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1.
Fe-N co-doped coral-like hollow carbon shell (Fe-N-CS) was synthesized via a simply impregnation-pyrolysis method. The Fe-N-CS showed an excellent ability for activating peroxymonosulfate (PMS), which could degrade about 93.74% tetracycline (20 mg/L) in 12 min. The Fe-N-CS/PMS system exhibited a good anti-interference capacity of various pH, inorganic anions, HA and different water qualities. More importantly, the Fe nanoparticles were anchored uniformly in the carbon layer, effectively limiting the metal leaching. The quenching tests and electron spin resonance (ESR) manifested that non-radical singlet oxygen (1O2) was the main reactive oxygen species (ROS) for TC degradation. The mechanism study showed that Fe nanoparticles, defect and graphite N played a key role in activating PMS to produce ROS. Moreover, three probable degradation pathways were proposed by using LC-MS measurements. Generally, this work had a new insight for the synthesis of heterogeneous Fe-N-C catalysts in the advanced oxidation process based on PMS.  相似文献   

2.
A series of Sr-doped BiFeO3 perovskites (Bi1-xSrxFeO3, BSFO) fabricated via sol-gel method was applied as peroxydisulfate (PDS) activator for ciprofloxacin (CIP) degradation. Various technologies were used to characterize the morphology and physicochemical features of prepared BSFO samples and the results indicated that Sr was successfully inserted into the perovskites lattice. The catalytic performance of BiFeO3 was significantly boosted by strontium doping. Specifically, Bi0.9Sr0.1FeO3 (0.1BSFO) exhibited the highest catalytic performance for PDS activation to remove CIP, where 95% of CIP (10 mg/L) could be degraded with the addition of 1 g/L 0.1BSFO and 1 mmol/L PDS within 60 min. Moreover, 0.1BSFO displayed high reusability and stability with lower metal leaching. Weak acidic condition was preferred to neutral and alkaline conditions in 0.1BSFO/PDS system. The boosted catalytic performance can be interpreted as the lower oxidation state of Fe and the existence of affluent oxygen vacancies generated by Sr doping, that induced the formation of singlet oxygen (1O2) which was confirmed as the dominant reactive species by radical scavenging studies and electron spin resonance (ESR) tests. The catalytic oxidation mechanism related to major 1O2 and minor free radicals was proposed. Current study opens a new avenue to develop effective A-site modified perovskite and expands their application for PDS activation in wastewater remediation.  相似文献   

3.
Environment-friendly nano-catalysts capable of activating peroxymonosulfate (PMS) have received increasing attention recently. Nevertheless, traditional nano-catalysts are generally well dispersed and difficult to be separated from reaction system, so it is particularly important to develop nano-catalysts with both good catalytic activity and excellent recycling efficiency. In this work, magnetically recoverable Fe3O4-modified ternary CoFeCu-layered double hydroxides (Fe3O4/CoFeCu-LDHs) was prepared by a simple co-precipitation method and initially applied to activate PMS for the degradation of Rhodamine B (RhB). X-ray diffraction (XRD), fourier transform infrared spectrometer (FT-IR), scanning electron microscope (SEM), transmission electron microscopy (TEM), Brunauer-Emmett-Teller method (BET), and vibrating sample magnetometer (VSM) were applied to characterize morphology, structure, specific surface area and magnetism. In addition, the effects of several key parameters were evaluated. The Fe3O4/CoFeCu-LDHs exhibited high catalytic activity, and RhB degradation efficiency could reach 100% within 20 min by adding 0.2 g/L of catalyst and 1 mmol/L of PMS into 50 mg/L of RhB solution under a wide pH condition (3.0-7.0). Notably, the Fe3O4/CoFeCu-LDHs showed good super-paramagnetism and excellent stability, which could be effectively and quickly recovered under magnetic condition, and the degradation efficiency after ten cycles could still maintain 98.95%. Both radicals quenching tests and electron spin resonance (ESR) identified both HO? and SO4?? were involved and SO4?? played a dominant role on the RhB degradation. Finally, the chemical states of the sample's surface elements were measured by X-ray photoelectron spectroscopy (XPS), and the possible activation mechanism in Fe3O4/CoFeCu-LDHs/PMS system was proposed according to comprehensive analysis.  相似文献   

4.
Magnetic CuO nanosheet(Mag-CuO), as a cheap, stable, efficient and easily separated peroxymonosulfate(PMS) activator, was prepared by a simple one-step precipitation method for the removal of organic compounds from salt-containing wastewater.The experiments showed that the removal efficiencies of various organic pollutants including Acid Orange 7, Methylene Blue, Rhodamine B and atrazine in a high-salinity system(0.2 mol/L Na_2SO_4) with the Mag-CuO/PMS process were 95.81%, 74.57%, 100% and 100%,respectively.Meanwhile, Mag-CuO still maintained excellent catalytic activity in other salt systems including one or more salt components(NaCl, NaNO_3, Na_2HPO_4, NaHCO_3).A radical-quenching study and electron paramagnetic resonance analysis confirmed that singlet oxygen(~1O_2) was the dominant reactive oxygen species for the oxidation of organic pollutants in high-salinity systems, which is less susceptible to hindrance by background constituents in wastewater than radicals(~·OH or SO_4~(·-)).The surface hydroxylation of the catalyst and catalytic redox cycle including Cu and Fe are responsible for the generation of~1O_2.The developed Mag-CuO catalyst shows good application prospects for the removal of organic pollutants from saline wastewater.  相似文献   

5.
Ibuprofen(IBU),a nonsteroidal anti-inflammatory drug,is becoming an important member of pharmaceuticals and personal care products(PPCPs)as emerging pollutants.To degrade IBU,magnetic Fe_3C nanoparticles embedded on N-doped carbon(Fe_3C/NC)were prepared as a catalyst by a sol–gel combustion method.As characterized,the Fe_3C/NC nanoparticles were composed of a NC nano-sheet and capsulated Fe_3C particles on the sheet.The Fe_3C/NC nanoparticles were confirmed an efficient catalyst for peroxymonosulfate(PMS)activation to generate sulfate radicals(SO_4~(·-)),single oxygen(~1O_2)and hydroxyl radicals(·OH)toward the degradation of IBU.The added IBU(10 mg/L)was almost completely removed in 30 min by using 0.1 g/L Fe_3C/NC and 2 g/L PMS.The catalyst was confirmed to have good ability and excellent reusability through leaching measurements and cycle experiments.A catalytic mechanism was proposed for the catalytic activation of PMS on Fe_3C/NC,which involves both Fe_3C reactive sites and N-doped carbon matrix as reactive sites in Fe_3C/NC.Moreover,the degradation pathway of IBU in the Fe_3C/NC-PMS system was proposed according to the detections of degradation intermediates.  相似文献   

6.
Photooxidative removal of pharmaceuticals and organic dyes is an effective way to eliminate growing micropollutants. However, photooxidation often results in byproducts as secondary hazardous substances such as phytotoxins. Herein, we found that photooxidation of common antibiotic tetracycline hydrochloride (TCH) over a metal-free 8-hydroxyquinoline (8-HQ) functionalized carbon nitride (CN) photocatalyst significantly reduces the TCH phytotoxic effect. The phytotoxicity test of photocatalytic treated TCH-solution evaluated towards seed growth of Cicer arietinum plant model endowed natural root and shoot growth. This study highlights the conceptual insights in designing of metal-free photocatalyst for environmental remediation.  相似文献   

7.
The widely used carbamazepine(CBZ) is one of the most persistent pharmaceuticals and suffers insufficient removal efficiency by conventional wastewater treatment.A synthesized Co-based perovskite(LaCoO3) was used to activate peroxymonosulfate(PMS) in order to degrade CBZ.Results showed that LaCoO3 exhibited an excellent performance in PMS activation and CBZ degradation at neutral pH,with low cobalt leaching.The results of FT-IR and XPS verified the high structurally and che...  相似文献   

8.
Nitrogen-rich graphitized carbon microspheres (NGCs) with hierarchically porous were constructed by self-assembly. Under different heat treatment conditions, the structure, morphology and properties of NGCs were studied by using multiple characterization techniques. The results showed that the chemical microenvironments (e.g. surface chemistry, degree of graphitization and defective, etc.) and microstructures properties (e.g. morphology, specific surface area, particle size, etc.) could be delicately controlled via thermal carbonization processes. The degradation of ofloxacin (OFLX) by NGCs activated peroxymonosulfate (PMS) was studied systematically. It was found that the synergistic coupling effect between optimum N or O bonding species configuration ratio (graphitic N and C=O) and special microstructure was the main reason for the enhanced catalytic activity of NGC-800 (calcination temperature at 800°C). Electron paramagnetic resonance (EPR) experiments and radical quenching experiments indicated that the hydroxyl (?OH), sulfate (SO4??) and singlet oxygen (1O2) were contributors in the NGC-800/PMS systems. Further investigation of the durability of chemical structures and surface active sites revealed that undergo N bonding species configuration reconstruction and cannibalistic oxidation during PMS activation reaction. The used NGC-800 physicochemical properties could be recovered by heat treatment to achieve the ideal catalytic performance. The findings proposed a valuable insight for catalytic performance and controllable design of construction.  相似文献   

9.
Cobalt iron spinel (CoFe2O4) has been considered as a good heterogeneous catalysis to peroxymonosulfate (PMS) in the degradation of persistent organic pollutants due to its magnetic properties and good chemical stability. However, its catalytic activity needs to be further improved. Here, a facial strategy, “in-situ substitution”, was adopted to modify CoFe2O4 to improve its catalytic performance just by suitably increasing the Co/Fe ratio in synthesis process. Compared with CoFe2O4, the newly synthesized Co1.5Fe1.5O4, could not only significantly improve the degradation efficiency of phenol, from 50.69 to 93.6%, but also exhibited more effective mineralization ability and higher PMS utilization. The activation energy advantage for phenol degradation using Co1.5Fe1.5O4 was only 44.2 kJ/mol, much lower than that with CoFe2O4 (127.3 kJ/mol). A series of related representations of CoFe2O4 and Co1.5Fe1.5O4 were compared to explore the possible reasons for the outstanding catalytic activity of Co1.5Fe1.5O4. Results showed that Co1.5Fe1.5O4 as well represented spinel crystal as CoFe2O4 and the excess cobalt just partially replaced the position of iron without changing the original structure. Co1.5Fe1.5O4 had smaller particle size (8.7 nm), larger specific surface area (126.3 m2/g), which was more favorable for exposure of active sites. Apart from the superior physical properties, more importantly, more reactive centers Co (Ⅱ) and surface hydroxyl compounds generated on Co1.5Fe1.5O4, which might be the major reason. Furthermore, Co1.5Fe1.5O4 behaved good paramagnetism, wide range of pH suitability and strong resistance to salt interference, making it a new prospect in environmental application.  相似文献   

10.
Recently, metal-based carbon materials have been verified to be an effective persulfate activator, but secondary pollution caused by metal leaching is inevitable. Hence, a green metalfree 3D macroscopic N-doped porous carbon nanosheets(NPCN) was synthesized successfully. The obtained NPCN showed high adsorption capacity of tetracycline(TC) and excellent persulfate(PS) activation ability, especially when calcined at 700 °C(NPCN-700). The maximum adsorption capacity of NPCN-700 was 121.51 mg/g by ...  相似文献   

11.
Herein,a one-step co-pyrolysis protocol was adopted for the first time to prepare a novel pyrogenic carbon-Cu0/Fe3O4 heteroatoms (FCBC) in CO2 ambiance to discern the roles of each component in PDS activation.During co-pyrolysis,CO2 catalyzed formation of reducing gases by biomass which facilitated reductive transformation of Fe3+ and Cu2+ to Cu0 and Fe3O4,respectively.According to the a...  相似文献   

12.
Cyanide(CN-) is extensively used in the process of plating devices and for surface treatment in the electroplating industry and is extremely hazardous to humans and the environment. Peroxymonosulfate(PMS)- based advanced oxidation processes(AOPs) hold considerable promise for CN- removal. However, the activity of sulfate radical and hydroxyl radical generated in the PMS activation process is low in the base condition, leading to a drop in its efficiency in CN- re...  相似文献   

13.
Photocatalytic degradation was considered as a best strategy for the removal of antibiotic drug pollutants from wastewater. The photocatalyst of ABC (Ag2CO3/BiOBr/CdS) composite synthesized by hydrothermal and precipitation method. The ABC composite used to investigate the degradation activity of tetracycline (TC) under visible light irradiation. The physicochemical characterization methods (e.g. scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution-transmission electron microscopy (HR-TEM), ultraviolet visible spectroscopy (UV), photoluminescence (PL) and time resolved photoluminescence (TRPL) clearly indicate that the composite has been construct successfully that enhances the widened visible light absorption, induces charge transfer and separation efficiency of electron – hole pairs. The photocatalytic activity of all samples was examined through photodegradation of tetracycline in aqueous medium. The photocatalytic degradation rate of ABC catalyst could eliminate 98.79% of TC in 70 min, which is about 1.5 times that of Ag2CO3, 1.28 times that of BiOBr and 1.1 times that of BC catalyst, respectively. The role of operation parameters like, TC concentration, catalyst dosage and initial pH on TC degradation activity were studied. Quenching experiment was demonstrated that ·OH and O2· were played a key role during the photocatalysis process that was evidently proved in electron paramagnetic resonance (EPR) experiment. In addition, the catalyst showed good activity perceived in reusability and stability test due to the synergistic effect between its components. The mechanism of degradation of TC in ABC composite was proposed based on the detailed analysis. The current study will give an efficient and recyclable photocatalyst for antibiotic aqueous pollutant removal.  相似文献   

14.
In this work,hydrothermal technique combined with KOH activation were employed to develop a series of porous carbons (NPCK-x) using tobacco stem as a low-cost carbon source and (NH4)2C2O4 as a novel nitrogen-doping agent.Physicochemical properties of NPCK-x were characterized by Brunauer-Emmett-Teller,field emission scanning electron microscopy,X-ray diffraction,Raman microscope,elemental analysis,and X-ray photoelectron spectroscopy.Results showed tha...  相似文献   

15.
The extensive use of tetracycline hydrochloride (TCH) poses a threat to human health and the aquatic environment. Here, magnetic p-n Bi2WO6/CuFe2O4 catalyst was fabricated to efficiently remove TCH. The obtained Bi2WO6/CuFe2O4 exhibited 92.1% TCH degradation efficiency and 50.7% and 35.1% mineralization performance for TCH and raw secondary effluent from a wastewater treatment plant in a photo-Fenton-like system, respectively. The remarkable performance was attributed to the fact that photogenerated electrons accelerated the Fe(III)/Fe(II) and Cu(II)/Cu(I) conversion for the Fenton-like reaction between Fe(II)/Cu(I) and H2O2, thereby generating abundant ?OH for pollutant oxidation. Various environmental factors including H2O2 concentration, initial pH, catalyst dosage, TCH concentration and inorganic ions were explored. The reactive oxidation species (ROS) quenching results and electron spin resonance (ESR) spectra confirmed that ?O2? and ?OH were responsible for the dark and photo-Fenton-like systems, respectively. The degradation mechanisms and pathways of TCH were proposed, and the toxicity of products was evaluated. This work contributes a highly efficient and environmentally friendly catalyst and provides a clear mechanistic explanation for the removal of antibiotic pollutants in environmental remediation.  相似文献   

16.
Antibiotics have been identified as obesogens contributing to the prevalence of obesity. Moreover, their environmental toxicity shows sex dependence, which might also explain the sex-dependent obesity observed. Yet, the direct evidence for such a connection and the underlying mechanisms remain to be explored. In this study, the effects of tetracycline, which is a representative antibiotic found in both environmental and food samples, on Drosophila melanogaster were studied with consideration of both sex and circadian rhythms (represented by the eclosion rhythm). Results showed that in morning-eclosed adults, tetracycline significantly stimulated the body weight of females (AM females) at 0.1, 1.0, 10.0 and 100.0 µg/L, while tetracycline only stimulated the body weight of males (AM males) at 1.0 µg/L. In the afternoon-eclosed adults, tetracycline significantly stimulated the body weight of females (PM females) at 0.1, 1.0 and 100.0 µg/L, while it showed more significant stimulation in males (PM males) at all concentrations. Notably, the stimulation levels were the greatest in PM males among all the adults. The results showed the clear sex dependence of the obesogenic effects, which was diminished by dysrhythmia. Further biochemical assays and clustering analysis suggested that the sex- and rhythm-dependent obesogenic effects resulted from the bias toward lipogenesis against lipolysis. Moreover, they were closely related to the preference for the energy storage forms of lactate and glucose and also to the presence of excessive insulin, with the involvement of glucolipid metabolism. Such relationships indicated potential bridges between the obesogenic effects of pollutants and other diseases, e.g., cancer and diabetes.  相似文献   

17.
Global environmental problems have been increasing with the growth of the world economy and have become a crucial issue. To replace fossil fuels, sustainable and eco-friendly catalysts are required for the removal of organic pollutants. In this study, nickel ferrite (NiFe2O4) was prepared using a simple wet-chemical synthesis, followed by calcination; bismuth phosphate (BiPO4) was also prepared using a hydrothermal method. Further, NiFe2O4/BiPO4 nanocomposites were prepared using a hydrothermal technique. Numerous characterization studies, such as structural, morphology, surface area, optical, photoluminescence, and photoelectrochemical investigations, were used to analyze NiFe2O4/BiPO4 nanocomposites. The morphology analysis indicated a successful decoration of BiPO4 nanorods on the surface of NiFe2O4 nanoplate. Further, the bandgap of the NiFe2O4/BiPO4 nanocomposites was modified owing to the formation of a heterostructure. The as-prepared NiFe2O4/BiPO4 nanocomposite exhibited promising properties to be used as a novel heterostructure for tetracycline (TC) and Rhodamine B (RhB) removal. The NiFe2O4/BiPO4 nanocomposite degrades TC (98%) and RhB (99%) pollutants upon solar-light irradiation within 100 and 60 min, respectively. Moreover, the trapping experiments confirmed the Z-scheme approach of the prepared nanocomposites. The efficient separation and transfer of photogenerated electron-hole pairs rendered by the heterostructure were confirmed by utilizing electrochemical impedance spectroscopy, photocurrent experiments, and photoluminescence. Mott–Schottky measurements were used determine the positions of the conduction and valence bands of the samples, and the detailed mechanism of photocatalytic degradation of toxic pollutants was projected and discussed.  相似文献   

18.
Oxidation-absorption technology is a key step for NOx removal from low-temperature gas. Under the condition of low O3 concentration (O3/NO molar ratio = 0.6), F-TiO2 (F-TiO2), which is cheap and environmentally friendly, has been prepared as ozonation catalysts for NO oxidation. Catalytic activity tests performed at 120°C showed that the NO oxidation efficiency of F-TiO2 samples was higher than that of TiO2 (about 43.7%), and the NO oxidation efficiency of F-TiO2-0.15 was the highest, which was 65.3%. Combined with physicochemical characteristics of catalysts and the analysis of active species, it was found that there was a synergistic effect between F sites and oxygen vacancies on F-TiO2, which could accelerate the transformation of monomolecular O3 into multi-molecule singlet oxygen (1O2), thus promoting the selective oxidation of NO to NO2. The oxidation reaction of NO on F-TiO2-0.15 follows the Eley-Rideal mechanism, that is, gaseous NO reacts with adsorbed O3 and finally form NO2.  相似文献   

19.
In order to enhance the removal performance of graphitic carbon nitride (g-C3N4) on organic pollutant, a simultaneous process of adsorption and photocatalysis was achieved via the compounding of biochar and g-C3N4. In this study, g-C3N4 was obtained by a condensation reaction of melamine at 550°C. Then the g-C3N4/biochar composites were synthesized by ball milling biochar and g-C3N4 together, which was considered as a simple, economical, and green strategy. The characterization of resulting g-C3N4/biochar suggested that biochar and g-C3N4 achieved effective linkage. The adsorption and photocatalytic performance of the composites were evaluated with enrofloxacin (EFA) as a model pollutant. The result showed that all the g-C3N4/biochar composites displayed higher adsorption and photocatalytic performance to EFA than that of pure g-C3N4. The 50% g-C3N4/biochar performed best and removed 45.2% and 81.1% of EFA (10 mg/L) under darkness and light with a dosage of 1 mg/mL, while g-C3N4 were 19.0% and 27.3%, respectively. Besides, 50% g-C3N4/biochar showed the highest total organic carbon (TOC) removal efficiency (65.9%). Radical trapping experiments suggested that superoxide radical (?O2?) and hole (h+) were the main active species in the photocatalytic process. After 4 cycles, the composite still exhibited activity for catalytic removal of EFA.  相似文献   

20.
AgCl/ZnO/g-C3N4, a visible light activated ternary composite catalyst, was prepared by combining calcination, hydrothermal reaction and in-situ deposition processes to treat/photocatalyse tetracycline hydrochloride (TC-HCl) from pharmaceutical wastewater under visible light. The morphological, structural, electrical, and optical features of the novel photocatalyst were characterized using scanning electron microscopy (SEM), UV-visible light absorption spectrum (UV–Vis DRS), X-ray diffractometer (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and transient photocurrent techniques. All analyses confirmed that the formation of heterojunctions between AgCl/ZnO and g-C3N4 significantly increase electron-hole transfer and separation compared to pure ZnO and g-C3N4. Thus, AgCl/ZnO/g-C3N4 could exhibit superior photocatalytic activity during TC-HCl assays (over 90% removal) under visible light irradiation. The composite could maintain its photocatalytic stability even after four consecutive reaction cycles. Hydrogen peroxide (H2O2) and superoxide radical (·O2) contributed more than holes (h+) and hydroxyl radicals (·OH) to the degradation process as showed by trapping experiments. Liquid chromatograph-mass spectrometer (LC-MS) was used for the representation of the TC-HCl potential degradation pathway. The applicability and the treatment potential of AgCl/ZnO/g-C3N4 against actual pharmaceutical wastewater showed that the composite can achieve removal efficiencies of 81.7%, 71.4% and 69.0% for TC-HCl, chemical oxygen demand (COD) and total organic carbon (TOC) respectively. AgCl/ZnO/g-C3N4 can be a prospective key photocatalyst in the field of degradation of persistent, hardly-degradable pollutants, from industrial wastewater and not only.  相似文献   

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