Efficient decontamination of organic pollutants under high salinity conditions by a nonradical peroxymonosulfate activation system

Chen, Fei; Liu, Lianlian; Chen, Jie‐Jie; Li, Wen‐Wei; Chen, You‐Peng; Zhang, Yingjie; Wu, Jindi; Mei, Shu‐Chuan; Yang, Qi; Yu, Han‐Qing

doi:10.1016/j.watres.2020.116799

Cited by 333 publications

(69 citation statements)

References 47 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Chen et al [120] prepared efficient Fe/O co-doped g-C 3 N 4 nanosheet catalyst by a simple calcination method, and the degradation mechanism of the catalyst on organic pollutants was clarified. In contrast to the traditional advanced oxidation technology based on PMS, the activation of PMS is through singlet oxygen and Fe(V)=O double nonradical pathway.…”

Section: Degradation Of Organic Pollutantsmentioning

confidence: 99%

Research Progress and Application of Single-Atom Catalysts: A Review

Wang²,

Liu

et al. 2021

Molecules

View full text Add to dashboard Cite

Due to excellent performance properties such as strong activity and high selectivity, single-atom catalysts have been widely used in various catalytic reactions. Exploring the application of single-atom catalysts and elucidating their reaction mechanism has become a hot area of research. This article first introduces the structure and characteristics of single-atom catalysts, and then reviews recent preparation methods, characterization techniques, and applications of single-atom catalysts, including their application potential in electrochemistry and photocatalytic reactions. Finally, application prospects and future development directions of single-atom catalysts are outlined.

show abstract

Section: Degradation Of Organic Pollutantsmentioning

confidence: 99%

Research Progress and Application of Single-Atom Catalysts: A Review

Wang²,

Liu

et al. 2021

Molecules

View full text Add to dashboard Cite

show abstract

“…Graphitic carbon nitride (g-C 3 N 4 ) is a unique two-dimensional material, which has been extensively explored in recent years for water and wastewater treatment due to its stable structure and cost-effectiveness. − More importantly, the N-rich environment can afford sufficient N atoms to coordinate with various metals (e.g., Fe, Co, Mn, and Cu), significantly accelerating the catalytic property. , Owing to the exceptional redox properties of the centered metal atom, the peroxide can be activated via a unique nonradical pathway. For example, Li et al proposed that PMS can simulate a two-electron conversion of Fe(III) to Fe(V) in Fe(III)-doped g-C 3 N 4 .…”

Section: Introductionmentioning

confidence: 99%

Novel Nonradical Oxidation of Sulfonamide Antibiotics with Co(II)-Doped g-C₃N₄-Activated Peracetic Acid: Role of High-Valent Cobalt–Oxo Species

Liu

Guo

Jia

et al. 2021

Environ. Sci. Technol.

177

View full text Add to dashboard Cite

Herein, we report that Co(II)-doped g-C 3 N 4 can efficiently trigger peracetic acid (PAA) oxidation of various sulfonamides (SAs) in a wide pH range. Quite different from the traditional radical-generating or typical nonradical-involved (i.e., singlet oxygenation and mediated electron transfer) catalytic systems, the PAA activation follows a novel nonradical pathway with unprecedented high-valent cobalt−oxo species [Co(IV)] as the dominant reactive species. Our experiments and density functional theory calculations indicate that the Co atom fixated into the nitrogen pots of g-C 3 N 4 serves as the main active site, enabling dissociation of the adsorbed PAA and conversion of the coordinated Co(II) to Co(IV) via a unique two-electron transfer mechanism. Considering Co(IV) to be highly electrophilic in nature, different substituents (i.e., five-membered and six-membered heterocyclic moieties) on the SAs could affect their nucleophilicity, thus leading to the differences in degradation efficiency and transformation pathway. Also, benefiting from the selective oxidation of Co(IV), the established oxidative system exhibits excellent anti-interference capacity and achieves satisfactory decontamination performance under actual water conditions. This study provides a new nonradical approach to degrade SAs by efficiently activating PAA via heterogeneous cobalt-complexed catalysts. KEYWORDS: peracetic acid, Co(II)-doped g-C 3 N 4 , high-valent cobalt-oxo, nonradical oxidation, sulfonamide antibiotics, SO 2 extrusion

show abstract

“…10,11 The inhibitory effects by the reactions between radical ROS and the background substrates such as Cl − and dissolved organics could be mitigated by the nonradical pathways, which could limit the spectrum of oxidizable pollutants and avoid the undesired consumption of the reactive oxidant by the reaction with background substances. 12,13 Recently, iron-loaded catalysts have demonstrated potential as PS activators for pollutant degradation without relying on typical radical ROS. 12,14,15 The high reactivity of the iron-loaded catalyst/PS system was due to the generation of powerful high-valent iron species [e.g., Fe(IV)], which abstracted electrons directly from organic pollutants to fulfil the degradation.…”

Section: ■ Introductionmentioning

confidence: 99%

“…12,13 Recently, iron-loaded catalysts have demonstrated potential as PS activators for pollutant degradation without relying on typical radical ROS. 12,14,15 The high reactivity of the iron-loaded catalyst/PS system was due to the generation of powerful high-valent iron species [e.g., Fe(IV)], which abstracted electrons directly from organic pollutants to fulfil the degradation. Although methyl phenyl sulfoxide (PMSO) has been used as the probe compound for identifying Fe(IV), 16 Mossbauer spectroscopy) was still less explored because Fe(IV) was a short-lived species.…”

Section: ■ Introductionmentioning

confidence: 99%

“…The inhibitory effects by the reactions between radical ROS and the background substrates such as Cl – and dissolved organics could be mitigated by the nonradical pathways, which could limit the spectrum of oxidizable pollutants and avoid the undesired consumption of the reactive oxidant by the reaction with background substances. , Recently, iron-loaded catalysts have demonstrated potential as PS activators for pollutant degradation without relying on typical radical ROS. ,, The high reactivity of the iron-loaded catalyst/PS system was due to the generation of powerful high-valent iron species [e.g., Fe(IV)], which abstracted electrons directly from organic pollutants to fulfil the degradation. Although methyl phenyl sulfoxide (PMSO) has been used as the probe compound for identifying Fe(IV), direct spectroscopic techniques (e.g., Mössbauer spectroscopy) was still less explored because Fe(IV) was a short-lived species. , Also, researchers hypothesized that surface-mediated electron transfer might be the origins of nonradical oxidation pathways in the iron-loaded catalysts .…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Persulfate Oxidation of Sulfamethoxazole by Magnetic Iron-Char Composites via Nonradical Pathways: Fe(IV) Versus Surface-Mediated Electron Transfer

Liang

Duan

et al. 2021

Environ. Sci. Technol.

234

View full text Add to dashboard Cite

Despite the vital roles of reactive radical species in the coupled iron–carbon composite/persulfate (PS) system for eliminating pollutants, nonradical contributions are typically overlooked. Herein, we developed two efficient magnetic iron–char composites via low-temperature (BCFe-400) and high-temperature (BCFe-700) pyrolysis. The two composites activated PS through nonradical pathways for sulfamethoxazole (SMX) degradation. In the BCFe-400/PS system, high-valent iron Fe(IV) was the dominant active species for the oxidation, evidenced by methyl phenyl sulfoxide-based probe tests, Mössbauer spectroscopy, and in situ Raman analyses with kinetic evaluation. In the BCFe-700/PS system, surface-mediated electron transfer dominated the oxidation, and the nonradical regime was probed by the electrochemical test and in situ Raman analysis. Furthermore, the BCFe-400/PS system maintained high efficiency in continuous degradation of SMX due to the feasible Fe2+generation toward Fe(IV) formation. In the BCFe-700/PS system, the stability of the system was limited due to the hindered electron transfer between the surface reactive complex (i.e., BCFe-700–PS*) and SMX, and thermal treatment would help recover the reactivity. Both BCFe-400/PS and BCFe-700/PS systems exhibited high performances for SMX removal in the presence of chloride and humic acid and in real water matrixes (e.g., seawater, piggery wastewater, and landfill leachate), exhibiting the great merits of the nonradical system. Overall, the study would provide new insights into PS activation by iron-loaded catalysts to efficiently degrade pollutants via nonradical pathways.

show abstract

Efficient decontamination of organic pollutants under high salinity conditions by a nonradical peroxymonosulfate activation system

Cited by 333 publications

References 47 publications

Research Progress and Application of Single-Atom Catalysts: A Review

Research Progress and Application of Single-Atom Catalysts: A Review

Novel Nonradical Oxidation of Sulfonamide Antibiotics with Co(II)-Doped g-C₃N₄-Activated Peracetic Acid: Role of High-Valent Cobalt–Oxo Species

Persulfate Oxidation of Sulfamethoxazole by Magnetic Iron-Char Composites via Nonradical Pathways: Fe(IV) Versus Surface-Mediated Electron Transfer

Contact Info

Product

Resources

About

Efficient decontamination of organic pollutants under high salinity conditions by a nonradical peroxymonosulfate activation system

Cited by 333 publications

References 47 publications

Research Progress and Application of Single-Atom Catalysts: A Review

Research Progress and Application of Single-Atom Catalysts: A Review

Novel Nonradical Oxidation of Sulfonamide Antibiotics with Co(II)-Doped g-C3N4-Activated Peracetic Acid: Role of High-Valent Cobalt–Oxo Species

Persulfate Oxidation of Sulfamethoxazole by Magnetic Iron-Char Composites via Nonradical Pathways: Fe(IV) Versus Surface-Mediated Electron Transfer

Contact Info

Product

Resources

About

Novel Nonradical Oxidation of Sulfonamide Antibiotics with Co(II)-Doped g-C₃N₄-Activated Peracetic Acid: Role of High-Valent Cobalt–Oxo Species