron paramagnetic resonance and radical probe tests. The steady-state concentrations of ClO• (88.95 × 10 -14 M) and Cl 2 • - (493.02 × 10 -14 M) were much higher than those of HO• (6.91 × 10 -14 M). Both ClO• and Cl 2 • - played key roles in CBZ degradation in the E-Cl process. Probable degradation pathways of CBZ were proposed based on the intermediates identification and density function theory (DFT) calculations. This study demonstrates the potential of E-Cl systems for effective EPs removal in ROC, providing mechanistic insights for practical applications.

Separation and Purification TechnologyVol. 367
Peking University (CN), Chinese Research Academy of Environmental Sciences (CN), Tsinghua University (CN)
National Natural Science Foundation of China, Science and Technology Major Project of Inner Mongolia, National Key Research and Development Program of China
Clean water and sanitation
Openalex Percentile: Top 92%
Advanced oxidation water treatment
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