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1.
J Colloid Interface Sci ; 678(Pt B): 313-324, 2024 Sep 06.
Artículo en Inglés | MEDLINE | ID: mdl-39245021

RESUMEN

The water pollution caused by the abuse of antibiotics has significant harmful effects on the environment and human health. The photo-Fenton process is currently the most effective method for removing antibiotics from water, but it encounters challenges such as inadequate response to visible light, low yield and utilization of photogenerated electrons, and slow electron transport. In this study, spin state regulation was introduced into the photo-Fenton process, and the spin state of Co3+ was regulated through Ce displacement doping. The intermediate-spin state Ce-LaCoO3 could degrade 91.6 % of tetracycline within 120 min in the photo-Fenton system, which is 15.2 % higher than that of low-spin state LaCoO3. The improved degradation effect is attributed to the reasons that Ce-LaCoO3 in the intermediate-spin state have lower band gap, better charge transfer ability, and stronger adsorption capacity of H2O2, which can accelerate the redox cycle of Co2+/Co3+ and promote the generation of ·OH. This study presents a unique strategy for synthesizing efficient photo-Fenton materials to treat antibiotic wastewater effectively.

2.
Small ; : e2406125, 2024 Sep 09.
Artículo en Inglés | MEDLINE | ID: mdl-39246214

RESUMEN

A novel Fe-g-C3N4/Bi2MoO6 (FCNB) Z-scheme heterojunction enriched with oxygen vacancy is constructed and employed for the photo-Fenton degradation of tetracycline (TC). The 2% FCNB demonstrates prominent catalytic performance and mineralization efficiency for TC wastewater, showing activity of 8.20 times greater than that of pure photocatalytic technology. Density-functional theory (DFT) calculations and degradation experiments confirm that the formation of Fe-N4 sites induces spin-polarization in the material, and the difference in Fermi energy levels results in the formation of built-in electric field at the contact interface, which facilitates the continuous generation and migration of photogenerated carriers to address the issue of insufficient cycling power of Fe (III)/Fe (II).The reactive radicals persistently target the extremely reactive sites anticipated by the Fukui function, causing the mineralization of TC molecules into "non-toxic" compounds through processes of hydroxylation, demethylation, and deamidation. This work holds significant importance in the domain of eliminating organic pollutants from water.

3.
J Environ Manage ; 369: 122406, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-39226809

RESUMEN

The key to heterogeneous photo-Fenton technology lies in the efficient generation of hydrogen peroxide (H2O2). Herein, a newly-designed ZnO/ZnIn2S4 composite with heterostructure is synthesized. Benefiting from the formation of built-in electric field, the recombination of photoinduced electrons and holes is suppressed and interfacial charge transfer resistance is reduced. Importantly, the embedding of ZnO in ZnIn2S4 can improve the hydrophobicity and create microscopic three-phase interface, thereby boosting the capture capability for O2 and providing the convenience for the occurrence of O2 reduction reaction. More interestingly, the existence of ZnIn2S4 in the ZnO/ZnIn2S4 composite can reduce the Gibbs free energy (ΔG) of key intermediate (OOH*) formation, which will accelerate the generation of H2O2. As a result, the ZnO/ZnIn2S4 composite displays excellent performance in photocatalytic H2O2 production, and the highest yield was about 897.6 µmol/g/h within 60 min under visible light irradiation. The transfer of photoinduced carriers follows the S-scheme type mechanism. The photogenerated holes can be captured by drug residues (i.e., diclofenac sodium) to accelerate H2O2 production, while generated H2O2 can combine with Fe2+ to construct photo-Fenton system for achieving the advanced degradation of diclofenac sodium, which was mainly related to the formation of OH•. Furthermore, generated H2O2 can be applied for performing the inactivation of pathogenic bacteria. In short, current work will provide a valuable reference for future research.


Asunto(s)
Restauración y Remediación Ambiental , Peróxido de Hidrógeno , Óxido de Zinc , Peróxido de Hidrógeno/química , Óxido de Zinc/química , Restauración y Remediación Ambiental/métodos , Catálisis , Adsorción , Oxígeno/química
4.
J Colloid Interface Sci ; 678(Pt B): 545-558, 2024 Sep 06.
Artículo en Inglés | MEDLINE | ID: mdl-39260302

RESUMEN

Controlling high recombination of photogenerated carriers and optimizing low cycling of metal valence states are the two key control steps in enhancing photo-Fenton oxidation. To achieve multiscale synergy of photo-Fenton degradation, graphite carbon-modified copper ferrite composites (C/CFO) with poor/rich dual electron reaction centers were synthesized through direct carbonization of Fe/Cu bimetallic organic frameworks. A novel photo-Fenton catalytic system was constructed by irradiating the Fenton reaction with visible light. The photo-Fenton degradation efficiency of C/CFO for tetracycline (100 mg‧L-1) was 93.69% ± 0.02%, and the degradation rate constant was 4.84 times higher than that of the control. Optimized preparation and catalytic conditions, ensured good cyclic stability and broad applicability of C/CFO. This excellent stability performance improvement can be attributed to the following main factors: (1) The introduction of graphite carbon not only increases the specific surface area of C/CFO, but also acts as a bridge between the dual electron reaction centers, facilitating the transfer of photogenerated electrons. (2) On the one hand, the electron-poor reaction centers Fe and Cu capture photogenerated electrons, accelerate the Fenton reaction, and realize the valence cycling of Fe and Cu. On the other hand, the electron-rich reaction centers (oxygen vacancies) act as active sites for H2O2 adsorption, which greatly accelerate the decomposition of H2O2. Overall, the synergy of dual electron reaction centers effectively promoted photo-Fenton oxidation.

5.
Chemosphere ; 365: 143347, 2024 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-39284552

RESUMEN

Improving the charge separation, charge transfer, and effective utilization is crucial in a photocatalysis system. Herein, we prepared a novel direct Z-scheme NH2-MIL-125(Ti)@FeOCl (Ti-MOF@FeOCl) composite photocatalyst through a simple method. The prepared composite catalyst was utilized in the photo-Fenton degradation of Rhodamine B (RhB) and ciprofloxacin (CIP). The Ti-MOF@FeOCl (10FeTi-MOF) catalyst exhibited the highest catalytic performance and degraded 99.1 and 66% of RhB and CIP, respectively. However, the pure NH2-MIL-125(Ti) (Ti-MOF) and FeOCl catalysts achieved only 50 and 92% of RhB and 50 and 37% of CIP, respectively. The higher catalytic activities of the Ti-MOF@FeOCl composite catalyst could be due to the electronic structure improvements, photoinduced charge separations, and charge transfer abilities in the catalyst system. The composite catalysts have also enhanced adsorption and visible light-responsive properties, allowing for efficient degradation. Furthermore, the electron paramagnetic resonance (EPR) signals, the reactive species trapping experiments, and Mott-Schottky (M - S) measurements revealed that the photogenerated superoxide radical (•O2-), hydroxyl radical (•OH), and holes (h+) played a vital role in the degradation process. The results also demonstrated that the Ti-MOF@FeOCl heterojunction composite catalysts could be a promising photo-Fenton catalyst system for the environmental remediation. Environmental implications The discharging of toxic contaminants such as organic dyes, antibiotics, and other emerging pollutants to the environment deteriorates the ecosystem. Specifically, the residues of organic pollutants recognized as a threat to ecosystem and a cause for carcinogenic effects. Among them, ciprofloxacin is one of antibiotics which has biological resistance, and metabolize partially in the human or animal bodies. It is also difficult to degrade ciprofloxacin completely with traditional treatment methods. Similarly, organic dyes are also toxic and a cause for carcinogenic effects. Therefore, effective degradation of organic pollutants such as RhB and ciprofloxacin with appropriate method is crucial.

6.
Environ Sci Technol ; 2024 Sep 29.
Artículo en Inglés | MEDLINE | ID: mdl-39344077

RESUMEN

Nitric oxide (NO) is one of the major air pollutants that may cause ecological imbalance and severe human disease. However, the removal of NO faces challenges of low efficiency, high energy consumption, and production of toxic NO2 byproducts. Herein, we report an efficient *OOH intermediate-involved NO oxidation route with high NO3- selectivity via a gas phase photo-Fenton system. Fe single atoms (Fe SAs)-anchored NH2-UiO-66(Zr) (Fe SAs@NU) was synthesized. The five-coordinated Fe SAs undergo a transient structure reconstitution during the photo-Fenton process, which enables a novel heterolytic cleavage pathway of H2O2 to derive specific ·OOH/·O2- radicals as reactive oxygen species. Therefore, a high NO (550 parts per billion) removal rate of 81% (NO3- selectivity up to 99%) is achieved under visible-light irradiation (>420 nm). This study provides new insight for the high-performance photo-Fenton process via a transient structure reconstitution pathway for the removal of gas phase NOx pollutants.

7.
J Colloid Interface Sci ; 678(Pt C): 987-1000, 2024 Sep 21.
Artículo en Inglés | MEDLINE | ID: mdl-39326170

RESUMEN

The low utilization of visible light and easy recombination of charge carriers of graphitic carbon nitride (CN) restrain its application as photo-electron donor and metal site support in photo-Fenton system. Herein, a hydrogen bond-induced supramolecular self-assembly strategy was created to fabricate an ultra-dispersed Cu-loaded porous tubular CN composite (CA-Cu/TCN) by the hydrothermal-pyrolysis method with citric acid (CA) as initiator and chelating agent. CA-Cu/TCN with rich nitrogen vacancies (NVs) and abundant ultra-dispersed CuNx sites exhibited narrow bandgap, favorable visible light absorption capability, and high separation and transfer efficiency of charge carriers. CA-Cu/TCN effectively catalyzed the activation of H2O2 for generating abundant reactive oxygen species under visible light irradiation, contributing to efficient degradation of ciprofloxacin (CIP) with removal rate of 95.9 % and kinetic rate constant of 0.0948 min-1. The superior catalytic activity of CA-Cu/TCN can be ascribed to the effective transport of photogenerated electrons, high specific surface area, atomically dispersed Cu species, and enriched surface NVs. The mechanism of photo-Fenton catalytic degradation of CIP and possible degradation pathways were proposed as the dominant role of 1O2. Toxicity evaluation of CIP and intermediates indicated that the degradation of CIP was a gradual detoxification process. This work offers a novel self-assembly strategy to design and synthesize highly active and sustainable visible light-driven photo-Fenton catalysts for effectively degrading organic pollutants.

8.
Heliyon ; 10(17): e37199, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-39319118

RESUMEN

Nowadays, water pollution generated from textile effluents is one of the major problems for the human race and ecology. Hence, development of sustainable strategies to lower the water pollution level has become a burning need. In this regard, the present study focuses on the preparation of nano catalyst NiFe2O4 to catalyze the chemical reactions on industrial organic dyes for their fast cleansing from water. By sol-gel auto-combustion technique, NiFe2O4 nanoparticles were synthesized and exposed to thermal process at temperatures of 400, 600, and 800 °C. Highly crystalline phase with spinel cubic structured NiFe2O4 was formed with a crystal size of 18.71 nm, which was confirmed by XRD analysis. The FTIR spectra showed two fundamental absorption bands in the range 597.80-412.59 cm-1, which are the characteristics of tetrahedral M - O and octahedral M - O bond in NiFe2O4. The surface morphology of calcined NiFe2O4 was investigated by scanning electron microscope (SEM). The nanoparticle size analyzer exhibited that the synthesized NiFe2O4 nanoparticles had an average particle size of ∼ 291.3 nm. Three stage decomposition patterns were observed for NiFe2O4, which was analyzed by a temperature programmed STA. Zeta potential analyzer showed that the synthesized sample S1 and S2 were stable in the dispersion medium. Also, NiFe2O4 exhibited optical band gap energies for direct band transitions within the visible spectrum measured to be 1.43-1.45 eV, rendering them effective as photocatalysts under sunlight. The samples showed magnetic measurements by VSM with saturation magnetization, coercivity, remnant magnetization value of 66.81 emu/g, 4.13 Oe and 12.94 emu/g, respectively. The synthesized photocatalyst, NiFe2O4, at 400 °C, significantly degraded three toxic organic pollutants-Methylene blue, Rhodamine B, and Congo Red-under visible light through 'Photo-Fenton' reaction mechanisms. Among the three dyes, Methylene Blue exhibited the highest degradation percentage with a rate constant of 0.0149 min-1 and followed pseudo-first-order kinetic model.

9.
Chemosphere ; 364: 143052, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39121962

RESUMEN

In recent years, antibiotic pollution has received increasing attention. Tetracycline (TC) is a commonly used antibiotic in human medicine. The presence of TC in the environment inhibits bacterial growth and enhances antibiotic resistance in organisms. In this study, MoS2/MIL101(Fe) nanocomposites are mainly constructed to remove TC pollutants using photo-fenton technology and improve the ability of photo-fenton to treat antibiotic pollutants. The system shows excellent performance for the removal of tetracycline, and the removal rate of TC by MoS2/MIL101(Fe) nanocomposite reaches 93%. Through a series of experiments such as XRD, FTIR, XPS, SEM, ESR, UV-VIS DRS, Band gap energies, photocurrent response (I-t) and Zeta potential-pH, the results show that the system promotes the Fe3+/Fe2+ cycle reaction, significantly promotes the photodecomposition of H2O2 and the formation of O2- and •OH, and broadens the pH range of the photo-fenton oxidation reaction. The combination of the metal-assisted catalyst MoS2 and the metal-organic framework MIL101(Fe) has been demonstrated to effectively enhance the ability of the Fenton reaction for the treatment of antibiotics, showcasing innovative synergy. Furthermore, the utilization of molybdenite as a substitute for MoS2 in the preparation process avoids environmental pollution associated with the synthesis of MoS2. In this study, a novel, efficient, energy-saving and environmentally friendly catalyst for the removal of tetracycline has been developed, and has a wide range of applicability.


Asunto(s)
Antibacterianos , Disulfuros , Peróxido de Hidrógeno , Hierro , Molibdeno , Nanocompuestos , Tetraciclina , Nanocompuestos/química , Tetraciclina/química , Molibdeno/química , Hierro/química , Antibacterianos/química , Peróxido de Hidrógeno/química , Disulfuros/química , Estructuras Metalorgánicas/química , Catálisis , Contaminantes Químicos del Agua/química , Oxidación-Reducción
10.
Photochem Photobiol Sci ; 23(9): 1659-1672, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39186185

RESUMEN

The catalysts with three-dimensional porous (3DP) CeO2, LaFeO3 and SrTiO3 are synthesized by sol-gel method and chemical precipitation method. The resulting multi-component 3DP CeO2/LaFeO3/SrTiO3 composite material featured a high specific surface area (26.08 m2/g), which can provide more surface active sites to improve adsorption capacity and catalytic performance. The photocatalytic, Fenton-like, photo-Fenton-like performance of the catalyst are studied on decolorization of RhB under UV irradiation, respectively. 3DP CeO2/LaFeO3/SrTiO3 exhibits high catalytic performance. Compared with photocatalytic or Fenton-like performance, 3DP CeO2/LaFeO3/SrTiO3 catalyst exhibits higher photo-Fenton-like performance, facilitating efficient decolorization of the rhodamine B. Moreover, the initial reaction rate on decolorization of RhB with 3DP CeO2/LaFeO3/SrTiO3 is 10.55, 5.52, 3.67 and 1.51 times higher than that with SrTiO3, LaFeO3, 3DP CeO2 and 3DP CeO2/LaFeO3, respectively. Meanwhile, 3DP LaFeO3/CeO2/SrTiO3 has a wider pH usage range in the synergistic reaction. Finally, a catalytic mechanism for the decolorization of rhodamine B is proposed. The continuous cycling of Fe3+/Fe2+ and Ce4+/Ce3+ and the production of active substances are achieved under the photo-Fenton-like effect of the catalyst.

11.
ChemSusChem ; : e202401471, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-39147701

RESUMEN

Highlights   S-scheme heterojunction was fabricated through in-situ solvothermal method 3D worm-like BOR and 3D rocky stone CNPO composite exhibited high photoactivity through •O2- 3D/3D junction occurred through bridging bond for efficient charge separation Waste H2O2 was turned into wealth •OH for mineralization of OTC and LVX Bi0 plasmon assisted stability and H2O2 decomposition and Ov influenced its production.

12.
Environ Technol ; : 1-12, 2024 Aug 02.
Artículo en Inglés | MEDLINE | ID: mdl-39092595

RESUMEN

This is the first record on literature to use biochar as support for CoFe2O4 to applicate and evaluate it as photocatalyst for degradation of organic pollutants. The support was verified by XRD, FT-IR, SEM, EDS and band gap. Composites CFO1BQ3, CFO1BQ1, and CFO3BQ1 showed 100% degradation in 60 min. This outstanding performance can be related to the drop in band gap energy and recombination rate of e¯/h + . The composites showed better efficiency when compared to pure CoFe2O4 (∼78%). This might be associate to the fact that biochar has a high concentration of phenolic, hydroxyl and carboxylic functional groups on its surface. In this reaction h+, O2•-, and •OH were the reactive species involved in the degradation. The toxicity of ponceau was tested before and after the treatment, through biochemical biomarkers in Danio rerio fish. In general, the treatment proved to be efficient in reducing ponceau toxicity in D. rerio fish.

13.
ACS Appl Mater Interfaces ; 16(33): 43670-43681, 2024 Aug 21.
Artículo en Inglés | MEDLINE | ID: mdl-39136272

RESUMEN

Solar-driven interfacial water evaporation (SIWE) has emerged as a promising avenue for cost-effective freshwater production from seawater or wastewater. However, the simultaneous evaporation of volatile organic compounds (VOCs) presents a limitation for the widespread implementation of this technique. Thus, developing dual-functional evaporators capable of both desalining seawater and degrading VOCs is challenging. Herein, we fabricated an iron-based metal-organic framework MIL-88A/carbon nanotubes (CNTs) poly(vinyl alcohol) hydrogel (MCH) evaporator via the conventional freezing method for solar-driven seawater desalination and simultaneous photo-Fenton VOC degradation. Because of the superior photothermal conversion capability of CNTs, reduced thermal conductivity and water evaporation enthalpy within the hydrogel, and the photo-Fenton activity of rod-shaped MIL-88A, the MCH evaporator exhibits a higher evaporation rate of 2.26 kg m-2 h-1 under 1 sun illumination with simultaneous VOC degradation. The higher hydrophilicity and vertical channels in the MCH evaporator enable its self-salt cleaning ability, facilitating consistent seawater desalination, even in high salt concentrations up to 10 wt %. The synergistic effects of localized heating from CNTs and hydrogen peroxide activation through reactive sites of MIL-88A allow the MCH evaporator to degrade more than 93% of the added phenol during evaporation. This work presents a sustainable and efficient approach for solar-driven seawater desalination, offering simultaneous VOC degradation.

14.
Heliyon ; 10(15): e35286, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-39166086

RESUMEN

Wastewater from portable toilets (WWPT) is characterized by a high content of organic matter and a variety of chemical compounds that retain bad odors, especially phenols, a type of pollutant that is difficult to degrade by conventional treatments; in addition, it is persistent, toxic, and accumulates in the aquatic environment. Although different successful experiences with the use of Photo-Fenton are reported in the scientific domain, its application in WWPT is scarce and warrants study due to the wide use of portable toilets. The objective of this study was to evaluate the Photo-Fenton oxidation process in the removal of organic matter expressed as COD in a WWPT, as well as the reduction of phenols and BOD5. The experimental runs were carried out in a 0.50 L batch reactor to evaluate the effect of the factors (H2O2: 0.019, 25.56, 40.67, 87.24, 148.91, 174.45 g L-1 and pH: 2.80, 3.00, 3.27, 4.40, 5.53, 6.00 UNT) on COD removal and sludge production. It was found that the optimum operating conditions of pH 4.72 and H2O2 dosage of 174.45 g L-1 reduced the concentration of phenols by 97.83 % and 95.49 % of COD. In addition, 98.01 % of BOD5 was reduced, resulting in a biodegradability ratio (BOD5/COD) of 0.23 compared to the untreated wastewater of 0.53. From a cost perspective, the use of Photo-Fenton to treat wastewater under these conditions would be US$ 1.15 per liter.

15.
J Colloid Interface Sci ; 677(Pt B): 882-895, 2024 Aug 21.
Artículo en Inglés | MEDLINE | ID: mdl-39173520

RESUMEN

Enhancing the velocity of the oxidation-reduction cycle is crucial for improving the catalytic efficiency of Fenton processes. Therefore, the development of an effective strategy for wastewater degradation at low temperatures is essential. In this context, we present the preparation of an NH2-MIL-88B (Fe)/CuInS2 S-scheme heterojunction. Specifically, CuInS2 nanoparticles are introduced onto the Ferro-organic skeleton, resulting in the exposure of a significant number of active surface sites. Furthermore, NH2-MIL-88B (Fe)/CuInS2 demonstrates an extended photoresponse into the long-wavelength region, which contributes to its excellent photothermal properties. Notably, the degradation rate of tetracycline in low-temperature aqueous environments reaches as high as 99.7 %, several times higher than that of the original sample. Additionally, the hydrogen production of NH2-MIL-88B (Fe)/CuInS2 is 2.23 times that of single NH2-MIL-88B (Fe) and 3.46 times that of single CuInS2. Moreover, the system exhibits good H2O2 evolution performance, forming an efficient photo-Fenton system. The charge transfer process in S-scheme heterojunction is confirmed using in-situ X-ray photoelectron spectroscopy and electron paramagnetic resonance. Both transient photoluminescence and photo electrochemical tests further validate the enhanced photoelectrochemical properties of the NH2-MIL-88B (Fe)/CuInS2 S-scheme heterojunction. The exceptional performance of this system can be attributed to the synergistic effects of the S-scheme heterojunction and the bimetallic codoped photo-Fenton system. This research presents a novel approach for the breakdown of low-temperature wastewater using an improved photocatalytic Fenton system.

16.
J Hazard Mater ; 477: 135409, 2024 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-39096636

RESUMEN

Antibiotic-resistant bacteria (ARBs) have been widely detected in wastewater and become a potential threat to human health. This work found that low-load single-atom copper (0.1 wt%) anchored on g-C3N4 (SA-Cu/g-C3N4) exhibited excellent ability to activate H2O2 and inactivate ARBs during the photo-Fenton process. The presence of SA-Cu/g-C3N4 (0.4 mg/mL) and H2O2 (0.1 mM) effectively inactivated ARBs. More than 99.9999 % (6-log) of methicillin-resistant Staphylococcus aureus (MRSA), and carbapenem-resistant Acinetobacter baumannii (CRAB) could be inactivated within 5 min. Extended-spectrum ß-lactamase-producing pathogenic Escherichia coli (ESBL-E) and vancomycin-resistant Enterococcus faecium (VRE) were killed within 10 and 30 min, respectively. In addition, more than 5-log of these ARBs were killed within 60 min in real wastewater. Furthermore, D2O-labeling with Raman spectroscopy revealed that SA-Cu/g-C3N4 completely suppressed the viable but nonculturable (VBNC) state and reactivation of bacteria. Electron paramagnetic resonance spectroscopy results demonstrated that g-C3N4 mainly produced 1O2, while SA-Cu/g-C3N4 simultaneously produced both 1O2 and •OH. The •OH and 1O2 cause lipid peroxidation damage to the cell membrane, resulting in the death of the bacteria. These findings highlight that the SA-Cu/g-C3N4 catalyst is a promising photo-Fenton catalyst for the inactivation of ARBs in wastewater.


Asunto(s)
Acinetobacter baumannii , Antibacterianos , Cobre , Peróxido de Hidrógeno , Aguas Residuales , Cobre/química , Cobre/farmacología , Antibacterianos/farmacología , Antibacterianos/química , Catálisis , Acinetobacter baumannii/efectos de los fármacos , Peróxido de Hidrógeno/química , Peróxido de Hidrógeno/farmacología , Aguas Residuales/química , Staphylococcus aureus Resistente a Meticilina/efectos de los fármacos , Farmacorresistencia Bacteriana/efectos de los fármacos , Escherichia coli/efectos de los fármacos
17.
Environ Technol ; : 1-13, 2024 Jul 13.
Artículo en Inglés | MEDLINE | ID: mdl-39002157

RESUMEN

ABSTRACTMetal-organic frameworks (MOFs) with photocatalytic activity have garnered significant attentions in environmental remediation. Herein, copper-doped zeolitic imidazolate framework-7 (Cu-doped ZIF-7) was synthesized rapidly and easily using a microwave-assisted technique. Various analytical and spectroscopic methods were employed to access the framework, morphology, light absorption, photo-electrochemical and photocatalytic performance of the synthesized materials. Compared to ZIF-7, Cu/ZIF-7 (molar ratio of Cu2+ to Zn2+ is 1:1) demonstrates superior visible light absorption ability, narrower band gap, enhanced charge separation capability, and reduced electron-hole recombination performance. Under visible light irradiation, Cu/ZIF-7 serves as a Fenton-like catalyst and demonstrates exceptional activity for contaminant degradation, while virgin ZIF-7 remains inactive. With the addition of 9.8 mmol H2O2 and exposure to visible light for 30 min, 10 mg of Cu/ZIF-7 can completely decompose RhB solution (10 mg/L, 50 mL). The synergistic effect of the Cu/ZIF-7/H2O2/visible light system is attributed to visible light photocatalysis and Fenton-like reactions. Cu/ZIF-7 demonstrates excellent catalytic performance stability, with only a slight decrease in degradation efficiency from an initial 97.0% to 95.4% over four cycles. Additionally, spin-trapping ESR measurements and active species trapping experiments revealed that h+ and ·OH occupied a significant position for Rhodamine B (RhB) degradation. Degradation intermediate products of Rhodamine B have been identified using UPLC-MS, and the degradation pathways have been proposed and discussed. This work offers a facile and efficient technique for developing MOF-based visible light photocatalysts for water purification.

18.
Molecules ; 29(13)2024 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-38999155

RESUMEN

The composite photocatalyst FeOOH/g-C3N4 was prepared through thermal polycondensation and co-precipitation methods, followed by XRD, SEM and UV-vis characterization. The stability of FeOOH/g-C3N4 was explored by the recycling test. The active species in the reaction system were investigated by the capture experiment. The results indicated that the optimal preparation condition for g-C3N4 involved calcination at 600 °C for 4 h. XRD analysis revealed that g-C3N4 exhibits a high-purity phase, and Fe in FeOOH/g-C3N4 exists in a highly dispersed amorphous state. SEM analysis showed that FeOOH/g-C3N4 has a rough surface with an irregular layered structure. Element composition analysis confirmed that the content of elements in the prepared catalyst is consistent with the theoretical calculation. FeOOH/g-C3N4 possesses the largest specific surface area of 143.2 m2/g and a suitable pore distribution. UV-vis DRS analysis showed that the absorption intensity of FeOOH/g-C3N4 is stronger than that of g-C3N4. When the catalyst dosage was 1.0 g/L, the H2O2 dosage was 4 mmol/L, the PNP initial concentration was 10 mg/L and the initial pH value was 5, the PNP removal could reach 92% in 120 min. Even after 5 cycles, the efficiency of PNP removal by FeOOH/g-C3N4 remains nearly 80%. The capture experiment indicated that both •OH and •O2- play roles in the photocatalytic degradation of PNP, with •OH being more significant. These findings affirm that FeOOH has been successfully incorporated into g-C3N4, resulting in a conspicuous catalytic effect on the degradation of PNP in the visible light-assisted Fenton-like reaction.

19.
J Hazard Mater ; 476: 135173, 2024 Sep 05.
Artículo en Inglés | MEDLINE | ID: mdl-39003812

RESUMEN

The complicated loading process and easy falling off of powder catalysts still restrict the wide application of Photo-Fenton technology in practical water treatment. In this study, a magnetic fixed film plate column water treatment equipment is designed as a visible Photo-Fenton reactor to remove levofloxacin (LEV). The effect of magnetic force can ensure that the catalyst is firmly fixed, and the multi-level shallow column plate structure achieves full contact and efficient reaction between the catalyst and wastewater. Simultaneously, the Cu0/CuFe2O4 (STCCF) utilizes Cu0 to construct an S-scheme electron transfer channel, which improves the separation efficiency of photo-generated carriers and provides sufficient photo-generated electrons for the reduction of Fe (Ⅲ) and Cu (Ⅱ). The pseudo-first-order reaction kinetic constant k for the degradation of LEV in the visible Photo-Fenton system is 0.0349 min-1, which is 15.9 times that of the photocatalytic system and 4.8 times that of the Fenton system. After continuous operation for 72 h, the magnetic fixed film plate column reactor can still remove more than 90 % of LEV and 82 % of COD in the secondary effluent of simulated antibiotic pharmaceutical wastewater treatment process, and the effluent is stable and meets the standard. The magnetic fixed film plate column reactor can be used for advanced treatment of antibiotic pharmaceutical wastewater. This study provides a new insight into the application of the Photo-Fenton process.

20.
Environ Pollut ; 360: 124635, 2024 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-39084593

RESUMEN

A lot of attention has been drawn to photo-Fenton-like catalysis among advanced oxidation processes for environmental remediation applications. Herein, we have successfully fabricated iron-nickel bimetallic magnetic nano-alloy (INBMNA) as an efficient heterogeneous photo-Fenton-like catalyst using the chemical reduction method and characterized by several analytical techniques. The characterization results show that the catalyst has a spherical shape with a mesoporous nature and contains a large specific surface area. The impact of various parameters was investigated and optimized to check the catalytic performance of INBMNAs and the found results showed that excellent photo-Fenton-like activity persisted under 6.0 pH conditions for the degradation of hazardous pollutant (phenol) under solar light exposure and microwave radiation power, respectively. Additionally, the exposed INBMNA/H2O2 system provided continuous redox cycles of Fe3+/Fe2+ and Ni2+/Ni0 pair in the Fenton-active species for stable operation. The photo-Fenton-like activity was also performed to check the effect of different inorganic anions which significantly hinder phenol reduction. Besides, the steady performance of the catalyst to remove phenol was performed in tap water and river water. Free radical trapping experiments were tested to know the role of important radicals in the photo-Fenton process. Moreover, the mechanism and possible degradation pathways of phenol were checked. By cyclic degradation experiments, the performance of the catalyst is stable and almost unchanged and can be reused several times. This study provides a promising INBMNA/H2O2 system, which encourages its widespread use in environmental remediation applications.


Asunto(s)
Peróxido de Hidrógeno , Hierro , Níquel , Fenol , Contaminantes Químicos del Agua , Hierro/química , Níquel/química , Contaminantes Químicos del Agua/química , Catálisis , Fenol/química , Peróxido de Hidrógeno/química , Oxidación-Reducción , Aleaciones/química , Restauración y Remediación Ambiental/métodos , Purificación del Agua/métodos
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