Radical chemistry of diethyl phthalate oxidation via UV/peroxymonosulfate process: Roles of primary and secondary radicals

Lei, Yu; Lü, Jun; Zhu, Mengyu; Xie, Jingjing; Peng, Shuchuan; Zhu, Chengzhu

doi:10.1016/j.cej.2019.122339

Cited by 69 publications

(33 citation statements)

References 66 publications

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“…Chlorine atoms (Cl • ) and dichlorine radical anions (Cl 2 •– ) impact photochemical processes in radical-mediated advanced oxidation processes (AOPs) for water and wastewater treatment and in natural waters. − Cl • and Cl 2 •– can be generated from the reactions of sulfate radicals with chloride ions (Cl – ), the electrochemical treatment of high salinity wastewater, or the photolysis of free chlorine. , Cl • (E 0 = 2.55 V vs SHE) and Cl 2 •– (E 0 = 2.13 V vs SHE) are highly reactive in transforming a variety group of organic micropollutants. ,, Our research group has determined the reactivity of dozens of trace organic contaminants (TrOCs) toward Cl • ( k = (3.10 ± 0.50) × 10 9 to (4.08 ± 0.24) × 10 10 M –1 s –1 ) and Cl 2 •– ( k = < 1 × 10 6 to (2.78 ± 0.16) × 10 9 M –1 s –1 ) . The transformation rates of TrOCs are greatly reduced in the presence of dissolved organic matter (DOM), which is ubiquitous in water and wastewater and significantly scavenges radicals. ,− However, few studies have reported the reaction rates between Cl • or Cl 2 •– and DOM, especially DOM from different sources.…”

Section: Introductionmentioning

confidence: 99%

Reactivity of Chlorine Radicals (Cl^• and Cl₂^•–) with Dissolved Organic Matter and the Formation of Chlorinated Byproducts

Lei

Westerhoff

et al. 2020

Environ. Sci. Technol.

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164

132

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Chlorine radicals, including Cl• and Cl2 •–, can be produced in sunlight waters (rivers, oceans, and lakes) or water treatment processes (e.g., electrochemical and advanced oxidation processes). Dissolved organic matter (DOM) is a major reactant with, or a scavenger of, Cl• and Cl2 •– in water, but limited quantitative information exists regarding the influence of DOM structure on its reactivity with Cl• and Cl2 •–. This study aimed at quantifying the reaction rates and the formation of chlorinated organic byproducts produced from Cl• and Cl2 •– reactions with DOM. Laser flash photolysis experiments were conducted to quantify the second-order reaction rate constants of 19 DOM isolates with Cl• (k DOM–Cl•) and Cl2 •– (k DOM–Cl2•–), and compare those with the hydroxyl radical rate constants (k DOM–•OH). The values for k DOM–Cl• ((3.71 ± 0.34) × 108 to (1.52 ± 1.56) × 109 MC –1 s–1) were orders of magnitude greater than the k DOM–Cl2•– values ((4.60 ± 0.90) × 106 to (3.57 ± 0.53) × 107 MC –1 s–1). k DOM–Cl• negatively correlated with the weight-averaged molecular weight (M W) due to the diffusion-controlled reactions. DOM with high aromaticity and total antioxidant capacity tended to react faster with Cl2 •–. During the same experiments, we also monitored the formation of chlorinated byproducts through the evolution of total organic chlorine (TOCl) as a function of chlorine radical oxidant exposure (CT value). Maximum TOCl occurred at a CT of 4–8 × 10–12 M·s for Cl• and 1.1–2.2 × 10–10 M·s for Cl2 •–. These results signify the importance of DOM in scavenging chlorine radicals and the potential risks of producing chlorinated byproducts of unknown toxicity.

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Section: Introductionmentioning

confidence: 99%

Reactivity of Chlorine Radicals (Cl^• and Cl₂^•–) with Dissolved Organic Matter and the Formation of Chlorinated Byproducts

Lei

Westerhoff

et al. 2020

Environ. Sci. Technol.

Self Cite

164

132

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“…Coexisting inorganic ions in water bodies affect the oxidation degradation process of the target pollutants because they have significant impacts on the speciation concentration of reactive oxidants (Lei et al, 2020;Xu et al, 2020 , HCO 3 − and HPO 4 2− were used to carry out the experiments. The experimental results are depicted in Fig.…”

Section: Effects Of Coexisting Inorganic Ions On Smp Degradationmentioning

confidence: 99%

Photodegradation of Sulfamethoxypyridazine in UV/Co(II)/Peroxymonosulfate System: Kinetics, Influencing Factors, Degradation Pathways, and Toxicity Assessment

Zeng

Sun

Meng

et al. 2021

Water Air Soil Pollut

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effect. Radical scavenger experiments indicated that hydroxyl radicals (HO • ) are prevailing active species responsible for SMP removal in UV/Co(II)/PMS system. The degradation of SMP in UV/Co(II)/PMS system was accomplished mainly by hydroxylation of the aromatic ring, extrusion of SO 2 , oxidation of NH 2 group, and N − S bond cleavage. Eight intermediates for SMP degradation were identified, and their toxicities to aquatic organisms were predicted by using the ECOSAR program based on the structure − activity relationships (SARs), which suggested that the chronic toxicities of SMP and its degradation intermediates are more significant than their acute toxicities. The present research indicates that UV/Co(II)/ PMS system is applicable for SMP degradation in aqueous solutions and may be helpful to understand the transformation behavior of SAs.

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“…Over the past decades, advanced oxidation processes (AOPs) using peroxymonosulfate (PMS), referred to as PMS–AOPs, have received increasing attention for the abatement of contaminants in water. − The current understanding of the degradation of contaminants in PMS–AOPs is either the attack of reactive species generated from the activation of PMS or the mediated electron transfer between PMS and the contaminant depending on the catalysts/methods utilized . The reactive species generated in PMS–AOPs mainly include free radicals ( i.e.…”

Section: Introductionmentioning

confidence: 99%

Are Free Radicals the Primary Reactive Species in Co(II)-Mediated Activation of Peroxymonosulfate? New Evidence for the Role of the Co(II)–Peroxymonosulfate Complex

Zhao

Qian

et al. 2021

Environ. Sci. Technol.

165

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The catalytic activation of peroxymonosulfate (PMS) is under intensive investigation with potentials as an alternative advanced oxidation process (AOP) in wastewater treatment. Among all catalysts examined, Co(II) exhibits the highest reactivity for the activation of PMS, following the conventional Fenton-like mechanism, in which free radicals (i.e., sulfate radicals and hydroxyl radicals) are reckoned as the reactive species. Herein, we report that the primary reactive species (PRS) is proposed to be a Co(II)−PMS complex (Co(II)−OOSO 3 − ), while free radicals and Co(III) species act as the secondary reactive species (SRS) that play a minor role in the Co(II)/PMS process. This Co(II)−OOSO 3 − exhibits several intriguing properties including ability to conduct both one-electrontransfer and oxygen-atom-transfer reactions with selected molecules, both nucleophilic and electrophilic in nature, and strongly pHdependent reactivity. This study provides novel insights into the chemical nature of the Co(II)-catalyzed PMS activation process.

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Radical chemistry of diethyl phthalate oxidation via UV/peroxymonosulfate process: Roles of primary and secondary radicals

Cited by 69 publications

References 66 publications

Reactivity of Chlorine Radicals (Cl^• and Cl₂^•–) with Dissolved Organic Matter and the Formation of Chlorinated Byproducts

Reactivity of Chlorine Radicals (Cl^• and Cl₂^•–) with Dissolved Organic Matter and the Formation of Chlorinated Byproducts

Photodegradation of Sulfamethoxypyridazine in UV/Co(II)/Peroxymonosulfate System: Kinetics, Influencing Factors, Degradation Pathways, and Toxicity Assessment

Are Free Radicals the Primary Reactive Species in Co(II)-Mediated Activation of Peroxymonosulfate? New Evidence for the Role of the Co(II)–Peroxymonosulfate Complex

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Radical chemistry of diethyl phthalate oxidation via UV/peroxymonosulfate process: Roles of primary and secondary radicals

Cited by 69 publications

References 66 publications

Reactivity of Chlorine Radicals (Cl• and Cl2•–) with Dissolved Organic Matter and the Formation of Chlorinated Byproducts

Reactivity of Chlorine Radicals (Cl• and Cl2•–) with Dissolved Organic Matter and the Formation of Chlorinated Byproducts

Photodegradation of Sulfamethoxypyridazine in UV/Co(II)/Peroxymonosulfate System: Kinetics, Influencing Factors, Degradation Pathways, and Toxicity Assessment

Are Free Radicals the Primary Reactive Species in Co(II)-Mediated Activation of Peroxymonosulfate? New Evidence for the Role of the Co(II)–Peroxymonosulfate Complex

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Reactivity of Chlorine Radicals (Cl^• and Cl₂^•–) with Dissolved Organic Matter and the Formation of Chlorinated Byproducts

Reactivity of Chlorine Radicals (Cl^• and Cl₂^•–) with Dissolved Organic Matter and the Formation of Chlorinated Byproducts