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1.
J Environ Sci (China) ; 124: 379-396, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36182147

RESUMO

Wastewater containing an azo dye Orange G (OG) causes massive environmental pollution, thus it is critical to develop a highly effective, environmental-friendly, and reusable catalyst in peroxymonosulfate (PMS) activation for OG degradation. In this work, we successfully applied a magnetic MnFe2O4/α-MnO2 hybrid fabricated by a simple hydrothermal method for OG removal in water. The characteristics of the hybrid were investigated by X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, Brunauer-Emmett-Teller method, vibrating sample magnetometry, electron paramagnetic resonance, thermogravimetric analysis, and X-ray photoelectron spectroscopy. The effects of operational parameters (i.e., catalytic system, catalytic dose, solution pH, and temperature) were investigated. The results exhibited that 96.8% of OG degradation was obtained with MnFe2O4/α-MnO2(1:9)/PMS system in 30 min regardless of solution pH changes. Furthermore, the possible reaction mechanism of the coupling system was proposed, and the degradation intermediates of OG were identified by mass spectroscopy. The radical quenching experiments and EPR tests demonstrated that SO4•̶, O2•̶, and 1O2 were the primary reactive oxygen species responsible for the OG degradation. The hybrid also displayed unusual stability with less than 30% loss in the OG removal after four sequential cycles. Overall, magnetic MnFe2O4/α-MnO2 hybrid could be used as a high potential activator of PMS to remove orange G and maybe other dyes from wastewater.


Assuntos
Compostos de Manganês , Águas Residuárias , Compostos Azo/química , Corantes , Fenômenos Magnéticos , Compostos de Manganês/química , Óxidos , Peróxidos/química , Espécies Reativas de Oxigênio , Água
2.
Nanotechnology ; 33(47)2022 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-35926317

RESUMO

A novel silver@silver chloride/carbon nanofiber (Ag@AgCl/CNF) hybrid was synthesized by electrospinning, heat treament, and subsequentin situchemical oxidation strategy. The synthesized materials were characterized using x-ray diffraction, Fourier-transform infrared, UV-Vis diffuse reflectance spectroscopy, scanning electron microscopy, and energy dispersive x-ray. The experimental results reveal that the electrospun AgNO3/PAN was carbonized and reduced to Ag/CNF, the Ag/CNF was then partly oxidized to form Ag@AgCl/CNF in which Ag@AgCl nanoparticles (ca. 10-20 nm in diameter) were uniformly bounded to CNFs (ca. 165 nm in diameter). The obtained Ag@AgCl/CNF was employed for Na2S2O8activation under visible light irradiation to treat Rhodamine B (RhB). A remarkable RhB removal of ca. 94.68% was achieved under optimal conditions, and the influence of various parameters on removal efficiency was studied. Quenching experiments revealed that HO•, SO4•-,1O2, and O2•-were major reactive oxygen species, in which O2•-played a pivotal role in RhB degradation. A possible mechanistic route for RhB degradation was proposed.

3.
Chemosphere ; 361: 142452, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38810804

RESUMO

CuCoFe-LDO/BCD was successfully synthesized from CuCoFe-LDH and biochar derived from durian shell (BCD). Ciprofloxacin (CFX) degraded more than 95% mainly by O2•- and 1O2 in CuCoFe-LDO/BCD(2/1)/PMS system within 10 min with a rate constant of 0.255 min-1, which was 14.35 and 2.66 times higher than those in BCD/PMS and CuCoFe-LDO/PMS systems, respectively. The catalytic system exhibited good performance over a wide pH range (3-9) and high degradation efficiency of other antibiotics. Built-in electric field (BIEF) driven by large difference in the work function/Fermi level ratio between CuCoFe-LDO and BCD accelerated continuous electron transfer from CuCoFe-LDO to BCD to result in two different microenvironments with opposite charges at the interface, which enhanced PMS adsorption and activation via different directions. As a non-radical, 1O2 was mainly generated via PMS activation by C=O in BCD. The presence of C=O in BCD resulted in an increase in atomic charge of C in C=O and redistributed the charge density of other C atoms. As a result, strong adsorption of PMS at C atom in C=O and other C with a high positive charge was favorable for 1O2 generation, whereas an enhanced adsorption of PMS at negatively charged C accounted for the generation of •OH and SO4•-. After adsorption, electrons in C of BCD became deficient and were fulfilled with those transferred from CuCoFe-LDO driven by BIEF, which ensured the high catalytic activity of CuCoFe-LDO/BCD. O2•-, on the other hand, was generated via several pathways that involved in the transformation of •OH and SO4•- originated from PMS activation by the transition of metal species in CuCoFe-LDO and negatively charged C in BCD. This study proposed a new idea of fabricating a low-cost metal-LDH and biomass-derived catalyst with a strong synergistic effect induced by BIEF for enhancing PMS activation and antibiotic degradation.


Assuntos
Antibacterianos , Carvão Vegetal , Peróxidos , Carvão Vegetal/química , Antibacterianos/química , Catálise , Peróxidos/química , Ciprofloxacina/química , Óxidos/química , Cobre/química , Adsorção , Poluentes Químicos da Água/química
4.
Environ Sci Pollut Res Int ; 31(18): 26773-26789, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38456975

RESUMO

In this study, CoCr layered double hydroxide material (CoCr-LDH) was prepared and used as an effective catalyst for peroxymonosulfate (PMS) activation to degrade organics in water. The prepared CoCr-LDH material had a crystalline structure and relatively porous structure, as determined by various surface analyses. In Rhodamine B (RhB) removal, the most outstanding PMS activation ability belongs to the material with a Co:Cr molar ratio of 2:1. The removal of RhB follows pseudo-first-order kinetics (R2 > 0.99) with an activation energy of 38.23 kJ/mol and efficiency of 98% after 7 min of treatment, and the total organic carbon of the solution reduced 47.2% after 10 min. The activation and oxidation mechanisms were proposed and the RhB degradation pathways were suggested with the key contribution of O2•- and 1O2. Notably, CoCr-LDH can activate PMS over a wide pH range of 4 - 9, and apply to a wide range of organic pollutants and aqueous environments. The material has high stability and good recovery, which can be reused for 5 cycles with a stable efficiency of above 88%, suggesting a high potential for practical recalcitrant water treatment via PMS activation by heterogeneous catalysts.


Assuntos
Peróxidos , Poluentes Químicos da Água , Purificação da Água , Poluentes Químicos da Água/química , Peróxidos/química , Purificação da Água/métodos , Rodaminas/química , Cinética , Oxirredução , Catálise
5.
Chemosphere ; 287(Pt 2): 132141, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34521013

RESUMO

In this study, cobalt ferrite coated carbon felt (CoFe2O4/CF) was synthesized by solvothermal method and applied as cathode for electro-Fenton (EF) treatment of tartrazine (TTZ) in water. The materials were characterized by SEM, XRD, FTIR, CV, and EIS to explore their physical, chemical, and electrical properties. The effects of solvothermal temperature and metal content on the TTZ removal were examined, showing that 220 °C with 2 mM of Co and 4 mM of Fe precursors were the best synthesis condition. Various influencing factors such as applied current density, pH, TTZ concentration, and electrolytes were investigated, and the optimal condition was found at 8.33 mA cm-2, pH 3, 50 mgTTZ L-1, and 50 mM of Na2SO4, respectively. By radical quenching test, , 1O2, and HO were recognized as the key reactive oxygen species and the reaction mechanism was proposed for the EF decolorization of TTZ using CoFe2O4/CF cathode. The reusability and stability test showed that the highly efficient CoFe2O4/CF cathode is very promising for practical application in wastewater treatment, especially for dyes and other recalcitrant organic compounds to improve its biodegradability.


Assuntos
Carbono , Poluentes Químicos da Água , Fibra de Carbono , Eletrodos , Peróxido de Hidrogênio , Oxirredução , Tartrazina , Água , Poluentes Químicos da Água/análise
6.
RSC Adv ; 11(46): 28496-28507, 2021 Aug 23.
Artigo em Inglês | MEDLINE | ID: mdl-35478589

RESUMO

In this study, Mn2O3/MIL-100(Fe) composite was successfully synthesized by the hydrothermal method and applied for photocatalytic removal of rhodamine B (RhB) in water. The physical and chemical properties of the synthesized materials were characterized by XRD, FTIR, SEM, UV-visible, and BET analyses. Experimental results showed a great enhancement in the photocatalytic ability of the Mn2O3/MIL-100(Fe) composite as compared to individual Mn2O3 or MIL-100(Fe) under visible light and persulfate activation. The affecting factors such as pH, photocatalyst dose, RhB concentration, and Na2S2O8 concentration were investigated to find out the best conditions for efficient photocatalysis. By conducting a radical quenching test, all radicals of HO˙, SO4˙-, 1O2, and O2˙- were found to be important in photocatalytic decomposition. The mechanism was proposed for the enhancement of photocatalytic RhB removal via band potential calculation, charge separation, surface redox reaction, and key reactive oxidation species. With its durability, reusability, and high efficiency, the Mn2O3/MIL-100(Fe) composite emerges as a potential photocatalyst working under visible light for application in wastewater treatment.

7.
RSC Adv ; 10(7): 3775-3788, 2020 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-35492672

RESUMO

In this work, we report the facile hydrothermal synthesis of manganese cobaltite nanoparticles (MnCo2O4.5 NPs) which can efficiently activate peroxymonosulfate (PMS) for the generation of sulfate free radicals (SO4˙-) and degradation of organic dyes. The synthesized MnCo2O4.5 NPs have a polyhedral morphology with cubic spinel structure, homogeneously distributed Mn, Co, and O elements, and an average size less than 50 nm. As demonstrated, MnCo2O4.5 NPs showed the highest catalytic activity among all tested catalysts (MnO2, CoO) and outperformed other spinel-based catalysts for Methylene Blue (MB) degradation. The MB degradation efficiency reached 100% after 25 min of reaction under initial conditions of 500 mg L-1 Oxone, 20 mg L-1 MnCo2O4.5, 20 mg L-1 MB, unadjusted pH, and T = 25 °C. MnCo2O4.5 NPs showed a great catalytic activity in a wide pH range (3.5-11), catalyst dose (10-60 mg L-1), Oxone concentration (300-1500 mg L-1), MB concentration (5-40 mg L-1), and temperature (25-55 °C). HCO3 -, CO3 2- and particularly Cl- coexisting anions were found to inhibit the catalytic activity of MnCo2O4.5 NPs. Radical quenching experiments revealed that sulfate radicals are primarily responsible for MB degradation. A reaction sequence for the catalytic activation of PMS was proposed. The as-prepared MnCo2O4.5 NPs could be reused for at least three consecutive cycles with small deterioration in their performance due to low metal leaching. This study suggests a facile route for synthesizing MnCo2O4.5 NPs with high catalytic activity for PMS activation and efficient degradation of organic dyes.

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