The role of active manganese species and free radicals in permanganate/bisulfite process

Chen, Jie; Rao, Dandan; Dong, Hongyu; Sun, Bo; Shao, Bin; Cao, Gaoshao; Guan, Xiaohong

doi:10.1016/j.jhazmat.2019.121735

Cited by 87 publications

(41 citation statements)

References 61 publications

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“…Very recently, intermediate Mn species dominated extremely fast oxidation of organic contaminants by coupling KMnO 4 , and bisulfite has attracted much attention, which initiates a new category of permanganate-based AOPs. , However, the relatively low electron utilization and residual salinity in effluents are the intrinsic shortages for environmental application. To overcome these drawbacks, biochar was employed as an electron sacrificer for promoting KMnO 4 oxidation .…”

Section: Introductionmentioning

confidence: 99%

Insights into the Electron-Transfer Mechanism of Permanganate Activation by Graphite for Enhanced Oxidation of Sulfamethoxazole

Peng

Zhou

et al. 2021

Environ. Sci. Technol.

189

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Many reagents as electron sacrificers have been recently investigated to induce decomposition of permanganate (KMnO 4 ) to produce highly reactive intermediate Mn species toward oxidation of organic contaminants; however, this strategy meanwhile causes low KMnO 4 utilization efficiency. This study surprisingly found that graphite can mediate direct electron transfer from organics (e.g., sulfamethoxazole (SMX)) to KMnO 4 , resulting in high KMnO 4 utilization efficiency, rather than reductive sites of graphite-induced conversion of KMnO 4 to highly reactive intermediate Mn species. The galvanic oxidation process (GOP) and comparative experiments of different organic contaminants prove that the KMnO 4 /graphite system mainly extracts electrons from organic contaminants via a one-electron pathway instead of a two-electron pathway. More importantly, the KMnO 4 /graphite system has superior reusability, graphite can keep a long-lasting reactivity, and the KMnO 4 utilization efficiency elevates significantly after each cycle of graphite. The transformation of SMX in the KMnO 4 /graphite system mainly includes self-coupling, hydroxylation, oxidation, and hydrolytic reaction. The work will improve insights into the electrontransfer mechanism and unveil the advantages of efficient KMnO 4 utilization in the KMnO 4 -based technologies in environmental remediation.

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Section: Introductionmentioning

confidence: 99%

Insights into the Electron-Transfer Mechanism of Permanganate Activation by Graphite for Enhanced Oxidation of Sulfamethoxazole

Peng

Zhou

et al. 2021

Environ. Sci. Technol.

189

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“…When the pH increased from 3.0 to 11.0, DCF removal efficiency and PM consumption both decreased significantly, which indicated that the MFC-PM process for DCF removal was a highly pH-dependent reaction, and lower pH values were suitable for DCF removal. On one hand, the oxidation potential of PM decreased with increasing pH, which could affect the reaction activity of PM (Equations ( 9)-( 11)) [19]. On the other hand, the cathode potentials changed markedly, and arrived at the highest value in the condition of pH = 3.0.…”

Section: Effect Of Catholyte Phmentioning

confidence: 99%

“…•− ), are generated by the rapid oxidation of pollutants [18,19]. Ultraviolet (UV) irradiation, biochar, and some reagents (e.g., bisulfite and humic acid (HA)) have been successfully applied to activate PM.…”

Section: Introductionmentioning

confidence: 99%

Degradation of Diclofenac in Urine by Electro-Permanganate Process Driven by Microbial Fuel Cells

Wang

Zhang

et al. 2021

Water

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A novel microbial fuel cell-assisted electro-permanganate process (MFC-PM) was proposed for enhanced diclofenac degradation compared to that of the permanganate oxidation process. By utilizing eco-friendly bio-electricity in situ, the MFC-PM process could activate the simultaneous anodic biological metabolism of urea and the cathodic electro-permanganate process. Density functional analysis and experimental evidence revealed the reactive manganese species (Mn(VII)aq, Mn(VI)aq, Mn(V)aq, and Mn(III)aq), generated via single electron transfer, contributed to diclofenac degradation in the cathodic chamber. The sites of diclofenac with a high Fukui index were preferable to be attacked by reactive manganese species, and diclofenac degradation was mainly accomplished through the ring hydroxylation, ring opening, and decarboxylation processes. Biological detection revealed clostridia were the primary electron donor in the anode chamber in an anaerobic environment. Furthermore, maximum output power density of 1.49 W m−3 and the optimal removal of 94.75% diclofenac were obtained within 20 min under the conditions of pH = 3.0, [DCF]0 = 60 µM, and [PM]0 = 30 µM. Diclofenac removal efficiency increased with external resistance, higher PM dosage, and lower catholyte pH. In addition, the MFC-PM process displayed excellent applicability in urine and other background substances. The MFC-PM process provided an efficient and energy-free bio-electricity catalytic permanganate oxidation technology for enhancing diclofenac degradation.

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“…•À ), and HO • ) (Chen et al, 2020;Chen et al, 2021;Sun et al, 2016;Sun, Bao, et al, 2018;Sun, Li, et al, 2018;Zhu et al, 2019;Zhu et al, 2020). This oxidation technology (denoted as PM/BS process) is able to eliminate a wide range of EOCs at extraordinarily rapid rates that were 5 to 6 orders of magnitude faster than those using permanganate alone and $5 to 7 orders of magnitude faster than other conventional advanced oxidation processes (UV, UV/H 2 O 2 , photo-Fenton, etc.)…”

Section: Introductionmentioning

confidence: 99%

“…Moreover, an extra treatment unit (normally a tank) for reaction is indispensable when these oxidation technologies are applied, which may limit their application, especially when restricted space is available. To overcome these disadvantages, our group invented a novel oxidation technology, where S (IV), a mixture of bisulfite (HSO 3 − , BS), and sulfite (SO 3 2− ) were employed to activate PM to generate various reactive oxidizing species (ROS, including Mn(V), Mn (VI), sulfate radical (SO 4 •− ), and HO • ) (Chen et al, 2020; Chen et al, 2021; Sun et al, 2016; Sun, Bao, et al, 2018; Sun, Li, et al, 2018; Zhu et al, 2019; Zhu et al, 2020). This oxidation technology (denoted as PM/BS process) is able to eliminate a wide range of EOCs at extraordinarily rapid rates that were 5 to 6 orders of magnitude faster than those using permanganate alone and ∼5 to 7 orders of magnitude faster than other conventional advanced oxidation processes (UV, UV/H 2 O 2 , photo‐Fenton, etc.)…”

Section: Introductionmentioning

confidence: 99%

A novel design of in‐line static mixer for permanganate/bisulfite process: Numerical simulations and pilot‐scale testing

Han

Guan

Sun

et al. 2022

Water Environment Research

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An increasing number of chemical technologies to wipe out contaminants within an incredibly short period of time have been developed recently, while their application was always hindered by the inefficient or improper mixing of reactants. To address this issue, the present work proposed a new static mixer named Tai-Chi which consists of blade, fin, and spoiler elements. Tai-Chi mixer can slice and divert the solutions inside and generate high shear flow to promote mixing process. Numerical simulations helped to determine the optimal operating conditions for Tai-Chi mixer, including laying its components anterior to the injection nozzles and keeping the velocity rate ratio of main pipe to branch pipe within the range of 0.5 to 1. Numerical simulations further proved that Tai-Chi mixer could strike a great balance between mixing performance (coefficient of variation [CoV] reaches 0.1 within 5 to 7 pipe diameters downstream) and head loss (nearly a half of other high shear static mixer in the market). Data of pilot-scale testing by Tai-Chi mixer confirm that 80% sulfamethoxazole could be eliminated in permanganate/bisulfite process within 8 pipe diameters, as well as showed the superiority of Tai-Chi's mixing performance in early stage compared with other static mixers in the market. Practitioner Points• A Tai-Chi static mixer with blade, fin, and spoiler elements is devised.• The optimal condition of flow rate and installment of Tai-Chi mixer is determined.• Ultra-fast mixing is achieved by Tai-Chi (CoV < 0.1 within 5-7 pipe diameters).• Pilot-scale test verifies the mixing efficiency of Tai-Chi mixer.

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The role of active manganese species and free radicals in permanganate/bisulfite process

Cited by 87 publications

References 61 publications

Insights into the Electron-Transfer Mechanism of Permanganate Activation by Graphite for Enhanced Oxidation of Sulfamethoxazole

Insights into the Electron-Transfer Mechanism of Permanganate Activation by Graphite for Enhanced Oxidation of Sulfamethoxazole

Degradation of Diclofenac in Urine by Electro-Permanganate Process Driven by Microbial Fuel Cells

A novel design of in‐line static mixer for permanganate/bisulfite process: Numerical simulations and pilot‐scale testing

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