Application of peroxymonosulfate and its activation methods for degradation of environmental organic pollutants: Review
TL;DR: A literature review on environmental application of peroxymonosulfate (PMS) in degradation of contaminants to clarify the performance of PMS is carried out in this paper, which describes the PMS usage in remediation of environmental pollutants with focus on the different methods of activation and the effect of main operational parameters on PMS-based processes.
About: This article is published in Chemical Engineering Journal.The article was published on 2017-02-15. It has received 1650 citations till now.
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TL;DR: Sulfate radical-based advanced oxidation processes (AOPs) have received increasing attention in recent years due to their high capability and adaptability for the degradation of emerging contaminants as mentioned in this paper.
2,267 citations
TL;DR: This Critical Review comparatively examines the activation mechanisms of peroxymonosulfate and peroxydisulfates and the formation pathways of oxidizing species and the impacts of water parameters and constituents such as pH, background organic matter, halide, phosphate, and carbonate on persulfate-driven chemistry.
Abstract: Reports that promote persulfate-based advanced oxidation process (AOP) as a viable alternative to hydrogen peroxide-based processes have been rapidly accumulating in recent water treatment literature. Various strategies to activate peroxide bonds in persulfate precursors have been proposed and the capacity to degrade a wide range of organic pollutants has been demonstrated. Compared to traditional AOPs in which hydroxyl radical serves as the main oxidant, persulfate-based AOPs have been claimed to involve different in situ generated oxidants such as sulfate radical and singlet oxygen as well as nonradical oxidation pathways. However, there exist controversial observations and interpretations around some of these claims, challenging robust scientific progress of this technology toward practical use. This Critical Review comparatively examines the activation mechanisms of peroxymonosulfate and peroxydisulfate and the formation pathways of oxidizing species. Properties of the main oxidizing species are scrutinized and the role of singlet oxygen is debated. In addition, the impacts of water parameters and constituents such as pH, background organic matter, halide, phosphate, and carbonate on persulfate-driven chemistry are discussed. The opportunity for niche applications is also presented, emphasizing the need for parallel efforts to remove currently prevalent knowledge roadblocks.
1,412 citations
TL;DR: In this article, the state of the art of AOPs exclusively at alkaline pH, the type of compounds and effluents effectively degraded, the influence of pH on the efficiency of the processes, economic evaluation and degradation pathways were presented.
774 citations
TL;DR: A new routine for effective PMS activation by heterogeneous iron-complexed catalysts to efficiently degrade organic contaminants via nonradical pathway is provided.
Abstract: Herein, we proposed a new peroxymonosulfate (PMS) activation system employing the Fe(III) doped g-C3N4 (CNF) as catalyst. Quite different from traditional sulfate radical-based advanced oxidation processes (SR-AOPs), the PMS/CNF system was capable of selectively degrading phenolic compounds (e.g., p-chlorophenol, 4-CP) in a wide pH range (3–9) via nonradical pathway. The generated singlet oxygen (1O2) in the PMS/CNF3 (3.46 wt % Fe) system played negligible role in removing 4-CP, and high-valent iron-oxo species fixated in the nitrogen pots of g-C3N4 (≡FeV═O) was proposed as the dominant reactive species by using dimethyl sulfoxide as a probe compound. The mechanism was hypothesized that PMS was first bound to the Fe(III)-N moieties to generate ≡FeV═O, which effectively reacted with 4-CP via electron transfer. GC-MS analysis indicated that 4-chlorocatechol and 1,4-benzoquinone were the major intermediates, which could be further degraded to carboxylates. The kinetic results suggested that the formation of ...
611 citations
TL;DR: In this paper, the state of the art in Sulfate radical-based advanced Oxidation processes (SR-AOPs) application for industrial wastewater treatment is presented, and an integrated presentation of the dominant pathways towards IWW decontamination is discussed.
609 citations
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TL;DR: In this paper, the complex mechanisms of Fenton and Fenton-like reactions and the important factors influencing these reactions, from both a fundamental and practical perspective, in applications to water and soil treatment, are discussed.
Abstract: Fenton chemistry encompasses reactions of hydrogen peroxide in the presence of iron to generate highly reactive species such as the hydroxyl radical and possibly others. In this review, the complex mechanisms of Fenton and Fenton-like reactions and the important factors influencing these reactions, from both a fundamental and practical perspective, in applications to water and soil treatment, are discussed. The review covers modified versions including the photoassisted Fenton reaction, use of chelated iron, electro-Fenton reactions, and Fenton reactions using heterogeneous catalysts. Sections are devoted to nonclassical pathways, by-products, kinetics and process modeling, experimental design methodology, soil and aquifer treatment, use of Fenton in combination with other advanced oxidation processes or biodegradation, economic comparison with other advanced oxidation processes, and case studies.
3,218 citations
TL;DR: Electro-Fenton (EF) Process 6585 4.2.1.
Abstract: 2.2. Fenton’s Chemistry 6575 2.2.1. Origins 6575 2.2.2. Fenton Process 6575 2.3. Photo-Fenton Process 6577 3. H2O2 Electrogeneration for Water Treatment 6577 3.1. Fundamentals 6578 3.2. Cathode Materials 6579 3.3. Divided Cells 6580 3.4. Undivided Cells 6583 4. Electro-Fenton (EF) Process 6585 4.1. Origins 6585 4.2. Fundamentals of EF for Water Remediation 6586 4.2.1. Cell Configuration 6586 4.2.2. Cathodic Fe2+ Regeneration 6586 4.2.3. Anodic Generation of Heterogeneous Hydroxyl Radical 6587
2,652 citations
TL;DR: Nine transition metals were tested for the activation of three oxidants and the generation of inorganic radical species such as sulfate, peroxymonosulfate, and hydroxyl radicals to postulate the rate-determining step of the redox reactions taking place when a metal is coupled with an oxidant in aqueous solution.
Abstract: Nine transition metals were tested for the activation of three oxidants and the generation of inorganic radical species such as sulfate, peroxymonosulfate, and hydroxyl radicals. From the 27 combinations, 14 M/Ox couples demonstrated significant reactivity toward transforming a model organic substrate such as 2,4-dichlorophenol and are further discussed here. It was found that Co(II) and Ru(III) are the best metal catalysts for the activation of peroxymonosulfate. As expected on the basis of the Fenton reagent, Fe(III) and Fe(II) were the most efficient transition metals for the activation of hydrogen peroxide. Finally, Ag(I) showed the best results toward activating persulfate. Quenching studies with specific alcohols (tert-butyl alcohol and ethanol) were also performed to identify the primary radical species formed from the reactive M/Ox interactions. The determination of these transient species allowed us to postulate the rate-determining step of the redox reactions taking place when a metal is coupled with an oxidant in aqueous solution. It was found that when Co(II), Ru(III), and Fe(II) interact with peroxymonosulfate, freely diffusible sulfate radicals are the primary species formed. The same was proven for the interaction of Ag(I) with persulfate, but in this case caged or bound to the metal sulfate radicals might be formed as well. The conjunction of Ce(III), Mn(II), and Ni(II) with peroxymonosulfate showed also to generate caged or bound to the metal sulfate radicals. A combination of sulfate and hydroxyl radicals was formed from the conjunction of V(III) with peroxymonosulfate and from Fe(II) with persulfate. Finally, the conjunction of Fe(III), Fe(II), and Ru(III) with hydrogen peroxide led primarily to the generation of hydroxyl radicals. It is also suggested here that the redox behavior of a particular metal in solution cannot be predicted based exclusively on its size and charge. Additional phenomena such as metal hydrolysis as well as complexation with other counterions present in solution might affect the thermodynamics of the overall process and are further discussed here.
2,453 citations
1,930 citations
TL;DR: In this paper, the authors provide a state-of-the-art review on the development in heterogeneous catalysts including single metal, mixed metal, and nonmetal carbon catalysts for organic contaminants removal, with particular focus on peroxymonosulfate (PMS) activation.
Abstract: Sulfate radical-based advanced oxidation processes (SR-AOPs) employing heterogeneous catalysts to generate sulfate radical (SO4 −) from peroxymonosulfate (PMS) and persulfate (PS) have been extensively employed for organic contaminant removal in water. This article aims to provide a state–of–the–art review on the recent development in heterogeneous catalysts including single metal, mixed metal, and nonmetal carbon catalysts for organic contaminants removal, with particular focus on PMS activation. The hybrid heterogeneous catalyst/PMS systems integrated with other advanced oxidation technologies is also discussed. Several strategies for the identification of principal reactive radicals in SO4 −–oxidation systems are evaluated, namely (i) use of chemical probe or spin trapping agent coupled with analytical tools, and (ii) competitive kinetic approach using selective radical scavengers. The main challenges and mitigation strategies pertinent to the SR-AOPs are identified, which include (i) possible formation of oxyanions and disinfection byproducts, and (ii) dealing with sulfate produced and residual PMS. Potential future applications and research direction of SR-AOPs are proposed. These include (i) novel reactor design for heterogeneous catalytic system based on batch or continuous flow (e.g. completely mixed or plug flow) reactor configuration with catalyst recovery, and (ii) catalytic ceramic membrane incorporating SR-AOPs.
1,802 citations