Development of a New Permanganate/Chlorite Process for Water Decontamination

Development of new technologies with strong selectivity for target pollutants and low sensitivity toward a water matrix remains challenging. Herein, we introduced a novel strategy that used chlorite as an activator for Mn(VII) at pH 4.8, turning the inert reactivity of the pollutants toward Mn(VII) into a strong reactivity. This paved a new way for triggering reactions in water decontamination. By utilizing sulfamethoxazole (SMX) as a typical pollutant, we proposed coupled pathways involving electron transfer across hydrogen bonds (TEHB) and oxidation by reactive manganese species. The results indicated that a hydrogen bonding complex, SMX-ClO<sub>2</sub><sup>-</sup>*, formed through chlorite binding the amino group of SMX initially in the TEHB route; such a complex exhibited a stronger reduction capability toward Mn(VII). Chlorite, in the hydrogen bonding complex SMX-ClO<sub>2</sub><sup>-</sup>*, can then complex with Mn(VII). Consequently, a new reactive center (SMX-ClO<sub>2</sub><sup>-</sup>-Mn(VII)*) was formed, initiating the transfer of electrons across hydrogen bonds and the preliminary degradation of SMX. This is followed by the involvement of the generated Mn(V)-ClO<sub>2</sub><sup>-</sup>/Mn(III) in the reduction process of Mn(VII). Such a process showed pH-dependent degradation, with a removal ratio ranging from 80% to near-stagnation as pH increased from 4.8 to 7. Combining with p<i>K</i><sub>a</sub> analysis showed that the predominant forms of contaminants were crucial for the removal efficiency of pollutants by the Mn(VII)/chlorite process. The impact of the water matrix was demonstrated to have few adverse or even beneficial effects. With satisfactory performance against numerous contaminants, this study introduced a novel Mn(VII) synergistic strategy, and a new reactivity pattern focused on reducing the reduction potential of the contaminant, as opposed to increasing the oxidation potential of oxidants.

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Publication Details

Journal
Environmental Science & Technology
Published
2024-09-02
DOI
https://doi.org/10.1021/acs.est.4c02257
Citations
9
Primary Topic
Advanced oxidation water treatment
Type
article
Field-Weighted Citation Impact
1.81

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article

Development of a New Permanganate/Chlorite Process for Water Decontamination

Hongguang Guo, Erdeng Du, Xiaohong Guan, Min Zheng et al.
9 citations
Environmental Science & Technology
Advanced oxidation water treatment
1.81
article

Development of a New Permanganate/Chlorite Process for Water Decontamination

Hongguang Guo, Erdeng Du, Xiaohong Guan, Min Zheng, Liping Luo, Jingquan Wang
article en
9 citations

Abstract

Development of new technologies with strong selectivity for target pollutants and low sensitivity toward a water matrix remains challenging. Herein, we introduced a novel strategy that used chlorite as an activator for Mn(VII) at pH 4.8, turning the inert reactivity of the pollutants toward Mn(VII) into a strong reactivity. This paved a new way for triggering reactions in water decontamination. By utilizing sulfamethoxazole (SMX) as a typical pollutant, we proposed coupled pathways involving electron transfer across hydrogen bonds (TEHB) and oxidation by reactive manganese species. The results indicated that a hydrogen bonding complex, SMX-ClO<sub>2</sub><sup>-</sup>*, formed through chlorite binding the amino group of SMX initially in the TEHB route; such a complex exhibited a stronger reduction capability toward Mn(VII). Chlorite, in the hydrogen bonding complex SMX-ClO<sub>2</sub><sup>-</sup>*, can then complex with Mn(VII). Consequently, a new reactive center (SMX-ClO<sub>2</sub><sup>-</sup>-Mn(VII)*) was formed, initiating the transfer of electrons across hydrogen bonds and the preliminary degradation of SMX. This is followed by the involvement of the generated Mn(V)-ClO<sub>2</sub><sup>-</sup>/Mn(III) in the reduction process of Mn(VII). Such a process showed pH-dependent degradation, with a removal ratio ranging from 80% to near-stagnation as pH increased from 4.8 to 7. Combining with p<i>K</i><sub>a</sub> analysis showed that the predominant forms of contaminants were crucial for the removal efficiency of pollutants by the Mn(VII)/chlorite process. The impact of the water matrix was demonstrated to have few adverse or even beneficial effects. With satisfactory performance against numerous contaminants, this study introduced a novel Mn(VII) synergistic strategy, and a new reactivity pattern focused on reducing the reduction potential of the contaminant, as opposed to increasing the oxidation potential of oxidants.

Environmental Science & TechnologyVol. 58(37)
Sichuan University (CN), UNSW Sydney (AU), Changzhou University (CN), East China Normal University (CN)
National Natural Science Foundation of China, Department of Science and Technology of Sichuan Province, National Key Research and Development Program of China
Clean water and sanitation
Openalex Percentile: Top 16%
Advanced oxidation water treatment
1.81
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