Highly efficient electro-peroxone enhanced by oxygen-doped carbon nanotubes with triple role of in-situ H2O2 generation, activation and catalytic ozonation

Gu, Jinyu; Xie, Jinxin; Li, Shasha; Song, Ge; Zhou, Minghua

doi:10.1016/j.cej.2022.139597

Cited by 28 publications

(14 citation statements)

References 66 publications

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“…38 where j is the measured current density; j k and j L are the kinetic and diffusion-limiting current densities, respectively; ω is the disk rotation rate; n is the number of electrons transferred per oxygen molecule; F is Faraday's constant ( F = 96 485 C); n is the number of electrons transferred per oxygen molecule; and D 0 are the oxygen bulk concentration (1.2 × 10 −6 mol cm −3 ) and diffusion coefficient of oxygen (1.9 × 10 −5 cm 2 s −1 ), respectively; and ν is the kinetic viscosity of the electrolyte (1.1 × 10 −2 cm 2 s −1 ). 39,40 The K–L plots revealed good linearity for all the samples, and n was calculated from the slope of the K–L plots (Fig. 7c).…”

Section: Resultsmentioning

confidence: 94%

“…Owing to the embedded and functionalized oxygen atoms, the surrounding site became an uneven electric charge state. 14,39 Thus, the neighboring carbon atoms were positively charged by the charge redistribution. 17,39 The conjugated oxygen atoms led to a positive charge, thus the neighboring carbon can be an active site for OER.…”

Section: Electrochemical Characteristicsmentioning

confidence: 99%

“…14,39 Thus, the neighboring carbon atoms were positively charged by the charge redistribution. 17,39 The conjugated oxygen atoms led to a positive charge, thus the neighboring carbon can be an active site for OER. The positively charged carbon facilitated the adsorption of the surrounding OH-by electrostatic forces, which efficiently evolved oxygen molecules during the OER.…”

Section: Electrochemical Characteristicsmentioning

confidence: 99%

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Defect- and oxygen-rich nanocarbon derived from solution plasma for bifunctional catalytic activity of oxygen reduction and evolution reactions

Kim,

Cha,

Kim

2023

RSC Adv.

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Section: Resultsmentioning

confidence: 94%

Section: Electrochemical Characteristicsmentioning

confidence: 99%

Section: Electrochemical Characteristicsmentioning

confidence: 99%

See 1 more Smart Citation

Defect- and oxygen-rich nanocarbon derived from solution plasma for bifunctional catalytic activity of oxygen reduction and evolution reactions

Kim,

Cha,

Kim

2023

RSC Adv.

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“…It is worth noting that precursors themselves can be electrochemically generated, for example, via direct oxidation of the sulfate anion (eq ). − The potential production of H 2 O 2 via oxygen reduction reaction (ORR, eq ) by carbonaceous cathodes often used for precursor activation is another reaction that can complicate matters. ,,− …”

Section: Introductionmentioning

confidence: 99%

Peroxymonosulfate-Based Electrochemical Advanced Oxidation: Complication by Oxygen Reduction Reaction

Lim,

Kim,

Rigby

et al. 2023

Environ. Sci. Technol.

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Peroxymonosulfate (PMS)-based electrochemical advanced oxidation processes (EAOPs) have received widespread attention in recent years, but the precise nature of PMS activation and its impact on the overall process performance remain poorly understood. This study presents the first demonstration of the critical role played by the oxygen reduction reaction in the effective utilization of PMS and the subsequent enhancement of overall pollutant remediation. We observed the concurrent generation of H2O2 via oxygen reduction during the cathodic PMS activation by a model nitrogen-doped carbon nanotube catalyst. A complex interplay between H2O2 generation and PMS activation, as well as a locally increased pH near the electrode due to the oxygen reduction reaction, resulted in a SO4 •–/•OH-mixed oxidation environment that facilitated pollutant degradation. The findings of this study highlight a unique dependency between PMS-driven and H2O2-driven EAOPs and a new perspective on a previously unexplored route for further enhancing PMS-based treatment processes.

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“…26,27 In addition, in situ H 2 O 2 activation might also occur at the cathode surface to generate HO• and/or singlet oxygen ( 1 O 2 ), contributing to pollutants removal. 28,29 Recently, Xu and von Gunten 30 found that H 2 O 2 could enhance Mn(VII) oxidation toward organic pollutants, and they further investigated the reaction mechanism and identified the role of the main active species. When Mn(VII) was present in excess, Mn(VII) reacted quickly with H 2 O 2 via one-electron reduction to produce Mn(VI) and superoxide radical (O 2…”

Section: Introductionmentioning

confidence: 99%

Enhanced Degradation of Diclofenac by Electro-Activated Permanganate: A Critical Role of In Situ Formed H₂O₂

Zhang,

Guan,

Guo

et al. 2023

ACS EST Eng.

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Electrochemical technologies and permanganate oxidation are two attractive strategies in water treatment due to their low cost, easy operation, good adaptability, and environmental friendliness. Interestingly, recent studies have demonstrated that the combination of electrolysis and Mn(VII) (E-Mn(VII) process) shows a synergetic effect on organic contaminants degradation. However, the underlying mechanism of the E-Mn(VII) process remains unclear. In this study, the enhanced removal of diclofenac (DCF) by the E-Mn(VII) process was also demonstrated, and the main reactive species were reidentified. It was found that H 2 O 2 was considerably formed via the reduction of O 2 on the cathode, and it played a key role in facilitating Mn(VII) transformation into MnO 2 . Increasing O 2 concentration, working potential, and pH value were conducive to H 2 O 2 formation as well as Mn(VII) transformation to MnO 2 . Higher Mn(VII) dosages did not impact H 2 O 2 formation but also led to faster MnO 2 formation. The enhanced formation of MnO 2 was favorable for the fast degradation of DCF in the E-Mn(VII) process owing to the catalytic effect of MnO 2 on Mn(VII) oxidation. This was confirmed by the observation that (i) the E-Mn(VII) process showed a similar pH-dependent oxidation trend to that of MnO 2 catalytic oxidation of Mn(VII) (i.e., the reactivity was much stronger at lower pH); and (ii) the addition of MnO 2 prepared ex situ had a significant enhancing effect on DCF oxidation by the E-Mn(VII) process. Moreover, the possible contribution of reactive manganese intermediates such as soluble free Mn(III), Mn(VI), and Mn(V) was ruled out by the results of the probe experiments, UV−visible spectrophotometry, and examining the reactivity of Mn(III) complexes prepared ex situ. Also, the results of radical scavenging experiments indicated the negligible contribution of HO•. Furthermore, for the practical application of the E-Mn(VII) process in water decontamination, suitable operating parameters (e.g., a moderate potential and relatively lower pH) should be determined to avoid the fast loss of Mn(VII) and the electrical energy consumption. Overall, this work brings new insights into the reaction mechanism of the E-Mn(VII) process as well as proposes an efficient, sustainable, and feasible strategy for water and wastewater treatment.

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Highly efficient electro-peroxone enhanced by oxygen-doped carbon nanotubes with triple role of in-situ H2O2 generation, activation and catalytic ozonation

Cited by 28 publications

References 66 publications

Defect- and oxygen-rich nanocarbon derived from solution plasma for bifunctional catalytic activity of oxygen reduction and evolution reactions

Defect- and oxygen-rich nanocarbon derived from solution plasma for bifunctional catalytic activity of oxygen reduction and evolution reactions

Peroxymonosulfate-Based Electrochemical Advanced Oxidation: Complication by Oxygen Reduction Reaction

Enhanced Degradation of Diclofenac by Electro-Activated Permanganate: A Critical Role of In Situ Formed H₂O₂

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Highly efficient electro-peroxone enhanced by oxygen-doped carbon nanotubes with triple role of in-situ H2O2 generation, activation and catalytic ozonation

Cited by 28 publications

References 66 publications

Defect- and oxygen-rich nanocarbon derived from solution plasma for bifunctional catalytic activity of oxygen reduction and evolution reactions

Defect- and oxygen-rich nanocarbon derived from solution plasma for bifunctional catalytic activity of oxygen reduction and evolution reactions

Peroxymonosulfate-Based Electrochemical Advanced Oxidation: Complication by Oxygen Reduction Reaction

Enhanced Degradation of Diclofenac by Electro-Activated Permanganate: A Critical Role of In Situ Formed H2O2

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Product

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Enhanced Degradation of Diclofenac by Electro-Activated Permanganate: A Critical Role of In Situ Formed H₂O₂