Factors and mechanisms that influence the reactivity of trivalent copper: A novel oxidant for selective degradation of antibiotics

Feng, Yong; Qing, Weihua; Kong, Lingjun; Li, Hailong; Wu, Deli; Fan, Yiting; Lee, Po‐Heng; Shih, Kaimin

doi:10.1016/j.watres.2018.10.090

Cited by 78 publications

(33 citation statements)

References 46 publications

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“…51 It is known that it readily reacts with phenols and benzoic acid (BA) but hardly oxidizes nitrobenzene (NB), which is different from • OH. 8,52,53 Here, NB and BA were degraded by 30 and 35%, respectively, within 15 Since Cu(III) has an equilibrium shift with • OH, 52,54 we suppose that the secondary oxidant is • OH. It is known that the DMPO−OH signal of the EPR spectra alone cannot be used to differentiate • OH and Cu(III).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Cu(III), with a reducing potential of 1.57–2.3 V, is a selective oxidant . It is known that it readily reacts with phenols and benzoic acid (BA) but hardly oxidizes nitrobenzene (NB), which is different from • OH. ,, Here, NB and BA were degraded by 30 and 35%, respectively, within 15 min of Cu(II)/PMS oxidation. The NB degradation was almost completely inhibited by 10 mM of t -BuOH (Figure S6b, SI), a possible signature of • OH oxidation, while the BA degradation was only partially inhibited (Figure S6c, SI), indicating the major contribution of Cu(III) oxidation.…”

Section: Resultsmentioning

confidence: 99%

“…Since Cu(III) has an equilibrium shift with • OH, , we suppose that the secondary oxidant is • OH. It is known that the DMPO–OH signal of the EPR spectra alone cannot be used to differentiate • OH and Cu(III) .…”

Section: Resultsmentioning

confidence: 99%

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Trace Cupric Species Triggered Decomposition of Peroxymonosulfate and Degradation of Organic Pollutants: Cu(III) Being the Primary and Selective Intermediate Oxidant

Wang

Jiang

et al. 2020

Environ. Sci. Technol.

336

145

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Activation of persulfates to degrade refractory organic pollutants is currently a hot topic of advanced oxidation. Developing simple and effective activation approaches is crucial for the practical application of persulfates. We report in this research that trace cupric species (Cu(II) in several μM) can efficiently trigger peroxymonosulfate (PMS) oxidation of various organic pollutants under slightly alkaline conditions. The intermediate oxidant dominating this process was investigated with electron paramagnetic resonance (EPR), chemical probing, and in situ Raman spectroscopy. Unlike conventional PMS activation, which generates sulfate radical, hydroxyl radical, or singlet oxygen as major oxidants, Cu(III) was confirmed to be the primary and selective intermediate oxidant during the Cu(II)/PMS oxidation. Hydroxyl radical is the secondary intermediate oxidant formed from the reaction of Cu(III) with OH − . Hybrid oxidation by the two oxidants imparts Cu(II)/PMS with high efficiency in the degradation of a series of pollutants. The results of this work suggest that, with no need of introducing complex catalysts, trace Cu(II) inherent in or artificially introduced to some water or wastewater can effectively trigger PMS oxidation of organic pollutants.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

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Trace Cupric Species Triggered Decomposition of Peroxymonosulfate and Degradation of Organic Pollutants: Cu(III) Being the Primary and Selective Intermediate Oxidant

Wang

Jiang

et al. 2020

Environ. Sci. Technol.

336

145

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“…For both processes, in which the degradation rate was in the order of 0.012 min −1 , although the generation of hydroxyl radicals increased the reaction rate slightly, an increase in the degradation rate was not implied. This may be because hydroxyl radicals (HO ● ), being highly energetic and not very selective oxidants, can be captured by other species in the reaction medium that are susceptible to oxidation [ 33 ]. Among these species would be the chloride ions released as the pesticide is broken down, which would capture part of the hydroxyl radicals generated, thus reducing the degradation rate of the process.…”

Section: Resultsmentioning

confidence: 99%

Comparative Effect of UV, UV/H2O2 and UV/H2O2/Fe on Terbuthylazine Degradation in Natural and Ultrapure Water

et al. 2022

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Different advanced oxidation processes (AOPs) (ultraviolet radiation, hydrogen peroxide photolysis and photo-Fenton) were applied to test the degradation of terbuthylazine in three types of water: (a) ultrapure water, (b) surface water from the Gaditana area (Los Hurones reservoir, Cádiz, Spain) and (c) groundwater from the Tempul spring in Jerez de la Frontera (Cádiz, Spain). The experiments were carried out on a laboratory scale, using two different types of reactors, batch and semi-continuous. In batch reactors, the most efficient process for the experiments carried out with both ultrapure water and underground groundwater was ultraviolet radiation, whereas for surface water from the Gaditana area, the process that obtained the best results was the photolysis of hydrogen peroxide with 2.5 mg L−1 of H2O2. In semi-continuous reactors, the most efficient process was the photolysis of hydrogen peroxide with 2.5 mg L−1 of H2O2 for all the matrices studied. In both types of reactors, terbuthylazine degradation percentages higher than 90% were achieved; the main difference was in the reaction time, which varied from minutes in the batch reactor to seconds in the semi-continuous reactor. In all the applied AOPs, N-terbutyl-6-hydroxy-N′ethyl-1,3,5-triazine-2,4-diamine (TBA-212) was generated as a reaction intermediate.

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“…To substantiate the capability of Cu(III) for the oxidative degradation of HEDP, the standard sample of Cu(III) was prepared and verified via multiple characterization methods (Text S6 and Figure S13). A complete oxidation of HEDP (0.10 mM) by the standard Cu(III) was realized within 3 min.…”

Section: Results and Discussionmentioning

confidence: 99%

Self-Enhanced Selective Oxidation of Phosphonate into Phosphate by Cu(II)/H₂O₂: Performance, Mechanism, and Validation

Sun

Shan

Yang

et al. 2021

Environ. Sci. Technol.

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Phosphonate is an important category of highly soluble organophosphorus in contaminated waters, and its oxidative transformation into phosphate is usually a prerequisite step to achieve the in-depth removal of the total phosphorus. Currently, selective oxidation of phosphonate into phosphate is urgently desired as conventional advanced oxidation processes suffer from severe matrix interferences. Herein, we employed 1-hydroxyethylidene-1,1-diphosphonic acid (HEDP) as a model phosphonate and demonstrated its efficient and selective oxidation by the Cu(II)/H2O2 process at alkaline pH. In the presence of trace Cu(II) (0.020 mM), 90.8% of HEDP (0.10 mM) was converted to phosphate by H2O2 in 30 min at pH 9.5, whereas negligible conversion was observed by UV/H2O2 or a Fenton reaction (pH = 3.0). The oxidation of HEDP by Cu(II)/H2O2 was insignificantly affected by natural organic matters (10.0 mg TOC/L) and various anions including chloride, sulfate, and nitrate (10.0 mM). The complexation of Cu(II) with HEDP coupling Cu(III) produced in situ enabled an intramolecular electron transfer process, which features high selective oxidation. Selective degradation of HEDP was further validated by adding stoichiometric H2O2 into an industrial effluent, where the existing Cu(II) could serve as the catalyst. This study also provides a successful case to trigger selective oxidation of trace pollutants of concern upon synergizing with the nature of the contaminated water.

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Factors and mechanisms that influence the reactivity of trivalent copper: A novel oxidant for selective degradation of antibiotics

Cited by 78 publications

References 46 publications

Trace Cupric Species Triggered Decomposition of Peroxymonosulfate and Degradation of Organic Pollutants: Cu(III) Being the Primary and Selective Intermediate Oxidant

Trace Cupric Species Triggered Decomposition of Peroxymonosulfate and Degradation of Organic Pollutants: Cu(III) Being the Primary and Selective Intermediate Oxidant

Comparative Effect of UV, UV/H2O2 and UV/H2O2/Fe on Terbuthylazine Degradation in Natural and Ultrapure Water

Self-Enhanced Selective Oxidation of Phosphonate into Phosphate by Cu(II)/H₂O₂: Performance, Mechanism, and Validation

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Factors and mechanisms that influence the reactivity of trivalent copper: A novel oxidant for selective degradation of antibiotics

Cited by 78 publications

References 46 publications

Trace Cupric Species Triggered Decomposition of Peroxymonosulfate and Degradation of Organic Pollutants: Cu(III) Being the Primary and Selective Intermediate Oxidant

Trace Cupric Species Triggered Decomposition of Peroxymonosulfate and Degradation of Organic Pollutants: Cu(III) Being the Primary and Selective Intermediate Oxidant

Comparative Effect of UV, UV/H2O2 and UV/H2O2/Fe on Terbuthylazine Degradation in Natural and Ultrapure Water

Self-Enhanced Selective Oxidation of Phosphonate into Phosphate by Cu(II)/H2O2: Performance, Mechanism, and Validation

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Product

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Self-Enhanced Selective Oxidation of Phosphonate into Phosphate by Cu(II)/H₂O₂: Performance, Mechanism, and Validation