Effect of phosphate on peroxymonosulfate activation: Accelerating generation of sulfate radical and underlying mechanism

Duan, Pijun; Liu, Xinning; Liu, Binhua; Akram, Muhammad; Li, Yanwei; Pan, Jingwen; Yue, Qinyan

doi:10.1016/j.apcatb.2021.120532

Cited by 189 publications

(36 citation statements)

References 57 publications

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“…8,9 Single-atom catalysts (SACs) inherit the advantages of both homogeneous and heterogeneous catalysts, maximize the atomic efficiency by anchoring individual metal atoms on the substrate for the maximum exposure to the reactants, and provide a family of well-defined molecular structures for mechanistic studies. 4,10,11 Nevertheless, the mechanisms of carbon-based catalysts in persulfate chemistry are controversial because of the different metal centers, 12 coordination configurations, 13 as well as the substrates for SAC confining (e.g., carbon matrixes 14,15 and metal substrates 16,17 ). On the whole, SACs normally activate PMS via nonradical pathways [electron-transfer pathway (ETP), high-valent metal-oxo species, and 1 O 2 ], radical oxidation (SO 4…”

Section: Introductionmentioning

confidence: 99%

Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N₄–C Intensified Radical and Nonradical Pathways

Yang

Hou

Zhang

et al. 2022

Environ. Sci. Technol.

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190

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Single-atom catalysts (SACs)-based peroxymonosulfate (PMS) systems are highly selective to the type of organic pollutants while the mechanisms remain ambiguous. In this work, we carried out experimental and theoretical investigations to reveal the origins of selectivity of radical and nonradical pathways in a designated Co−N 4 −C/PMS system. Two typical pollutants [bisphenol A (BPA) and metronidazole (MNZ)] with different molecular structures were employed for comparison. We found that radical oxidation (SO 4•− and HO • ) and nonradical electrontransfer pathway (ETP) co-existed in the Co−N 4 −C/PMS system. Pollutants (e.g., MNZ) with a high redox potential were degraded primarily by free radicals rather than ETP, while the oxidization of low-redox pollutants (e.g., BPA) was dominated by ETP at the surface region of Co−N 4 −C which overwhelmed the contributions of radicals in the homogeneous phase. Intriguingly, the contributions of radical and nonradical pathways could be manipulated by the PMS loading, which simultaneously increased the radical population and elevated the oxidation potential of Co−N 4 −C-PMS* complexes in ETP. Findings from this work will unravel the mysterious selective behavior of the SACs/PMS systems in the oxidation of different micropollutants.

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Section: Introductionmentioning

confidence: 99%

Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N₄–C Intensified Radical and Nonradical Pathways

Yang

Hou

Zhang

et al. 2022

Environ. Sci. Technol.

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190

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“…improved the removal of the material, which is due to its ability to activate PMS. 51 In previous studies, it was reported that CO 3 2À is a scavenger of O 2 À , which can react with O 2 À to produce CO 3 À . 52,53 CO 3 À is more reactive than O 2 À and 1 O 2 , and therefore it can improve the removal efficiency of tetracycline.…”

Section: àmentioning

confidence: 99%

Iron pyrophosphate doped carbon nanocomposite for tetracycline degradation by activation of peroxymonosulfate

Zhang

et al. 2022

New J. Chem.

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“…Authors have indicated that a pseudo-first order kinetic model (Equation ( 9)) can be used to describe the organic pollutants rate of degradation under the use of different TAOs, including those based on PS activation (Pirsaheb et al 2020;Duan et al 2021;Hadi et al 2021). The inset graph in Figure 8 presents the results obtained after evaluating the relationship between the initial reaction rate and the initial CPX concentration and evidenced that in effect the proposed model fits the experimental C 0 is the pollutant initial concentration at the time t and k is the reaction rate constant.…”

Section: Cpx Degradation Kinetics: Effect Of Pollutant Initial Concentrationmentioning

confidence: 99%

Cephalexin removal by persulfate activation using simulated sunlight and ferrous ions

Perdomo

Minota

Zúñiga-Benítez

et al. 2021

Water Science and Technology

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This study presents the main results related to the use of activated persulfate (PS) in the elimination of the beta-lactam antibiotic cephalexin (CPX). Experiments were done using K2S2O8 and simulated sunlight. A face-centered central composite experimental design was used to analyze the effects of the solution pH and the PS concentration on the reaction, and to determine the optimized conditions that favor the CPX elimination. The results indicated that the removal of CPX is promoted by an acidic pH and under the higher evaluated PS dose (7.5 mg L−1). CPX total removal was achieved in 30 min. The analysis of the effect of the pollutant initial concentration indicated that a pseudo-first order kinetic model can be used to describe the reaction. Likewise, the use of Fe2+ ions for PS activation (in the dark) was evaluated and allowed to establish that a higher concentration of ions favors the pollutant removal. Control tests and under the presence of scavenger agents indicated that both HO• and SO4−• radicals would be present in the solution and promote the CPX elimination. The assessment of the solution dissolved organic carbon, nitrates and sulfates was also carried out, and indicated that a portion of the organic matter was mineralized.

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Effect of phosphate on peroxymonosulfate activation: Accelerating generation of sulfate radical and underlying mechanism

Cited by 189 publications

References 57 publications

Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N₄–C Intensified Radical and Nonradical Pathways

Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N₄–C Intensified Radical and Nonradical Pathways

Iron pyrophosphate doped carbon nanocomposite for tetracycline degradation by activation of peroxymonosulfate

Cephalexin removal by persulfate activation using simulated sunlight and ferrous ions

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Effect of phosphate on peroxymonosulfate activation: Accelerating generation of sulfate radical and underlying mechanism

Cited by 189 publications

References 57 publications

Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N4–C Intensified Radical and Nonradical Pathways

Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N4–C Intensified Radical and Nonradical Pathways

Iron pyrophosphate doped carbon nanocomposite for tetracycline degradation by activation of peroxymonosulfate

Cephalexin removal by persulfate activation using simulated sunlight and ferrous ions

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Product

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Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N₄–C Intensified Radical and Nonradical Pathways

Unveiling the Origins of Selective Oxidation in Single-Atom Catalysis via Co–N₄–C Intensified Radical and Nonradical Pathways