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1.
Nano Lett ; 23(14): 6323-6329, 2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37459426

RESUMO

There remains continued interest in improving the advanced water oxidation process [e.g., ultraviolet (UV)/hydrogen peroxide (H2O2)] for more efficient and environmentally friendly wastewater treatment. Here, we report the design, fabrication, and performance of graphene oxide (GO, on top)/nickel-doped iron oxyhydroxide (Ni:FeOOH, shell)/silicon nanowires (SiNWs, core) as a new multifunctional photocatalyst for the degradation of common pollutants like polystyrene and methylene blue through enhancing the hydroxyl radical (•OH) production rate of the UV/H2O2 system. The photocatalyst combines the advantages of a large surface area and light absorption characteristics of SiNWs with heterogeneous photo-Fenton active Ni:FeOOH and photocatalytically active/charge separator GO. In addition, the built-in electric field of GO/Ni:FeOOH/SiNWs facilitates the charge separation of electrons to GO and holes to Ni:FeOOH, thus boosting the photocatalytic performance. Our photocatalyst increases the •OH yield by 5.7 times compared with that of a blank H2O2 solution sample and also extends the light absorption spectrum to include visible light irradiation.

2.
Pharm Res ; 38(5): 915-930, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33881737

RESUMO

PURPOSE: To evaluate the effect of excipients, including sugars and amino acids, on photo-degradation reactions in pharmaceutical buffers induced by near UV and visible light. METHODS: Solutions of citrate or acetate buffers, containing 1 or 50 µM Fe3+, the model peptides methionine enkephalin (MEn), leucine enkephalin (LEn) or proctolin peptide (ProP), in the presence of commonly used amino acids or sugars, were photo-irradiated with near UV or visible light. The oxidation products were analyzed by reverse-phase HPLC and HPLC-MS/MS. RESULTS: The sugars mannitol, sucrose and trehalose, and the amino acids Arg, Lys, and His significantly promote the oxidation of peptide Met to peptide Met sulfoxide. These excipients do not increase the yields of hydrogen peroxide, suggesting that other oxidants such as peroxyl radicals are responsible for the oxidation of peptide Met. The addition of free Met reduces the oxidation of peptide Met, but, in citrate buffer, causes the addition of Met oxidation products to Tyr residues of the target peptides. CONCLUSIONS: Commonly used excipients enhance the light-induced oxidation of amino acids in model peptides.


Assuntos
Antioxidantes/química , Ácido Cítrico/química , Excipientes/química , Ferro/química , Peptídeos/química , Soluções Tampão , Armazenamento de Medicamentos , Concentração de Íons de Hidrogênio , Luz/efeitos adversos , Metionina/química , Oxirredução/efeitos da radiação , Peptídeos/efeitos da radiação , Peptídeos/uso terapêutico , Espectrometria de Massas em Tandem , Tirosina/química , Tirosina/efeitos da radiação , Raios Ultravioleta/efeitos adversos
3.
Mol Pharm ; 17(11): 4163-4179, 2020 11 02.
Artigo em Inglês | MEDLINE | ID: mdl-32986444

RESUMO

Near UV (λ = 320-400 nm) and visible light (λ = 400-800 nm) can lead to the oxidation of pharmaceutical proteins, which can affect efficiency and promote immunogenicity. However, no concise mechanism has been established for the photo-oxidation of pharmaceutical proteins under near UV and visible light. Here, we show that carboxylic acid buffer-Fe3+ complexes can function as photosensitizers, causing peptide degradation via the formation of various radicals and oxidants. Three pharmaceutical relevant carboxylic acid buffers (citrate, acetate, and succinate) were tested under near UV and visible light. Oxidation reactions were monitored for model peptides containing readily oxidizable amino acids, such as methionine- or leucine-enkephalin and proctolin peptide. Oxidation products were evaluated by RP-HPLC coupled to UV or fluorescent detection and RP-HPLC-MS/MS. Specifically for citrate buffer, the light-induced formation of H2O2, •OH, •CO2-, and formaldehyde was demonstrated. The peptides displayed oxidation of Met, hydroxylation of Tyr and Phe, as well as the formation of novel products from Tyr. Experiments with 18O2 resulted in the incorporation of 18O into various reaction products, consistent with a metal-catalyzed activation of O2 into reactive oxygen species. The addition of EDTA and DTPA did not prevent the oxidation of the peptides and, in some cases, enhanced the oxidation. Our results demonstrate that pharmaceutical buffer-Fe3+ complexes, exposed to UV and visible light, can promote various pathways of oxidation reactions in pharmaceutical formulations.


Assuntos
Encefalina Leucina/química , Encefalina Metionina/química , Compostos Férricos/química , Luz/efeitos adversos , Preparações Farmacêuticas/química , Fotólise/efeitos da radiação , Raios Ultravioleta/efeitos adversos , Acetatos/química , Soluções Tampão , Ácidos Carboxílicos/química , Cromatografia Líquida de Alta Pressão/métodos , Ácido Cítrico/química , Peróxido de Hidrogênio/química , Concentração de Íons de Hidrogênio , Oxirredução/efeitos da radiação , Fármacos Fotossensibilizantes/química , Ácido Succínico/química , Espectrometria de Massas em Tandem/métodos
4.
Ecotoxicol Environ Saf ; 200: 110744, 2020 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-32460050

RESUMO

Hematite nanoparticles (α-Fe2O3 NPs) were successfully synthesized by a low-cost solvent-free reaction using Ferrous sulfate waste (FeSO4·7H2O) and pyrite (FeS2) as raw materials and employed for the decolorization of Methyl Orange by the photo-Fenton system. The properties of α-Fe2O3 NPs before and after photo-Fenton reaction were characterized by X-ray powder diffraction (XRD), Field emission scanning electron microscopy (FESEM), Fourier transform infrared (FT-IR) spectrum and X-ray photoelectron spectroscopy (XPS), and the optical properties of α-Fe2O3 NPs were analyzed by UV-vis diffuse reflectance spectra (UV-vis DRS) and Photoluminescence (PL) spectra. The analytic results showed that the as-formed samples having an average diameter of ~50 nm exhibit pure phase hematite with sphere structure. Besides, little differences were found by comparing the characterization data of the particles before and after the photo-Fenton reaction, indicating that the photo-Fenton reaction was carried out in solution rather than on the surface of α-Fe2O3 NPs. A 24 central composite design (CCD) coupled with response surface methodology (RSM) was applied to evaluate and optimize the important variables. A significant quadratic model (P-value<0.0001, R2 = 0.9664) was derived using an analysis of variance (ANOVA), which was adequate to perform the process variables optimization. The optimal process conditions were performed to be 395 nm of the light wavelength, pH 3.0, 5 mmol/L H2O2 and 1 g/L α-Fe2O3, and the decolorization efficiency of methyl orange was 99.55% at 4 min.


Assuntos
Compostos Azo/química , Corantes/química , Compostos Férricos/química , Nanopartículas Metálicas/química , Catálise , Compostos Férricos/síntese química , Compostos Ferrosos/química , Ferro/química , Solventes , Sulfetos/química
5.
Angew Chem Int Ed Engl ; 59(42): 18515-18521, 2020 10 12.
Artigo em Inglês | MEDLINE | ID: mdl-32643814

RESUMO

As an emerging member of the graphene family, structurally defined graphene nanoribbons (GNRs) have shown promising applications in various fields. The evaluation of the degradability of GNRs is particularly important for assessing the persistence level and risk of these materials in living organisms and the environment. However, there is a void in the study of the degradation of GNRs. Here, we report the degradation behavior of GNRs in the presence of human myeloperoxidase (hMPO) or treated with the photo-Fenton (PF) reaction. With the assistance of potassium hydroxide or imidazole, which facilitates the dispersion of GNRs in the aqueous solution, GNRs underwent only partial degradation after 25-hour incubation with hMPO, while, the PF reaction degraded GNRs almost completely after 120 hours. These results indicate that structurally precise GNRs can be efficiently degraded under suitable conditions, providing more opportunities for future applications in different fields.

6.
J Environ Sci (China) ; 80: 208-217, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-30952338

RESUMO

The heterogeneous photo-Fenton reaction is an effective technique in combating organic contaminants for both soil and water remediation, and extensive studies have focused on enhancing its efficiency and reducing its costs. In this work, we developed novel photo-Fenton catalysts by simply milling commercially available TiO2 (P25) with Schwertmannite (Sh), a natural iron-oxyhydroxysulfate nanomineral. We expect that the photo-generated electrons from TiO2 could continuously migrate to Sh, which then could enhance the separation of electron-hole pairs on TiO2 and accelerate the reduction of Fe(III) to Fe(II) on Sh, leading to high degradation efficiency of the target organic contaminants. SEM and TEM results showed the distribution of TiO2 on Sh surface for the nanocomposites (TiO2/Sh). Under simulated sunlight irradiation, the much higher content of Fe(II) was determined on TiO2/Sh than on Sh via a common method in the iron ore, and the consumption of H2O2 and the production of •OH were more significant in the TiO2/Sh system than those in the TiO2 and Sh systems. These results well support our hypothesis that the photo-generated electrons could migrate from TiO2 to Sh on the composites, and can also explain the much higher degradation efficiency of Rhodamine B (RhB) in the TiO2/Sh system. Besides, TiO2/Sh had lower Fe dissolution as compared with Sh, and retained high catalytic stability after four repeated cycles. Above merits of the TiO2/Sh composites, in combining with their simple synthesis method and low-cost property, indicated that they should have promising applications as heterogeneous photo-Fenton catalysts.


Assuntos
Poluentes Ambientais/química , Compostos de Ferro/química , Modelos Químicos , Nanocompostos/química , Titânio/química , Recuperação e Remediação Ambiental/métodos , Compostos Férricos , Peróxido de Hidrogênio
7.
J Environ Sci (China) ; 83: 39-45, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31221386

RESUMO

This study for the first time proposed an efficient microbial electrolyte/UV system for Methyl Orange decomposition. With an external applied voltage of 0.2 V and cathode aeration of 20 mL/min, H2O2 could be in-situ generated from two-electron reduction of oxygen in cathode, reaching to 8.1 mg/L in 2 hr and continued to increase. The pollutant removal efficiency of approximate 94.7% was achieved at initial neutral pH, with the activation of •OH in the presence of UV illumination. Although the nature of its guiding principles remain on the vista of practical exploration, this proof-of-concept study provides an alternative operation pattern of solar-microbial hybrid technology for future wastewater treatment from a basic but multidisciplinary view.


Assuntos
Raios Ultravioleta , Eliminação de Resíduos Líquidos/métodos , Poluentes Químicos da Água/química , Compostos Azo/química , Fontes de Energia Bioelétrica , Águas Residuárias/química , Poluentes Químicos da Água/análise
8.
J Environ Manage ; 167: 206-13, 2016 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-26686073

RESUMO

Mefenamic acid (MEF) is a non-steroidal anti-inflammatory drug indicated for relief of mild to moderate pain, and for the treatment of primary dysmenorrhea. The presence of MEF in raw and sewage waters has been detected worldwide at concentrations exceeding the predicted no-effect concentration. In this study, using experimental designs, different oxidative processes (H2O2, H2O2/UV, fenton and Photo-fenton) were simultaneously evaluated for MEF degradation efficiency. The influence and interaction effects of the most important variables in the oxidative process (concentration and addition mode of hydrogen peroxide, concentration and type of catalyst, pH, reaction period and presence/absence of light) were investigated. The parameters were determined based on the maximum efficiency to save time and minimize the consumption of reagents. According to the results, the photo-Fenton process is the best procedure to remove the drug from water. A reaction mixture containing 1.005 mmol L(-1) of ferrioxalate and 17.5 mmol L(-1) of hydrogen peroxide, added at the initial reaction period, pH of 6.1 and 60 min of degradation indicated the most efficient degradation, promoting 95% of MEF removal. The development and validation of a rapid and efficient qualitative and quantitative HPLC/UV methodology for detecting this pollutant in aqueous solution is also reported. The method can be applied in water quality control that is generated and/or treated in municipal or industrial wastewater treatment plants.


Assuntos
Ácido Mefenâmico/isolamento & purificação , Eliminação de Resíduos Líquidos/métodos , Poluentes Químicos da Água/isolamento & purificação , Catálise , Cromatografia Líquida de Alta Pressão , Peróxido de Hidrogênio/química , Concentração de Íons de Hidrogênio , Ácido Mefenâmico/química , Oxalatos/química , Oxirredução , Esgotos , Raios Ultravioleta , Poluentes Químicos da Água/química
9.
J Environ Sci (China) ; 47: 34-38, 2016 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-27593270

RESUMO

The photo-Fenton reaction is a key source of the highly reactive hydroxyl radical (HO) that is produced by the reaction of simultaneous photo-induced generation of Fe(2)(+)-dissolved organic matter (DOM) with H2O2 in sunlit surface waters as well as in the treatment of organic pollutants in the advanced oxidation processes (AOPs). Concentrations of both H2O2 and Fe(2)(+)-DOM were dependent on time and total solar intensity flux, and their levels were highest in the diurnal samples collected at noon compared with the samples collected during the period before sunrise and after sunset. H2O2 and Fe(2)(+)-DOM concentrations during monthly readings were also found higher in comparison with the diurnal samples, shortly before sunrise or after sunset. A π-electron bonding system is formed between Fe and the functional groups in DOM (Fe-DOM), through electron donation from the functional groups of DOM to an empty d-orbital of Fe. The π-electron is loosely bound and is highly susceptible to a rapid excitation upon light exposure that will provide better understanding of the formation of aqueous electrons, superoxide radical anions, H2O2 and finally, photo-Fenton reactions, too. Our results imply that simultaneous generation of H2O2 and Fe(2)(+)-DOM upon sunlight exposure during the daytime is most likely to be the key photo-Fenton reaction pathway, taking place in surface waters.


Assuntos
Peróxido de Hidrogênio/química , Ferro/química , Processos Fotoquímicos , Rios/química , Poluentes Químicos da Água/química , Monitoramento Ambiental , Peróxido de Hidrogênio/análise , Ferro/análise , Oxirredução , Luz Solar , Raios Ultravioleta , Poluentes Químicos da Água/análise
10.
Bioresour Technol ; 395: 130390, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38301944

RESUMO

In this study, H2O2 (0.1 ‰) and NH2-MIL-101(Fe)-driven (150 mg/L) photo-Fenton-coupled anammox were proposed to simultaneously improve the removal efficiency of nitrogen and humic acid. Long-term experiments showed that the total nitrogen removal efficiency was increased by the photo-Fenton reaction to 91.9 ± 1.5 % by altering the bioavailability of refractory organics. Correspondingly, the total organic carbon removal efficiency was significantly increased. Microbial community analyses indicated that Candidatus_Brocadia maintained high activity during photo-Fenton reaction and was the most abundant genus in the reactor. Dissimilatory nitrate reduction to ammonium process and denitrification process were enhanced, resulting in reduced NO3--N production. The establishment of electron transfer between microorganisms and NH2-MIL-101 (Fe) improved the charge separation efficiency of the quantum dots and increased the intracellular adenosine triphosphate content of anammox bacteria. These results indicated that photo-Fenton-anammox process promoted the removal of nitrogen and refractory organics in one reactor which had good economic value and application prospects.


Assuntos
Compostos de Amônio , Desnitrificação , Estruturas Metalorgânicas , Oxirredução , Nitrogênio , Peróxido de Hidrogênio , Oxidação Anaeróbia da Amônia , Elétrons , Reatores Biológicos/microbiologia , Esgotos
11.
Chemosphere ; 312(Pt 1): 137253, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36395896

RESUMO

Photocatalytic disinfection is considered a promising method for eliminating the hazards of pathogenic bacteria. Graphitic carbon nitride (g-C3N4) is an ideal photocatalytic bacterial inactivation material for its advantage of tunable band structure, good stability and easy preparation. This work has constructed a novel defective 3D porous g-C3N4 by cyanamide carbonation using dendritic mesoporous silica template. The direct loading of Fe3O4 nanoparticles provided an excellent pg-C3N4-Fe3O4 photocatalyst suitable for water disinfection. Compared to pristine g-C3N4, the prepared 3D porous defective g-C3N4-Fe3O4 exhibited the enhanced visible light absorbance as indicated by the band gap decreasing of 0.66 eV, and about 3 and 10 fold increase of photo-induced current response and O2 adsorption respectively. The pg-C3N4-Fe3O4 showed excellent visible-light-driven photocatalytic bactericidal activity. It could kill 1 × 107 cfu mL-1Escherichia coli completely within 1 h under visible-light illumination (100 mW cm-2) with good reusability, its logarithmic bacterial inactivation efficiency was about 2.5 fold higher than pg-C3N4. The enhanced bactericidal performance is mainly ascribed to the Fe3O4 involved cascade photo-Fenton reaction.


Assuntos
Desinfecção , Luz , Porosidade , Catálise , Desinfecção/métodos , Bactérias , Escherichia coli
12.
Chemosphere ; 337: 139255, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37356589

RESUMO

Hydrothermal and wet impregnation methods are presented in this study for synthesizing CoOx(1 wt%)/Sn/Zr-codoped Fe2O3 nanorod photocatalysts for the degradation of organic pollutants and deactivation of bacteria. A hydrothermal route was used to synthesize self-assembled rod-like hierarchical structures of Sn(0-6%) doped Zr-Fe2O3 NRs. Additionally, a wet impregnation method was used to load CoOx onto the surface of photocatalysts (Sn(0-6%)-doped Zr-Fe2O3 NRs). A series of 1 wt% CoOx modified Sn(0-6%)-doped Zr-Fe2O3 NRs were synthesized, characterized, and utilized for the photocatalytic decomposition of organic contaminants, along with the killing of E. coli and S. aureus. In comparison with 0, 2, and 6% Sn co-doped Zr-Fe2O3 NRs, the CoOx(1 wt%)/4%Sn/Zr-Fe2O3 NRs photocatalyst exhibited an E. coli and S. aureus inactivation efficiencies (90 and 98%). A bio-TEM study of treated and untreated bacterial cells revealed that the CoOx(1 wt%)/4%Sn/Zr-Fe2O3 NRs photocatalyst led to considerable changes in the bacterial cell membranes' morphology. The optimal CoOx(1 wt%)/Sn(4%) co-doped Zr-Fe2O3 NRs photocatalyst achieved degradation efficiencies of 98.5% and 94.6% for BPA and orange II dye, respectively. As a result, this work will provide a facile and effective method for developing visible light-active photocatalysts for bacterial inactivation and organic pollutants degradation.


Assuntos
Escherichia coli , Nanotubos , Staphylococcus aureus , Catálise , Luz
13.
J Colloid Interface Sci ; 626: 639-652, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-35810703

RESUMO

Photo-Fenton reaction combining the photocatalytic reaction and Fenton reaction showed excellent degradation performance. However, it highly demanded the catalysts to display outstanding activity in these two reactions. Herein, Fe-doped carbon nitride/MXenes-derived C-TiO2/Ti3C2 (Fe-C3N4/Ti3C2/C-TiO2) was prepared via two steps: Fe-C3N4 and Ti3C2 were assembled via face-to-face attachment, following by in-situ partial oxidation of Ti3C2 to C-TiO2. DFT predicted a Z-scheme charge transfer routine via metallic Ti3C2 as bridge, which was verified by EPR and radical trapping experiments. Additionally, PDOS calculation revealed the charge density around the doped-Fe atoms was remarkably increased, leading to better H2O2 activation, which was experimentally confirmed by high yield of •OH. Moreover, Fe-C3N4/Ti3C2/C-TiO2 possessed the high photothermal effect to accelerate the surface reaction. By taking advantage of these merits, the degradation rate of Fe-C3N4/Ti3C2/C-TiO2 was at least 4.2 times higher than the reference catalysts. Our work provided an insight toward the g-C3N4/TiO2-based photo-Fenton catalysts with high performance.

14.
Carbohydr Polym ; 296: 119960, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36088002

RESUMO

A novel Fe-complex loaded visible-light active cellulose acetate (CA) composite membrane (Fe-complex/CA) was fabricated using the tape casting method. The Fe-complex was structurally characterized by single-crystal X-ray diffraction, and the prepared composite membrane was characterized by SEM, XPS, XRD, FTIR and UV-Vis diffuse reflectance spectroscopy. The Fe-complex/CA composite membrane exhibited relatively good visible light photocatalytic activity toward organic dyes and sulfadiazine antibiotics in the presence of low concentrations of H2O2. After irradiation for 60 min, the degradation efficiencies of basic fuchsin, methylene blue and sulfadiazine reached 100 %, 93.4 % and 95.7 %, respectively. The composite membrane maintained good photocatalytic activity after four catalytic cycles. Kinetic studies showed that the degradation processes of basic fuchsin, methylene blue and sulfadiazine were all in accordance with first-order reaction kinetics. In addition, the photocatalytic mechanism of the Fe-complex/CA composite membrane in the photo-Fenton reaction was also discussed in detail.


Assuntos
Peróxido de Hidrogênio , Azul de Metileno , Acetatos , Celulose/análogos & derivados , Cinética , Azul de Metileno/química , Sulfadiazina
15.
Chemosphere ; 304: 135318, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-35709833

RESUMO

It is an urgent need to develop new environmentally friendly spinel ferrites with high catalytic efficiency. In this work, a series of Mg-Fe-Al-O spinels with different ratios of Mg/Al were successfully synthesized by the reaction sintering method and were used as a heterogeneous photo-Fenton catalyst for degradation of Rhodamine B (RhB). The effect of different ratios of Mg/Al on the properties of Mg-Fe-Al-O spinel was characterized and analyzed through a range of advanced characterization techniques and DFT calculations. The influence factors on the photo-Fenton reaction catalyzed by Mg-Fe-Al-O spinels were systematically investigated. The results showed that the prepared Mg-Fe-Al-O spinels had larger lattice parameters, wider bandgap, and stronger magnetism, with the Mg content increased. Among them, Mg-9 (Mg0.88Fe1.88Al0.23O4) had the best catalytic performance in the photo-Fenton reaction. The degradation efficiency of RhB reached 98.45%, and the TOC removal efficiency was 83.47%. The elemental valence and PDOS of Mg-9 (Mg0.88Fe1.88Al0.23O4) spinels were closer to MgFe2O4. The photo-generated holes could directly oxidize water and hydroxyl to generate reactive oxygen species ·OH, improving the catalytic activity.


Assuntos
Peróxido de Hidrogênio , Ferro , Óxido de Alumínio , Catálise , Óxido de Magnésio , Rodaminas
16.
J Colloid Interface Sci ; 603: 685-694, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34225072

RESUMO

Antibiotics as emerging pollutants in water pose great risks to human health. Due to their persistence in the environment, advanced oxidation processes (AOPs) have been proposed for the degradation of antibiotics. Therefore, developing efficient catalysts for AOPs becomes critical for the removal of antibiotics. Herein, we develop self-propelled CuS-based micromotors (CuS@Fe3O4/Pt) as active heterogenous catalysts for efficient photo-Fenton degradation of antibiotics. Combining the merits of conventional heterogenous and homogenous catalysts, the prepared micromotors are easy to recycle and free of secondary pollution risks, while demonstrating high degradation efficiency due to self-induced intensification of mass transfer via autonomous motion and microbubble generation. The H2O2 in the Fenton reagents can serve as the fuel for the micromotors to drive their self-propulsion by bubbles generated from catalytic decomposition of H2O2 by the platinum layer. The dual-stimuli-responsiveness of the micromotors to magnetic field and light irradiation allows multi-modes of propulsion and guidance in different systems. The efficient photothermal effect of CuS enables the micromotors to achieve collective phototactic motion toward light, whereas magnetic responsiveness facilitates the recovery and collection of the micromotors. The synergistic effect of CuS and Fe3O4 NPs in H2O2 under visible light irradiation generates a large amount of OH· and ·O2- to effectively degrade tetracycline within several minutes. With these advantages, the dual-stimuli-responsive CuS-based micromotors provide a new strategy for enhanced degradation of antibiotics in water purification applications.


Assuntos
Peróxido de Hidrogênio , Purificação da Água , Antibacterianos/farmacologia , Cobre , Humanos
17.
Heliyon ; 7(6): e07427, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-34307932

RESUMO

Syrian natural magnetite has been utilized for the removal of methylene blue from aqueous solutions by photo-Fenton reaction. Experiments were carried out to evaluate the kinetic and thermodynamic parameters. Pseudo-first order, pseudo-second-order models were used to analyze the kinetic data obtained at different initial MB concentrations and temperatures. The photo-Fenton degradation process of MB is better described by the pseudo-first-order model. The activation energy Ea = 16.89 and 18.02 kJ/mol for MB degradation at concentrations 40 and 80 mg/l respectively, and that suggesting the degradation reaction proceeded with a low energy barrier, the values obtained (ΔG∗, ΔS∗, and ΔH∗) indicate that the process is endothermic and spontaneous.

18.
J Hazard Mater ; 405: 124668, 2021 03 05.
Artigo em Inglês | MEDLINE | ID: mdl-33301975

RESUMO

Photo-Fenton reaction is a more effective technique for pollutant disposal than photocatalytic reaction. Herein, Fe2O3@polypyrrole/Prussian blue (Fe2O3@PPy/PB) with a hierarchical porous structure was prepared by a reactive-template method. After transforming typical type-II Fe2O3@PPy to Z-scheme Fe2O3@PPy/PB via PB as a bridge, the degradation rate was increased by 1.4 times in photocatalytic reaction and 4.0 times in photo-Fenton reaction due to higher visible-light harvest, enhanced separation efficiency of photoinduced charges, lower interface resistance, and especially well-preserved redox potentials of holes and electrons. Mechanism studies revealed that holes were quenched by H2O2, and this led to •O2- generation and efficient separation of electrons. Meanwhile, O2 was reduced by separated electrons, and this further increased •O2- yield. Therefore, the main radicals changed from hole in photocatalytic reaction to •O2- in the photo-Fenton reaction, leading to an increase as high as 12.1-fold enhancement in the degradation rate. Conversely, only H2O2 participated into photocatalytic reaction using Fe2O3@PPy while O2 was absent, resulting in merely 4.2-fold improvement. This manuscript gives a comprehensive understanding on mechanisms of type-II and Z-scheme heterojunctions in both photocatalytic and photo-Fenton reactions. Obviously, the outcomes are beneficial for designing catalysts with high photo-Fenton activity.

19.
ACS Appl Mater Interfaces ; 13(19): 22694-22707, 2021 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-33944561

RESUMO

Heterojunction catalysts have drawn increasing interest for the visible light-driven Fenton reaction and bring tremendous opportunities for environmental remediation. Herein, a BiOI/MIL-53(Fe) Z-scheme heterojunction (named BMFe) was synthesized for the first time via a facile strategy. Compared with pristine BiOI and MIL-53(Fe) catalysts, the two-dimensional/three-dimensional (2D/3D) heterojunction catalyst manifested remarkable catalytic performance toward degradation of phenol, bisphenol A, methylene blue, and carbamazepine, which is attributed mainly to the interfacial integration and efficient charge separation. By virtue of coupling at the interface, as confirmed by XPS, 57Fe Mössbauer spectroscopy, and DFT calculations, the BMFe catalyst promoted the transfer of electron-hole pairs via Z-scheme and improved the chemical activation of hydrogen peroxide. The subsequent holes, free radicals, and nonradicals can effectively and continuously decompose pollutants, achieving a positive synergistic effect between photocatalysis and Fenton reactions. Simultaneously, the specially designed BiOX(X = Br, Cl)/MIL-53(Fe) and BiOI/Fe-MOFs(MIL-101, MIL-88) heterojunctions also exhibited advanced oxidative capacity for organic pollutants. Given their practical value for industrial applications, BMFe beads (1.0 ± 0.15 mm) synthesized via a blend cross-linking method can significantly advance long-term stability and recyclability. The integration of Fe-based metal-organic frameworks with bismuth oxyhalide semiconductors provides a new perspective on developing heterojunction catalysts for environmental remediation.

20.
Environ Sci Pollut Res Int ; 28(45): 64630-64641, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34318422

RESUMO

This article presents a study on the degradation of a residual textile mixture composed of cationic surfactant cetyltrimethylammonium bromide (CTAB) and the remazol yellow gold RNL-150% and reactive blue BF-5G textile dyes. This was carried out by employing the photo-peroxidation and photo-Fenton processes in LED and UV-C photoreactors. The photo-Fenton process was the most efficient as regards the degradation of the CTAB and dye mixture, for both types of radiation. In the kinetic study, degradations of 99% were obtained in 180 min for the chromophore groups using both types of radiation. The degradation of the CTAB and aromatic groups was, meanwhile, an average of 25% when employing LED radiation. The behavior of the degradation reaction was pseudo-first-order. Toxicity tests indicated that the solutions were better able to grow seeds and bacteria after treatment with the photo-Fenton process, using both types of radiation. The photo-Fenton processes carried out by employing LED and UV-C photoreactors were able to degrade the CTAB and dye mixture, thus highlighting the efficiency of LED radiation when its power (three times smaller) is compared to that of UV-C radiation. This process, therefore, represents an alternative for use in textile wastewater treatment systems.


Assuntos
Peróxido de Hidrogênio , Poluentes Químicos da Água , Compostos Azo , Cetrimônio , Ferro , Oxirredução , Ácidos Sulfanílicos , Têxteis , Triazinas
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