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1.
Environ Pollut ; 319: 121010, 2023 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-36608732

RESUMO

First time, this study synthesized a magnetic-modified sludge biochar (MSBC) as an activator of peroxymonosulfate (PMS) to eliminate sulfamethoxazole (SMX). The removal efficiency of SMX reached 96.1% at t = 60 min by PMS/MSBC system. The larger surface area and magnetic Fe3O4 of MSBC surface enhanced its activation performance for PMS. The PMS decomposition, premixing and reactive oxygen species (ROS) identification experiments combined with Raman spectra analysis demonstrated that the degradation process was dominated by surface-bound radicals. The transformed products (TPs) of SMX and the main degradation pathways were identified and proposed. The ecotoxicity of all TPs was lower than that of SMX. The magnetic performance was beneficial for its reuse and the removal efficiency of SMX was 83.3% even after five reuse cycles. Solution pH, HCO3- and CO32- were the critical environmental factors affecting the degradation process. MSBC exhibited environmental safety for its low heavy metal leaching. PMS/MSBC system also performed excellent removal performance for SMX in real waters including drinking water (88.1%), lake water (84.3%), Yangtze River water (83.0%) and sewage effluent (70.2%). This study developed an efficient PMS activator for SMX degradation in various waters and provided a workable way to reuse and recycle municipal sludge.


Assuntos
Sulfametoxazol , Poluentes Químicos da Água , Sulfametoxazol/química , Esgotos , Poluentes Químicos da Água/análise , Peróxidos/química , Água , Fenômenos Magnéticos
2.
Chem Commun (Camb) ; 59(8): 1090-1093, 2023 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-36625092

RESUMO

The photochemical oxidation of benzylic alcohols using N-hydroxyphthalimide (NHPI) catalyst, with Rose Bengal as a singlet oxygen photosensitizer, and the production of hydrogen peroxide (H2O2) under metal-free conditions is presented. Computational and experimental investigations support 1O2 as the oxidant that converts NHPI to the active radical intermediate phthalimide-N-oxyl (PINO). This is a green alternative to current methods of H2O2 production.


Assuntos
Peróxido de Hidrogênio , Peróxidos , Oxirredução , Oxigênio Singlete , Rosa Bengala
3.
Braz J Biol ; 82: e268209, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36651445

RESUMO

The objective of seed extracts from Anisophyllea boehmii and Aframomum sanguineum were to evaluate their ability to stabilize against oxidation of oils exposed to sunlight on one hand and subjected to high temperatures on the other hand. Determination of the peroxide value (PV) showed that the extracts had reduced the oxidation of sunflower oils. After 8 weeks of sunlight exposure, the concentration of 265.45 mg/l of A. boehmii extract showed a PV of 30.78 meq O2/kg, 67.4 mg/l extract of A. sanguineum had a PV of 42.75 meq O2/kg while the oils without extracts had a very high PV (125.06 meq O2/kg). Heating of the oils to 180°C for 8 hours was found, with A. boehmii extract (265.45 mg/l), to have a PV of 29.66 meq O2/kg, with that of A. sanguineum, while the PV of the oils without extract reached 50.66 meq O2/kg. In the light of these results, the seeds of A. boehmii and A. sanguineum contain antioxydant compounds, which, once extracted, can be used for many purposes in the food processing, pharmaceutical and cosmetic industries.


Assuntos
Óleos Vegetais , Sementes , Óleos Vegetais/farmacologia , Burundi , Oxirredução , Peróxidos/análise , Extratos Vegetais/farmacologia
4.
Chemosphere ; 314: 137726, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36596326

RESUMO

A cobalt (Co)-doped perovskite molybdenum trioxide (α-MoO3) catalyst (Co-MO) was synthesized by a facile pyrolysis strategy and used for degrading various organic contaminants via peroxymonosulfate (PMS) activation. The doped Co was inserted in the inter space between the octahedron [MoO6], facilitating the growth of the α-MoO3 crystal on the [010] direction. This unique structure accelerated the activation of PMS as the Co-MO could function as a carrier for electron transfer to facilitate the Co(II)/Co(III) cycle in the Co-MO/PMS system. As a result, the Co-MO/PMS system showed noticeable activity for removing 100% bisphenol A (BPA) under a broad conditions within 30 min. The radical quenching test and electron paramagnetic resonance analysis revealed that singlet oxygen (1O2) was the main active species for BPA degradation in the Co-MO/PMS system, while free radicals, such as O2•-, SO4•- and •OH, were also produced as the intermediate species. Furthermore, the carrier mechanism may enable the Co-MO/PMS system maintain relatively high performance during repeat use, and also excellent adaptability was revealed by the well function in various water matrices and high activity in degrading various refractory organic pollutants. Our findings pave a useful avenue for the rational design of novel cobalt-doped catalysts with high catalytic performance toward wide environmental applications.


Assuntos
Cobalto , Poluentes Ambientais , Poluentes Ambientais/química , Peróxidos/química
5.
Chemosphere ; 314: 137733, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36603681

RESUMO

With the increasing of eutrophication in water body, algae blooms have become one of the global environmental problems. The cyanobacteria waste has placed a severe burden on the environment and transforming cyanobacteria into functional materials may be a wise approach. Herein, cobaltous sulfide/nitrogen-doped biochar (N-BC/CoSx) composite was synthesized by pyrolysis of cyanobacteria waste. The N-BC/CoSx showed excellent performance in peroxymonosulfate (PMS) activation for enrofloxacin (ENR) degradation, which could remove more than 90% ENR within 60 min. The influencing factors of pH and catalyst dosage on ENR removal efficiency were studied. The N-BC/CoSx showed good recyclability in the cycle runs. The radicals (O2•-, OH andSO4•-) and the non-radical species (charge transfer and 1O2) were generated in the ENR degradation. The cycle of Co(II)/Co(III) m ay contribute to the radical generation process. This work proved that metal sulfide modified cyanobacteria biochar has a specific application value in water pollution control and provides a new method for resource utilization of cyanobacteria.


Assuntos
Carbono , Poluentes Ambientais , Nitrogênio , Peróxidos , Cobalto
6.
Water Sci Technol ; 87(1): 336-346, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36640041

RESUMO

The peroxide-based decontaminants had attracted great attention for degradation of chemical warfare agents (CWAs) because of their high performance, non-corrosive and environmental-friendly merits. Hydrogen peroxide can be activated by some organic activators to enhance the oxidation ability. In this work, a novel formula based on sodium percarbonate (SPC) complexed with 1-acetylguanidine (ACG) was investigated for decontamination of sulfur mustard (HD) and VX as CWAs. In the experimental results, the active species acetyl peroxide imide acid in the formula aqueous solution was detected in situ by Raman and 13C NMR spectroscopy. The optimized conditions of the decontamination formula (SPC/ACG) were suggested that, the molar ratio of active oxygen and activator ([O]/[ACG]) was 1:1 while the pH value of the formula aqueous solution was about 9. To achieve the decontamination percentage over 99%, the molar ratio of active oxygen to CWA ((O)/(CWA)) needed to be at least 3 for HD and 7 for VX. Meanwhile, the degradation products detected by gas chromatography/mass spectrometry (GC/MS), liquid chromatography/mass spectrometry (LC/MS) and ion chromatography (IC) indicated that the oxidation and elimination reactions should have occurred on HD molecule, while the degradation of VX mainly originate from the nucleophilic substitution and oxidation reactions.


Assuntos
Substâncias para a Guerra Química , Gás de Mostarda , Gás de Mostarda/análise , Gás de Mostarda/química , Descontaminação/métodos , Espécies Reativas de Oxigênio , Substâncias para a Guerra Química/análise , Substâncias para a Guerra Química/química , Peróxidos , Enxofre
7.
J Environ Manage ; 329: 117022, 2023 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-36549062

RESUMO

In this study, a ternary ZnO@spinel cobalt ferrite@carbon nanotube magnetic photocatalyst (ZSCF@CNT) was successfully synthesized and used to activate peroxymonosulfate (PMS) for Cefixime (CFX) antibiotic degradation under UVC irradiation. The morphology, optical, structural, and physicochemical properties of ZSCF@CNT were characterized and analyzed by XPS, XRD, FESEM-EDX, TEM, BET, VSM, UV-vis DRS and PL analysis. The results indicated that the ternary ZSCF@CNT photocatalyst exhibited superior catalytic activity on CFX elimination than that of individual components and binary composite catalysts, in which CFX with was rapidly removed under UVC irradiation and PMS. The effect of operational parameters including initial PMS, catalyst, and CFX concentrations and solution pH on the catalytic activity was investigated in detail; the optimal conditions were: pH: 7.0, catalyst: 0.3 g/L, PMS: 3.0 mM, leading to total CFX (10 mg/L) elimination in ∼20 min. Based on the radical scavenger tests, various radicals and non-radical species including sulfate, hydroxyl and superoxide radicals, singlet oxygen and electrons were involved in the ZSCF@CNT/PMS/UVC system. The high surface area, reduced agglomeration formation and excellent separation of photogenerated electron-hole pairs embodied in ZSCF@CNT photocatalyst conferred its superior catalytic activity and stability. The results from the tests in real water matrices revealed that ZSCF@CNT could be a promising photocatalyst to activate PMS for actual aqueous matrices' treatment.


Assuntos
Nanotubos de Carbono , Óxido de Zinco , Cefixima , Peróxidos/química
8.
Water Res ; 229: 119452, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36502655

RESUMO

Oxidation pretreatments prior to ultrafiltration are hindered by the need for energy input and sludge disposal. Herein, a simulated sunlight-induced natural organic matter (NOM) for peroxymonosulfate (PMS) activation was used as pretreatment to alleviate ultrafiltration membrane fouling caused by NOM itself in the Songhua River water. When light intensity was over 100 mW/cm2, the pretreatment removed NOM effectively, characterized with UV254, dissolved organic carbon (DOC) and maximum fluorescent intensity (Fmax), and improved filtration flux. At 200 mW/cm2 light intensity and 0.5 mM PMS, 57.5% of UV254 and 18.5% of DOC were removed, and humic-like fluorescent component was degraded by 84%-94% while ∼60% for protein-like substance. Membrane flux was increased by 94%, and reversible and irreversible fouling resistances were reduced by 62.4% and 51.9%, respectively. Both total fouling index (TFI) and hydraulic irreversible fouling index (HIFI) were moderately correlated with the DOC, whereas they prominently correlated with the UV254 and the Fmaxs of all fluorescence components, which could be served as key indicators to predict and control membrane fouling. Mathematical modeling showed that the pretreatment alleviated the fouling in the membrane pores and cake layer. The simulated sunlight-induced NOM (3NOM* and eaq¯) could activate PMS to form active species, which enabled to oxidize high molecular weight (MW) substances and mineralize low MW compounds in NOM as well as hinder their linking with inorganic cations, thereby reducing organic and inorganic membrane fouling simultaneously. This study may provide a new strategy for decentralized potable water treatment, especially in a single household or community.


Assuntos
Ultrafiltração , Purificação da Água , Luz Solar , Membranas Artificiais , Peróxidos
9.
J Colloid Interface Sci ; 633: 967-978, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36509039

RESUMO

In this work, we found that the presence of non-active ZnO crystals greatly accelerated the degradation of Bisphenol A (BPA) by 3.7 folds in the peroxymonosulfate (PMS, HSO5-)/Co3O4 system. Our mechanistic study revealed that the ZnO particles would create negative electric microfields around them, which are closely related with the zeta potentials (ζ) of ZnO and affected by solution pH. According to COMSOL simulation, the electrostatic repulsion between ZnO and PMS would drive HSO5- toward active Co3O4 surface, leading to the concentration increasing of HSO5- around active Co3O4 particles, which will then improve the degradation performance. The particle size of ZnO will also affect the promoting effect greatly by COMSOL simulation. Therefore, this study for the first time reveals synergy of electric microfields for enhanced heterogeneous Fenton-like reactions, providing a low-cost and effective strategy for enhanced persulfate catalysis.


Assuntos
Óxido de Zinco , Peróxidos/química , Óxidos/química , Cobalto/química , Catálise
10.
Chemosphere ; 313: 137648, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36572361

RESUMO

The selective oxidation of ammonia to dinitrogen gas in some special wastewater is of paramount significance, but still a challenge. In this study, chlorine radical (Cl•)-mediated oxidation process was developed to realize the selective oxidation of NH4+-N to N2, in which Cl• was generated in Co2+/peroxymonosulfate (PMS)/chloridion (Cl-) system. The effect of various operational parameters on the efficiency and selectivity of ammonia oxidation to N2 was investigated, such as PMS concentration, Co2+ concentration, Cl- concentration and pH value. The experiment results showed that Cl•-mediated NH4+-N oxidation reaction exhibited high NH4+-N removal efficiency and considerable selectivity to N2 in the range of pH from 2.0 to 6.5. The removal efficiency of NH4+-N was 90.39%, and the selectivity of NH4+-N to N2 achieved up to 97.16%. The possible mechanism for high efficient and selective oxidation of NH4+-N to N2 was tentatively proposed. The process developed in this study could provide a novel technology for the treatment and selective oxidation of ammonium in some special types of ammonium-containing wastewater.


Assuntos
Compostos de Amônio , Poluentes Químicos da Água , Amônia , Cloro , Peróxidos , Oxirredução , Cloretos
11.
Phytochemistry ; 206: 113548, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36481317

RESUMO

Antiosteoclastogenic-guided screening was conducted with 120 extracts of the medicinal plants collected in Egypt that led to the selection of Artemisia judaica L. (Asteraceae). Three undescribed davanone-related terpenoids, arteperoxides A-C, were isolated from the extract with two known derivatives, hydroxydavanone and davana acid. Structural analysis revealed that arteperoxides A-C were tris-normonoterpene-sesquiterpene conjugates with peroxide bridges. Although davanone derivatives with peroxides, such as a hydroperoxyl and peroxyhemiketal groups, have been isolated from Artemisia species, arteperoxides A-C are the first variations observed to contain peroxide bridges between two terpene-derived units. The absolute configurations of arteperoxides A and B were studied based on their spectroscopic data compared with those of the semisynthetic analogs that have ether linkages. The natural and synthetic compounds were tested for the antiosteoclastogenic activity, and arteperoxide C and hydroxydavanone were more potent than other compounds at 20 µM.


Assuntos
Artemisia , Plantas Medicinais , Sesquiterpenos , Artemisia/química , Peróxidos , Sesquiterpenos/farmacologia , Sesquiterpenos/química , Terpenos , Extratos Vegetais/farmacologia , Extratos Vegetais/química
12.
J Colloid Interface Sci ; 630(Pt B): 714-726, 2023 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-36347098

RESUMO

In this study, a novel carbon-wrapped-iron hierarchical porous catalyst (Fe/C-Mn800) was prepared from electrolytic manganese residue (EMR) and sewage sludge (SS), which showed outstanding degradation ability toward benzohydroxamic acid (BHA, nearly 90 % was removed within 60 min) with low metal leaching rate. Mechanism exploration found transition metal ions (Fe and Mn) can serve as electron acceptors and facilitate the generation of persistent free radicals (PFRs). These transition metal ions and PFRs mainly participated in the single-electron pathway via activating PMS to generate a large amount of reactive oxygen species (ROS). While the electron negative graphitic N and CO groups not only improve the electronegatively of catalyst, but also acted as the electron sacrificers to favor the electron transfer and directly oxidized the absorbed BHA through the ternary activated outer-sphere complexes. Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) analysis further demonstrated the crucial role of pre-adsorption during the degradation process. This work provided a deep insight into the degradation mechanism of metal/carbon composite and promising opportunity widened the horizon of the high-value utilization of EMR and SS.


Assuntos
Peróxidos , Resíduos Sólidos , Carbono/química , Radicais Livres , Metais , Peróxidos/química , Porosidade , Esgotos/química
13.
J Adv Res ; 43: 205-218, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-36585109

RESUMO

Amyotrophic lateral sclerosis (ALS) is a progressive neurodegenerative disease characterized by oxidative stress that triggers motor neurons loss in the brain and spinal cord. However, the mechanisms underlying the exact role of oxidative stress in ALS-associated neural degeneration are not definitively established. Oxidative stress-generated phospholipid peroxides are known to have extensive physiological and pathological consequences to tissues. Here, we discovered that the deficiency of glutathione peroxidase 4 (GPX4), an essential antioxidant peroxidase, led to the accumulation of phospholipid peroxides and resulted in a loss of motor neurons in spinal cords of ALS mice. Mutant human SOD1G93A transgenic mice were intrathecally injected with neuron-targeted adeno-associated virus (AAV) expressing GPX4 (GPX4-AAV) or phospholipid peroxidation inhibitor, ferrostatin-1. The results showed that impaired motor performance and neural loss induced by SOD1G93A toxicity in the lumbar spine were substantially alleviated by ferrostatin-1 treatment and AAV-mediated GPX4 delivery. In addition, the denervation of neuron-muscle junction and spinal atrophy in ALS mice were rescued by neural GPX4 overexpression, suggesting that GPX4 is essential for the motor neural maintenance and function. In comparison, conditional knockdown of Gpx4 in the spinal cords of Gpx4fl/fl mice triggered an obvious increase of phospholipid peroxides and the occurrence of ALS-like motor phenotype. Altogether, our findings underscore the importance of GPX4 in maintaining phospholipid redox homeostasis in the spinal cord and presents GPX4 as an attractive therapeutic target for ALS treatment.


Assuntos
Esclerose Amiotrófica Lateral , Doenças Neurodegenerativas , Camundongos , Humanos , Animais , Esclerose Amiotrófica Lateral/genética , Esclerose Amiotrófica Lateral/patologia , Superóxido Dismutase-1/genética , Doenças Neurodegenerativas/patologia , Superóxido Dismutase/genética , Neurônios Motores/patologia , Camundongos Transgênicos , Glutationa Peroxidase/genética , Peróxidos
14.
Water Res ; 229: 119489, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36528926

RESUMO

Peroxymonosulfate (PMS)-based photocatalysis is a promising alternative approach for wastewater disinfection. Singlet oxygen (1O2) is sensitive and efficient for bacterial inactivation. This study developed a 1O2-predominated PMS disinfection technique under visible light with CuS quantum dots (QDs) modified MIL-101(Fe) (CSQDs@MF). CuS QDs modification greatly enhanced the 1O2 quantum yield by 80% than that of MIL-101(Fe). Photoelectricity and photoluminescence tests demonstrated that both the enhanced electron transfer and energy transfer were responsible for improved 1O2 generation in Vis/PMS/CSQDs@MF system. The system took 60 min to inactivate 7.5-log E. coli, and it could be applied in a broad pH and dissolve oxygen range. Bacterial inactivation mechanism suggested that 1O2 attacked cell membrane first, then induced oxidative stress, up-regulated intracellular ROS level, eventually broke DNA strand. The system showed good disinfection performance on Gram-positive B. subtilis and fecal coliforms in practical wastewater, implying it is a promising alternative disinfection technology for wastewater treatment.


Assuntos
Pontos Quânticos , Desinfecção , Escherichia coli , Elétrons , Peróxidos , Oxigênio
15.
Water Res ; 229: 119503, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36549188

RESUMO

Electrochemically producing hydrogen peroxide (H2O2) from oxygen reduction reaction (ORR) with natural air diffusion electrode (NADE) is an attractive way to supply H2O2 for decentralized water treatment. In this study, the stability of NADE during H2O2 electroproduction in varying water matrices were evaluated, including synthetic electrolyte solutions (0.05 M Na2SO4) with or without calcium ions (Ca2+, 200 mg/L) and/or humic acid (HA, 40 mg/L), as well as a selected municipal wastewater (92.7 mg/L Ca2+, 3.6 mg/L Mg2+, and 23.9 mg/L total organic carbon). The results show that NADEs maintained a good stability during H2O2 electroproduction in Na2SO4 solutions regardless of the presence of HA. However, Ca2+ (and Mg2+) could form significant amounts of mineral precipitates on the surface and in the internal pores of NADEs during H2O2 electroproduction. These mineral precipitates can negatively influence H2O2 production by impeding the oxygen, electron, and proton transfer processes involved in ORR to H2O2. Moreover, the mineral precipitates shifted the NADEs from hydrophobic to hydrophilic, which may promote H2O2 reduction to H2O at the NADEs. Consequently, the apparent current efficiencies of H2O2 production decreased substantially from initially ∼90% to 50%-70% as the NADEs were continuously used for 60 h in the Ca-containing solutions and selected wastewater. These results indicate that water constituents that are commonly present in real water matrices, especially Ca2+, can cause serious deterioration of NADE stability during H2O2 electroproduction. Therefore, proper strategies are needed to mitigate electrode fouling during H2O2 electroproduction with NADEs in practical water and wastewater treatment.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Peróxido de Hidrogênio/química , Peróxidos , Oxirredução , Oxigênio , Eletrodos , Purificação da Água/métodos
16.
Chemosphere ; 314: 137684, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36584832

RESUMO

Metal-free carbon-based catalysts hold great promise for the degradation of organic pollutants by peroxymonosulfate (PMS) activation because they avoid the negative effects of metal catalysts such as harmful metal ions leaching. However, these carbon-based catalysts are limited by their high cost and complex synthesis, and the mechanisms for the activation of PMS are unclear. Herein, the N-rich carbon catalysts (GCN-x) derived from glucose and g-C3N4 were facilely synthesized by hydrothermal treatment and carbonization to explore the mechanism of PMS activation. The nitrogen content of catalysts could be adjusted by simply altering the ratio of glucose and g-C3N4. GCN-2.4 with a ratio of glucose and g-C3N4 of 2.4 displayed the highest efficiency for the degradation of pollutants represented by Levofloxacin. The electron paramagnetic resonance and quenching experiments demonstrated that the non-radical pathway was dominant in Levofloxacin degradation and singlet oxygen (1O2) was the main active specie. Further, we found 1O2 was generated from superoxide radical (• O2-) which has rarely been studied. Levofloxacin degradation rate was shown to be positively correlated with both the amount of graphitic N and pyridinic N. Graphitic N and pyridinic N were identified as the catalytic sites. The GCN-2.4/PMS system could also remove multifarious contaminants effectively. Overall, this research advances understanding of the role of N species in PMS activation and has potential practical application in wastewater treatment.


Assuntos
Poluentes Ambientais , Grafite , Carbono , Levofloxacino , Peróxidos , Metais
17.
J Hazard Mater ; 445: 130562, 2023 03 05.
Artigo em Inglês | MEDLINE | ID: mdl-36502719

RESUMO

High-temperature nitrogen (N) doping boosts the activity of biochars for peroxymonosulfate (PMS) activation, but the N heat loss causes the unsatisfactory catalytic efficiency. Improving the surface area for obtaining the high exposure of N sites is a promising solution. Herein, a soft template-KHCO3 etching strategy is used to synthesize the N-doped porous bowl-like carbon (NPBC) with ultrahigh external surface area (1610.8 m2 g-1). The bowl-like structure eliminates inert bulk interior and allows unobstructed mass transfer of reactants onto both outer and inner surfaces, while the large pore channels by KHCO3 etching further improves the exposure degree of limited N sites. Although NPBC has only 0.43% N content, 93.1% of bisphenol A (BPA) is removed within 1 min through the electron-transfer pathway by fully utilizing the N active centers, and the kinetic rate constant (k) reaches 5.29 min-1, exceeding reported values by 2-270 times. Moreover, the NPBC/PMS system possesses excellent applicability for various organics and conditions, effectively mineralizes BPA and reduces effluent biotoxicity. A quantitative index W representing N exposure degree is first proposed and shows high linearity with the k values of BPA degradation (R2=0.992, 0 

Assuntos
Carbono , Peróxidos , Carbono/química , Porosidade , Peróxidos/química
18.
J Colloid Interface Sci ; 634: 231-242, 2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36535161

RESUMO

Lower reaction speed and excessive oxidant inputs impede the removal of contaminants from water via the advanced oxidation processes based on peroxymonosulfate. Herein, we report a new confined catalysis paradigm via the hollow hetero-shell structured CN@C (H-CN@C), which permits effective decontamination through polymerization with faster reaction rates and lower oxidant dosage. The confined space structures regulated the CN and CO and electron density of the inner shell, which increased the electron transfer rate and mass transfer rate. As a result, CN in H-CN@C-10 reacted with peroxymonosulfate in preference to CO to generate singlet oxygen, improving the second-order reaction kinetics by 503 times. The identification of oxidation products implied that bisphenol AF could effectively remove by polymerization, which could reduce carbon dioxide emissions. These favorable properties make the nanoconfined catalytic polymerization of contaminants a remarkably promising nanocatalytic water purification technology.


Assuntos
Peróxidos , Purificação da Água , Polimerização , Peróxidos/química , Oxidantes
19.
J Colloid Interface Sci ; 634: 255-267, 2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36535163

RESUMO

Mn and N co-doped biochar (Mn-N-TS) was prepared as an effective catalyst to activate peroxymonosulfate (PMS) for ciprofloxacin (CIP) degradation. As opposed to Mn-TS and N-TS, Mn-N-TS had more active sites containing N and Mn, as well as a greater specific surface area (923.733 m2 g-1). The Mn-N-TS exhibited excellent PMS activation ability. In the Mn-N-TS/PMS system, the CIP removal efficiency was 91.9% in 120 min. Mn and N co-doping could accelerate electron transfer between CIP and PMS molecules. Simultaneously, defect sites, graphitic N, pyridinic N, C═O groups, and Mn(II)/Mn(III)/Mn(IV) redox cycles acted as active sites to activate PMS and generate free radicals (OH, SO4- and 1O2). Furthermore, the Mn-N-TS/PMS system could effectively degrade CIP in a wide pH range, background substances, and actual water. Finally, a probable mechanism of PMS activation by Mn-N-TS was proposed. In conclusion, this work gave a novel direction for the rational design of Mn and N co-doped biochar.


Assuntos
Ciprofloxacina , Peróxidos , Porosidade , Peróxidos/química , Oxirredução
20.
J Colloid Interface Sci ; 634: 521-534, 2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36549201

RESUMO

Herein, we engineered the cobalt core size and carbon shell thickness of Co@C by molten salt electrolysis (MSE) to investigate the enhanced essence of decreasing core size as well as the shell thickness dependence-mediated transition of catalytic mechanisms. We found that the reaction activation energy (RAE) of Co@C/peroxymonosulfate (PMS) systems was intimately dependent on the core sizes for sulfamethoxazole (SMX) degradation. The smaller core size of 26 nm provided a lower RAE of 13.39 kJ mol-1. In addition, increasing carbon shell thicknesses of Co@C altered the catalytic mechanisms from a radical pathway of SO4•- and •OH to to a non-radical pathway of 1O2 and electron-transfer process (ETP), which were verified by experimental results and density functional theory (DFT) calculations. Interestingly, increasing carbon shell thicknesses promoted the charge transfer between Co metal slab and carbon shell, increased the adsorption energy of PMS molecule on the Co@C slab, and decreased the length of OO, which favoured the occurrence of non-free radical processes.


Assuntos
Carbono , Peróxidos , Sulfametoxazol , Catálise
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