A comparison of SMX degradation by persulfate activated with different nanocarbons: Kinetics, transformation pathways, and toxicity

Peng, Yanhua; Xie, Guansheng; Shao, Ping; Ren, Wei; Li, Mengling; Hu, Yu‐Feng; Yang, Liming; Shi, Hui; Luo, Xubiao

doi:10.1016/j.apcatb.2022.121345

Cited by 96 publications

(14 citation statements)

References 45 publications

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“…Nitrogen-coordinated metal atoms doped in two-dimensional graphite exhibit remarkable activity and stability. , Even the surface structure and defects of graphite can become sites for activating PMS. ,,, The coordination number of Co plays a crucial role in adsorption . Yin et al prepared the coordination structures of two cobalt single-atom catalysts (Co–N 4 and Co–N 3 ).…”

Section: Theoretical Calculation Of Pms-aops Involving Cobalt-based H...mentioning

confidence: 99%

Current Mechanism of Peroxymonosulfate Activation by Cobalt-Based Heterogeneous Catalysts in Degrading Organic Compounds

et al. 2023

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Persulfate based advanced oxidation processes (PS-AOPs) have been regarded as a mainstream degradation technology of organic compounds due to their high efficiency in wastewater treatment. In particular, peroxymonosulfate (PMS) has a unique structure and chemical properties, which can be efficiently activated by Co-based catalysts to produce active species with a high oxidation potential. These active species usually determine the subsequent degradation of organic compounds in an efficient process, while the intrinsic reaction mechanism behind this complex process remains unclear and therefore impedes the continual development in this scientific community. Recently, density functional theory (DFT) calculations have emerged as a powerful means to identify the electronic properties and distinguish energy changes in the PMS activation system. With the assistance of this quantum calculation, increasing investigations have been conducted focusing on explaining the phenomenon that occurred in experiments. However, these calculations mainly contributed in part to the reaction mechanism of PMS activation by Co-based catalysts and sometimes even differ from each other, lacking a comprehensive summary based on DFT calculation results. In this review, we introduce the main uses of DFT in the catalytic activation of PMS, provide recent application of calculation examples of Co-based heterogeneous catalysts with different structures, and then discuss the mechanism of PMS activation in detail. Finally, the research results of the DFT method in this field are summarized, and the future research focus and challenges are put forward, which is conducive to guiding the practical design of Co-based catalysts and further application of PS-AOPs in creating value products.

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Section: Theoretical Calculation Of Pms-aops Involving Cobalt-based H...mentioning

confidence: 99%

Current Mechanism of Peroxymonosulfate Activation by Cobalt-Based Heterogeneous Catalysts in Degrading Organic Compounds

et al. 2023

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“…CNTs (carbon nanotubes) consist of sp 2 -conjugated carbon atoms, the defects of which serve as significant active sites and play the part of the carrier electron transmission. The ketone group on carbon nanotubes has a couple of electrons that offer one electron to PMS to form SO 4 − · while it is also proposed that ND (nanodiamond) in the tetrahedral has a distinctive sp 3 hybridization feature in the tetrahedral group and the carbonyl group on the surface of ND significantly contributes to PMS activation [ 160 ]. The use of MWCNTs (multi-walled carbon nanotubes) and GR (graphite) anodes for electrochemical activation of PMS indicates that electrolysis may increase the activation sites of carbon materials (e.g., carbonyl group), again verifying the above statement [ 161 ].…”

Section: Metal-free Nanomaterialsmentioning

confidence: 99%

State-of-the-Art on the Sulfate Radical-Advanced Oxidation Coupled with Nanomaterials: Biological and Environmental Applications

Yang

et al. 2022

JFB

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Sulfate radicals (SO4−) play important biological roles in biomedical and environmental engineering, such as antimicrobial, antitumor, and disinfection. Compared with other common free radicals, it has the advantages of a longer half-life and higher oxidation potential, which could bring unexpected effects. These properties have prompted researchers to make great contributions to biology and environmental engineering by exploiting their properties. Peroxymonosulfate (PMS) and peroxydisulfate (PDS) are the main raw materials for SO4− formation. Due to the remarkable progress in nanotechnology, a large number of nanomaterials have been explored that can efficiently activate PMS/PDS, which have been used to generate SO4−·for biological applications. Based on the superior properties and application potential of SO4−, it is of great significance to review its chemical mechanism, biological effect, and application field. Therefore, in this review, we summarize the latest design of nanomaterials that can effectually activate PMS/PDS to create SO4−, including metal-based nanomaterials, metal-free nanomaterials, and nanocomposites. Furthermore, we discuss the underlying mechanism of the activation of PMS/PDS using these nanomaterials and the application of SO4− in the fields of environmental remediation and biomedicine, liberating the application potential of SO4−. Finally, this review provides the existing problems and prospects of nanomaterials being used to generate SO4−· in the future, providing new ideas and possibilities for the development of biomedicine and environmental remediation.

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“…Nonradical reactive species, such as singlet oxygen ( 1 O 2 ), catalyst-activated persulfate (Cat-PS*) complexes, and high-valent metal-oxo complexes, are able to selectively attack electron-rich organic pollutants even in complicated water matrices. − Generally, the selective oxidation process mainly depends on the electron nature of organics and nonradical reactive species, which can accurately determine the direction and extent of nonradical oxidation. Specially, the electron-donating abilities of organics are determined by the electronic parameters, such as the Hammett constant (σ), , ionization potential (IP), one-electron oxidation potential ( E ox ), − and energy of the highest occupied molecular orbital ( E HOMO ). , Based on the results of quantitative structure–activity relationships (QSARs), organics with a stronger electron-releasing group (lower IP/ E ox /σ or higher E HOMO ) are removed by the nonradical reactive species at a faster oxidation rate, while the electron-withdrawing organics are refractory under the attack of the nonradical reactive species. − Thus, the threshold for selective oxidation of reactive species can be calculated semiquantitatively after the survey of kinetic experiments and theoretical calculations. Our previous studies found that the reduction potential of Cat-PS* complexes and the oxidation potential of organics are critical in regulating the thermodynamic feasibility of the carbon-based electron-transfer pathway (ETP). , Specifically, the thermodynamic prerequisite for initiating ETP is that the reduction potential of complexes surpasses the oxidation potential of organics.…”

Section: Introductionmentioning

confidence: 99%

Thermodynamic and Kinetic Behaviors of Persulfate-Based Electron-Transfer Regime in Carbocatalysis

Peng,

Zhang,

Ren

et al. 2023

Environ. Sci. Technol.

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A carbon-based advanced oxidation process is featured for the nonradical electron-transfer pathway (ETP) from electron-donating organic compounds to activated persulfate complexes, enabling it as a green technology for the selective oxidation of organic pollutants in complex water environments. However, the thermodynamic and kinetic behaviors of the nonradical electron-transfer regime had been ambiguous due to a neglect of the influence of pH on the mechanisms. In this study, three kinds of organic pollutants were divided in the carbon-based ETP regime: (i) physio-adsorption, (ii) adsorption-dominated ETP (oxidation rate slightly surpasses adsorption rate), and (iii) oxidation-dominated ETP (oxidation rate outpaces the adsorption rate). The differential kinetic behaviors were attributed to the physicochemical properties of the organic pollutants. For example, the hydrophobicity, molecular radius, and positive electrostatic potential controlled the mass-transfer process of the adsorption stage of the reactants (peroxydisulfate (PDS) and organics). Meanwhile, other descriptors, including the Fukui index, oxidation potential, and electron cloud density regulated the electrontransfer processes and thus the kinetics of oxidation. Most importantly, the oxidation pathways of these organic pollutants could be altered by adjusting the water chemistry. This study reveals the principles for developing efficient nonradical systems to selectively remove and recycle organic pollutants in wastewater.

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A comparison of SMX degradation by persulfate activated with different nanocarbons: Kinetics, transformation pathways, and toxicity

Cited by 96 publications

References 45 publications

Current Mechanism of Peroxymonosulfate Activation by Cobalt-Based Heterogeneous Catalysts in Degrading Organic Compounds

Current Mechanism of Peroxymonosulfate Activation by Cobalt-Based Heterogeneous Catalysts in Degrading Organic Compounds

State-of-the-Art on the Sulfate Radical-Advanced Oxidation Coupled with Nanomaterials: Biological and Environmental Applications

Thermodynamic and Kinetic Behaviors of Persulfate-Based Electron-Transfer Regime in Carbocatalysis

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