The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)...The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)degradation.The electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of CDs.Finally,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry technique.This research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.展开更多
Microplastics are persistent anthropogenic pollutants that have become a global concern due to their widespread distribution and unfamiliar threat to the environment and living organisms. Conventional technologies are...Microplastics are persistent anthropogenic pollutants that have become a global concern due to their widespread distribution and unfamiliar threat to the environment and living organisms. Conventional technologies are unable to fully decompose and mineralize plastic waste. Therefore, there is a need to develop an environmentally friendly, innovative and sustainable photocatalytic process that can destroy these wastes with much less energy and chemical consumption. In photocatalysis, various nanomaterials based on wide energy band gap semiconductors such as TiO2 and ZnO are used for the conversion of plastic contaminants into environmentally friendly compounds. In this work, the removal of plastic fragments by photocatalytic reactions using newly developed photocatalytic composites and the mechanism of photocatalytic degradation of microplastics are systematically investigated. In these degradation processes, sunlight or an artificial light source is used to activate the photocatalyst in the presence of oxygen.展开更多
A series of BiOBr@biomass carbon derived from locust leaves materials(BiOBr@BC)were fabricated and the photocatalytic property was investigated for photocatalytic degradation of rhodamine B(RhB)under visible light.The...A series of BiOBr@biomass carbon derived from locust leaves materials(BiOBr@BC)were fabricated and the photocatalytic property was investigated for photocatalytic degradation of rhodamine B(RhB)under visible light.The morphology,structure and photoelectrochemical properties of the photocatalysts were characterized by means of SEM,TEM,XRD,XPS,FT-IR,BET,PL,UV-vis/DRS,and EIS techniques.The results showed that the introduction of BC significantly enhanced the photocatalytic activity.When the content of biomass carbon(BC)in a composite is 3%(based on the mass of BiOBr),the obtained BiOBr@BC-3 exhibits excellent photocatalytic activity,degrading 99%of RhB within 20 min.The excellent degradation efficiency after the introduction of BC can be attributed to the enhanced visible light absorption,narrower band gap,and fast electron-hole pair separation rate.The photocatalytic mechanism on the degradation of RhB was illustrated based on the radicals'trapping experiments and semiconductor energy band position.The proposed material is expected to be of significant application value in the field of wastewater treatment.展开更多
Adsorption coupled with photocatalytic degradation is proposed to fulfill the removal and thorough elimination of organic dyes.Herein,we report a facile hydrothermal synthesis of MIL-100(Fe)/GO photocatalysts.The adso...Adsorption coupled with photocatalytic degradation is proposed to fulfill the removal and thorough elimination of organic dyes.Herein,we report a facile hydrothermal synthesis of MIL-100(Fe)/GO photocatalysts.The adsorption and photocatalytic degradation process of methylene blue(MB)on MIL‐100(Fe)/GO composites were systematically studied from performance and kinetic perspectives.A possible adsorption‐photocatalytic degradation mechanism is proposed.The optimized 1M8G composite achieves 95%MB removal(60.8 mg/g)in 210 min and displays well recyclability over ten cycles.The obtained MB adsorption and degradation results are well fitted onto Langmuir isotherm and pseudo‐second order kinetic model.This study shed light on the design of MOFs based composites for water treatment.展开更多
With the growing concern about the water environment,the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic micropollutan...With the growing concern about the water environment,the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic micropollutants.In this work,to overcome the drawbacks of the photocatalytic activity reduction caused by the photo-corrosion of non-stoichiometric BiO_(2–x),a novel material with amorphous FeOOH in situ grown on layered BiO_(2–x) to form a core-shell structure similar to popcorn chicken-like morphology was produced in two simple and environmentally beneficial steps.Through a series of degradation activity tests of hybrid materials under different conditions,the as-prepared materials exhibited remarkable degradation activity and stability toward tetracycline in the FeOOH@BiO_(2–x)/Vis/PS system due to the synergism of photocatalysis and persulfate activation.The results of XRD,SEM,TEM,XPS,FTIR,and BET show that the loading of FeOOH increases the specific surface area and active sites appreciably;the heterogeneous structure formed by FeOOH and BiO_(2–x) is more favorable to the effective separation of photogenerated carriers.The optimal degradation conditions were at a catalyst addition of 0.7 g·L^(–1),a persulfate concentration of 1.0 g·L^(–1),and an initial pH of 4.5,at which the degradation rate could reach 94.7%after 90 min.The influence of typical inorganic anions on degradation was also examined.ESR studies and radical quenching experiments revealed that·OH,SO_(4)^(-)·,and·O_(2)^(-)were the principal active species generated during the degradation of tetracycline.The results of the 1,10-phenanthroline approach proved that the effect of dissolved iron ions on the tetracycline degradation was limited,and the interfacial reaction that occurs on the active sites on the material's surface was a critical factor.This work provides a novel method for producing efficient broad-spectrum Bismuth-based composite photocatalysts and photocatalytic-activated persulfate synergistic degradation of tetracycline.展开更多
Deep degradation of organic pollutants by sunlight-induced coupled photocatalytic and Fenton (photo-Fenton) reactions is of immense importance for water purification. In this work, we report a novel bifunctional catal...Deep degradation of organic pollutants by sunlight-induced coupled photocatalytic and Fenton (photo-Fenton) reactions is of immense importance for water purification. In this work, we report a novel bifunctional catalyst (Fe-PEI-CN) by codoping graphitic carbon nitride (CN) with polyethyleneimine ethoxylated (PEI) and Fe species, which demonstrated high activity during p-chlorophenol (p-ClPhOH) degradation via H_(2)O_(2) from the photocatalytic process. The relationship between the catalytic efficiency and the structure was explored using diff erent characterization methods. The Fe modification of CN was achieved through Fe-N coordination, which ensured high dispersion of Fe species and strong stability against leaching during liquid- phase reactions. The Fe modification initiated the Fenton reaction by activating H_(2)O_(2) into ·OH radicals for deep degradation of p-ClPhOH. In addition, it eff ectively promoted light absorption and photoelectron-hole (e-h ^(+) ) separation, corresponding to improved photocatalytic activity. On the other hand, PEI could significantly improve the ability of CN to generate H_(2)O_(2) through visible light photocatalysis. The maximum H_(2)O_(2) yield reached up to 102.6 μmol/L, which was 22 times higher than that of primitive CN. The cooperation of photocatalysis and the self-Fenton reaction has led to high-activity mineralizing organic pollutants with strong durability, indicating good potential for practical application in wastewater treatment.展开更多
TiO_(2) nanobelts and Co_(3)O_(4)/TiO_(2) catalytic materials were prepared using the hydrothermal method.The cat-alyst was characterized by X-ray diffraction,scanning electron microscopy,transmission electron microsc...TiO_(2) nanobelts and Co_(3)O_(4)/TiO_(2) catalytic materials were prepared using the hydrothermal method.The cat-alyst was characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,X-ray electron spectroscopy,and fluorescence spectroscopy.At room temperature,with a relative humidity of 50.0%,the total gas flow rate of 1.0 L·min-1,the space velocity of 1.05×10^(4) h^(-1),and toluene volume concentration of 25.0µL·L^(-1),two 6 W vacuum ultraviolet lamps were used as light sources to catalyze,degrade,and mineralize toluene.The results show that the prepared catalyst is in the shape of nano-ribbons.The loading of Co_(3)O_(4) inhibits the recombina-tion of photogenerated electrons and holes and can effectively improve the catalytic performance.The Co_(3)O_(4)/TiO_(2) with a load of 6.0%Co_(3)O_(4) has the best catalytic effect.When N2 was used as a carrier gas,the degradation rate of tol-uene was only 34.7%.The toluene degradation is mainly due to the photolysis of vacuum ultraviolet light.When air was used as a carrier gas,O_(3) was produced.The Co_(3)O_(4)/TiO_(2) with a load of 6.0%and vacuum ultraviolet synergistical-ly promote toluene degradation.The highest degradation rate of toluene was 91.7%and the mineralization rate was 74.6%.The degradation rate of toluene was 2.6 times that of nitrogen as a carrier gas.展开更多
With the significant discharge of antibiotic wastewater into the aquatic and terrestrial ecosystems, antibiotic pollution has become a serious problem and presents a hazardous risk to the environment. To address such ...With the significant discharge of antibiotic wastewater into the aquatic and terrestrial ecosystems, antibiotic pollution has become a serious problem and presents a hazardous risk to the environment. To address such issues, various investigations on the removal of antibiotics have been undertaken. Photocatalysis has received tremendous attention owing to its great potential in removing antibiotics from aqueous solutions via a green, economic, and effective process. However, such a technology employing traditional photocatalysts suffers from major drawbacks such as light absorption being restricted to the UV spectrum only and fast charge recombination. To overcome these issues, considerable effort has been directed towards the development of advanced visible light-driven photocatalysts. This mini review summarises recent research progress in the state-of-the-art design and fabrication of photocatalysts with visible-light response for photocatalytic degradation of antibiotic wastewater. Such design strategies involve the doping of metal and non-metal into ultraviolet light-driven photocatalysts, development of new semiconductor photocatalysts, construction of heterojunction photocatalysts, and fabrication of surface plasmon resonance-enhanced photocatalytic systems. Additionally, some perspectives on the challenges and future developments in the area of photocatalytic degradation of antibiotics are provided.展开更多
In order to explore the reaction mechanism of Fe^3+ and the mineralization effect of the micropollutant, Fe^3+ assisted photocatalytic oxidation of sulfadiazine (SD) in the TiO2 suspended solution is investigated....In order to explore the reaction mechanism of Fe^3+ and the mineralization effect of the micropollutant, Fe^3+ assisted photocatalytic oxidation of sulfadiazine (SD) in the TiO2 suspended solution is investigated. The effect of Fe^3+ participation, the degradation kinetics of SD, the effect of SD mineralization and the possible mechanism of Fe^3+ participation in TiO2 suspension are analyzed by adding FeCl3, taking samples at a given time and determining the SD concentration. Results indicate that the degradation of SD catalyzed by TiO2/ Fe^3+ is faster than that catalyzed by TiO2 or Fe^3+ separately. The photocatalytic degradation of SD follows the pseudo-first- order kinetics model in a range of 20 to 80 mg/L of initial concentration. The mineralization rate of SD can be enhanced by the addition of Fe^3+ in the TiO2 suspended solution. The mechanism of the rapid degradation of SD is proposed, which indicates that Fe^3+ adsorbed on the surface of TiO2 particles acts as an electron acceptor. The amount of recombining electronhole pairs decreases, and the amount of hydroxyl radicals increases. The increased hydroxyl radical strengthens the degradation of SD in the TiO2/Fe^3+ suspended solution.展开更多
ZnO/Znml2O4 nanocomposites with heteronanostructures were successfully prepared by co-precipitation method. The as-prepared samples were characterized by HRTEM, TEM, XRD, BET, TG-DTA, and UV-Vis spectra techniques. Th...ZnO/Znml2O4 nanocomposites with heteronanostructures were successfully prepared by co-precipitation method. The as-prepared samples were characterized by HRTEM, TEM, XRD, BET, TG-DTA, and UV-Vis spectra techniques. The photoeatalytic activities of the as-prepared samples were evaluated by the photocatalytic degradation of methyl orange and inactivation of Escherichia coli in suspension under the irradiation of the simulated sunlight. The effects of compositions, calcination temperatures, concentration ofphotocatalysts and light source on the photocatalytic activities were systematically studied. The results show that when the concentration of ZnO/ZnA1204 photocatalyst with the starting Zn to Al molar ratio of 1:1.5 calcined at 600 ℃ is 1.0 g/L, the maximum photocatalytic degradation rate of 98.5% can be obtained in 50 min under the irradiation of the simulated sunlight. Under the same conditions, an inactivation rate of 99.8% for E.coli is achieved in 60 min.展开更多
Pervoskite type oxides LaCoO 3 was prepared by citrate method with the granula of 20 nm-30 nm. With a fluorescent Hg lamp or sunlight as irradiator, the degradation experiments of various water soluble dyes we...Pervoskite type oxides LaCoO 3 was prepared by citrate method with the granula of 20 nm-30 nm. With a fluorescent Hg lamp or sunlight as irradiator, the degradation experiments of various water soluble dyes were carried out in the suspension system of LaCoO 3 . The results show that the pervoskite type oxide LaCoO 3 has good photocatalytic activity.Studied by X ray photoelectron spectroscopy and photoacoustic spectra, its photocatalytic activity is found to be related with factors such as the d electron structure of ion Co 3+ ,Co—O binding energy and adsorbed oxygen on the surface etc.展开更多
A multifunctional Cu2O/Ag micro-nanocomposite, which has the characteristics of high cat- alytic activities under the visible light and high surface-enhanced Raman scattering (SERS) activity, was fabricated via a fa...A multifunctional Cu2O/Ag micro-nanocomposite, which has the characteristics of high cat- alytic activities under the visible light and high surface-enhanced Raman scattering (SERS) activity, was fabricated via a facile method and employed for the in situ SERS monitoring of the photocatalytic degradation reaction of crystal violet. Through the variation of the AgNO3 concentration, Ag content on the Cu2O template can be controllably tuned, which has great influence on the SERS effect. The results indicate that Ag nanopartieles form on the Cu2O nanoframes to obtain the Cu2O/Ag nanoeomposite, which can act as an excellent bifunetional platform for in situ monitoring of photocatalytic degradation of organic pollutions by SERS.展开更多
Titania-based composite catalysts were prepared through a sol-gel route employing multi-walled carbon nanotubes with different diameters. The materials were characterized using thermogravimetric analysis, nitrogen ads...Titania-based composite catalysts were prepared through a sol-gel route employing multi-walled carbon nanotubes with different diameters. The materials were characterized using thermogravimetric analysis, nitrogen adsorption-desorption isotherm, powder X-ray diffraction, scanning electron microscopy, and diffuse reflectance UV-Vis absorption spectra. The application of the catalysts to photocatalytic degradation of phenol was tested under UV-Vis irradiation. A synergetic effect on phenol removal was observed in case of composite catalysts, which was evaluated in terms of apparent rate constant, total organic carbon removal and photonic efficiency.展开更多
Bacillus thuringiensis(Bt)cotton production is challenged by two main problems,i.e.,the low concentration of Bt protein at the boll setting stage and the lowest insect resistance in bolls among all the cotton plant’s...Bacillus thuringiensis(Bt)cotton production is challenged by two main problems,i.e.,the low concentration of Bt protein at the boll setting stage and the lowest insect resistance in bolls among all the cotton plant’s organs.Therefore,increasing the Bt protein concentration at the boll stage,especially in bolls,has become the main goal for increasing insect resistance in cotton.In this study,two protein degradation inhibitors(ethylene diamine tetra acetic acid(EDTA)and leupeptin)were sprayed on the bolls,subtending leaves,and whole cotton plants at the peak flowering stage of two Bt cultivars(medium maturation Sikang 1(SK1))and early maturation Zhongmian 425(ZM425)in 2019 and 2020.The Bt protein content and protein degradation metabolism were assessed.The results showed that the Bt protein concentrations were enhanced by 21.3 to 38.8%and 25.0 to 38.6%in the treated bolls of SK1 and ZM425 respectively,while they were decreased in the subtending leaves of these treated bolls.In the treated leaves,the Bt protein concentrations increased by 7.6 to 23.5%and 11.2 to 14.9%in SK1 and ZM425,respectively.The combined application of EDTA and leupeptin to the whole cotton plant increased the Bt protein concentrations in both bolls and subtending leaves.The Bt protein concentrations in bolls were higher,increasing by 22.5 to 31.0%and 19.6 to 32.5%for SK1 and ZM425,respectively.The organs treated with EDTA or/and leupeptin showed reduced free amino acid contents,protease and peptidase activities and significant enhancements in soluble protein contents.These results indicated that inhibiting protein degradation could improve the protein content,thus increasing the Bt protein concentrations in the bolls or/and leaves of cotton plants.Therefore,the increase in the Bt protein concentration without yield reduction suggested that these two protein degradation inhibitors may be applicable for improving insect resistance in cotton production.展开更多
The degradation of phenol was carried out using heterogeneous Fenton-type catalysts in the presence of H_2O_2 and UV. Catalysts were prepared by exchanging and immobilizing Fe 2+ in zeolite 13X, silica gel or Al_2O...The degradation of phenol was carried out using heterogeneous Fenton-type catalysts in the presence of H_2O_2 and UV. Catalysts were prepared by exchanging and immobilizing Fe 2+ in zeolite 13X, silica gel or Al_2O_3. The concentration of phenol solution was 100 mg/L. The amount of H_2O_2 added was the stoichiometric amount of H_2O_2 required for the total oxidation of phenol. Under the irradiation of medium pressure light (300 W) phenol was mineralized within 1 h in the presence of Fe 2+/zeolite 13X. The COD removal rate was enhanced in the presence of Fe 2+/zeolite 13X compared to that of Fe 2+/silica gel or Fe 2+/Al_2O_3. Analogous homogenous photo-Fenton reaction with equivalent Fe 2+ was also carried out to evaluate the catalysis efficiency of Fe 2+/zeolite 13X. Results showed that the COD removal rate was near to that of homogeneous Fenton, while heterogeneous Fe 2+/zeolite 13X catalyst could be recycled.展开更多
Photocatalytic degradation of phenol selected as model compound of organic pollutant had been investigated in aqueous titanium dioxide (TiO2) dispersion under UV irradiation. The effects of various parameters such a...Photocatalytic degradation of phenol selected as model compound of organic pollutant had been investigated in aqueous titanium dioxide (TiO2) dispersion under UV irradiation. The effects of various parameters such as pH, catalyst concentration, phenol concentration, anions, metal ions, electron acceptors, and surfactants on the photocatalytic degradation of phenol were investigated. The degradation kinetics was determined by the change in phenol concentration employing UV-Vis spectrometry as a function of irradiation time. The degradation kinetics of phenol follows pseudo first-order kinetics. The results showed a significant dependence of the photocatalytic degradation of phenol on the functional parameters. The probable promising roles of the additives on the degradation process were discussed.展开更多
The photocatalytic degradation of Rhodamine B (RhB) was carried out using TiO2 supported on activated carbon (TiO2-AC) under microwave irradiation. Composite catalyst TiO2-AC was prepared and characterized using X...The photocatalytic degradation of Rhodamine B (RhB) was carried out using TiO2 supported on activated carbon (TiO2-AC) under microwave irradiation. Composite catalyst TiO2-AC was prepared and characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM) and Brunauer-Emmett-Teller (BET). In the process of microwave-enhanced photocatalysis (MPC), RhB (30 mg/L) was almost completely decoloured in 10 min, and the mineralization efficiency was 96.0% in 20 min. The reaction rate constant of RhB in MPC using TiO2-AC by pseudo first-order reaction kinetics was 4.16 times of that using Degussa P25. Additionally, according to gas chromatography/mass spectrometry (GC/MS) and liquid chromatography/mass spectrometry (LC/MS) identification, the major intermediates of RhB in MPC included two kinds of N-de-ethylation intermediates (N,N-diethyl-N'-ethyl-rhodamine (DER)), oxalic acid, malonic acid, snccinic acid, and phthalic acid, maleic acid, 3-nitrobenzoic acid, and so on. The degradation of RhB in MPC was mainly attributed to the destruction of the conjugated structure, and then the intermediates transformed to acid molecules which were mineralized to water and carbon dioxide.展开更多
Kinetic processes of a-naphthaleneacetic acid (NAA) photolysis were studied under different conditions. The results showed that the ultraviolet light was more effective than fluorescent light in promoting degradation,...Kinetic processes of a-naphthaleneacetic acid (NAA) photolysis were studied under different conditions. The results showed that the ultraviolet light was more effective than fluorescent light in promoting degradation, and the degradation of NAA under ultraviolet light followed the first order kinetics with the photolysis rate constant of 1.15 x 10-2 min-1 and half-life time (t1/2) of 60 min. Further, it was proved that the photolysis rate was higher in the presence of oxygen, titanium dioxide (TiO2), and low pH (acidic solution). At last, two photolysis intermediates were identified by GC-MS and possible photolysis pathways were proposed.展开更多
Anatase TiO2 films were successfully prepared on foam nickel substrates by sol-gel technique using tetrabutyl titanate as precursor. The characteristics of the TiO2 films were investigated by XPS, XRD, FE-SEM, TEM and...Anatase TiO2 films were successfully prepared on foam nickel substrates by sol-gel technique using tetrabutyl titanate as precursor. The characteristics of the TiO2 films were investigated by XPS, XRD, FE-SEM, TEM and UV-Vis absorption spectra. The photocatalytic activities of TiO2 films were investigated by photocatalytic degradation reactions of gaseous acetaldehyde, an indoor pollutant, under ultraviolet light irradiation. It was found that Ni^2+ doping into TiO2 films due to the foam nickel substrates resulted in the extension of absorption edges of TiO2 films from UV region to visible light region. The pre-heating for foam nickel substrates resulted in the formation of NiO layer, which prevented effectively the injection of photogenerated electrons from TiO2 films to metal nickel. The TiO2 films displayed high photocatalytic activity for the degradation of acetaldehyde, and were enhanced by calcining the substrates and coating TiO2 films repeatedly. The high activity was mainly attributed to the improvement of the characteristics of substrate surface and the increase of active sites on photocatalyst.展开更多
The photocatalytic degradation of dye pollutant sulforhodamine-B (SRB) in aqueous titanium dioxide (TiO2) dispersions was examined under three lighting regimes: UV light (330 nm〈λ〈 380 nm), sunlight, and vis...The photocatalytic degradation of dye pollutant sulforhodamine-B (SRB) in aqueous titanium dioxide (TiO2) dispersions was examined under three lighting regimes: UV light (330 nm〈λ〈 380 nm), sunlight, and visible light (λ〉450 nm), all investigated at pH=2.5. Total organic carbon (TOC) and chemical oxygen demand (CODer) assays show that the degradation rate of SRB is much higher when irradiated with UV and sunlight compared with visible light. The temporal concentration changes of SRB illustrated a first-order reaction and the rate constant, k, is 0.197 min^-1, 0.152 min^-1, 0.027 min^-1, respectively, under the three lighting conditions. The final mineralized products were amine compounds identified by infrared spectrophotometry. When irradiated with visible light, the photocatalytic degradation rate could be improved by lowering the H2O2 concentration and inhibited by increasing the H2O2 concentration, but results contrary to the above were obtained when UV light was used for irradiation.展开更多
基金the funding support from the National Natural Science Foundation of China(21906072,22006057)the Natural Science Foundation of Jiangsu Province(BK20190982)“Doctor of Mass entrepreneurship and innovation”Project in Jiangsu Province。
文摘The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)degradation.The electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of CDs.Finally,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry technique.This research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.
文摘Microplastics are persistent anthropogenic pollutants that have become a global concern due to their widespread distribution and unfamiliar threat to the environment and living organisms. Conventional technologies are unable to fully decompose and mineralize plastic waste. Therefore, there is a need to develop an environmentally friendly, innovative and sustainable photocatalytic process that can destroy these wastes with much less energy and chemical consumption. In photocatalysis, various nanomaterials based on wide energy band gap semiconductors such as TiO2 and ZnO are used for the conversion of plastic contaminants into environmentally friendly compounds. In this work, the removal of plastic fragments by photocatalytic reactions using newly developed photocatalytic composites and the mechanism of photocatalytic degradation of microplastics are systematically investigated. In these degradation processes, sunlight or an artificial light source is used to activate the photocatalyst in the presence of oxygen.
基金the National Natural Science Foundation of China(51572185)Natural Science Foundation of Shanxi Province(202203021211158 and 20210302123176)+1 种基金the Key Research&Development Program of Shanxi Province(Social Development,201903D321060)the Key Research&Development program of Shanxi Province(International Cooperation,201903D421079)for the financial support.
文摘A series of BiOBr@biomass carbon derived from locust leaves materials(BiOBr@BC)were fabricated and the photocatalytic property was investigated for photocatalytic degradation of rhodamine B(RhB)under visible light.The morphology,structure and photoelectrochemical properties of the photocatalysts were characterized by means of SEM,TEM,XRD,XPS,FT-IR,BET,PL,UV-vis/DRS,and EIS techniques.The results showed that the introduction of BC significantly enhanced the photocatalytic activity.When the content of biomass carbon(BC)in a composite is 3%(based on the mass of BiOBr),the obtained BiOBr@BC-3 exhibits excellent photocatalytic activity,degrading 99%of RhB within 20 min.The excellent degradation efficiency after the introduction of BC can be attributed to the enhanced visible light absorption,narrower band gap,and fast electron-hole pair separation rate.The photocatalytic mechanism on the degradation of RhB was illustrated based on the radicals'trapping experiments and semiconductor energy band position.The proposed material is expected to be of significant application value in the field of wastewater treatment.
基金National Natural Science Foundation of China(Grant No.21902001,22179001)Distinguished Young Research Project of Anhui Higher Education Institution(Grant No.2022AH020007)+1 种基金University Synergy Innovation Program of Anhui Province(Grant No.GXXT-2023-009)Higher Education Natural Science Foundation of Anhui Province(Grant No.2023AH050114).
文摘Adsorption coupled with photocatalytic degradation is proposed to fulfill the removal and thorough elimination of organic dyes.Herein,we report a facile hydrothermal synthesis of MIL-100(Fe)/GO photocatalysts.The adsorption and photocatalytic degradation process of methylene blue(MB)on MIL‐100(Fe)/GO composites were systematically studied from performance and kinetic perspectives.A possible adsorption‐photocatalytic degradation mechanism is proposed.The optimized 1M8G composite achieves 95%MB removal(60.8 mg/g)in 210 min and displays well recyclability over ten cycles.The obtained MB adsorption and degradation results are well fitted onto Langmuir isotherm and pseudo‐second order kinetic model.This study shed light on the design of MOFs based composites for water treatment.
基金supported by the National Key Research and Development Program of China(2019YFC1904100)the National Natural Science Foundation of China(21503144)+3 种基金the Science and Technology Innovation Project for Students of Hebei Province(22E50174D)the Science and Technology Project of Hebei Education Department(QN2021047)the Program of Hebei Vocational University of Industry and Technology(dxs202207,ZY202401)the Key Program of Natural Science of Hebei Province(B2020209017).
文摘With the growing concern about the water environment,the advanced oxidation process of persulfate activation assisted by photocatalysis has attracted considerable attention to decompose dissolved organic micropollutants.In this work,to overcome the drawbacks of the photocatalytic activity reduction caused by the photo-corrosion of non-stoichiometric BiO_(2–x),a novel material with amorphous FeOOH in situ grown on layered BiO_(2–x) to form a core-shell structure similar to popcorn chicken-like morphology was produced in two simple and environmentally beneficial steps.Through a series of degradation activity tests of hybrid materials under different conditions,the as-prepared materials exhibited remarkable degradation activity and stability toward tetracycline in the FeOOH@BiO_(2–x)/Vis/PS system due to the synergism of photocatalysis and persulfate activation.The results of XRD,SEM,TEM,XPS,FTIR,and BET show that the loading of FeOOH increases the specific surface area and active sites appreciably;the heterogeneous structure formed by FeOOH and BiO_(2–x) is more favorable to the effective separation of photogenerated carriers.The optimal degradation conditions were at a catalyst addition of 0.7 g·L^(–1),a persulfate concentration of 1.0 g·L^(–1),and an initial pH of 4.5,at which the degradation rate could reach 94.7%after 90 min.The influence of typical inorganic anions on degradation was also examined.ESR studies and radical quenching experiments revealed that·OH,SO_(4)^(-)·,and·O_(2)^(-)were the principal active species generated during the degradation of tetracycline.The results of the 1,10-phenanthroline approach proved that the effect of dissolved iron ions on the tetracycline degradation was limited,and the interfacial reaction that occurs on the active sites on the material's surface was a critical factor.This work provides a novel method for producing efficient broad-spectrum Bismuth-based composite photocatalysts and photocatalytic-activated persulfate synergistic degradation of tetracycline.
基金the National Key Research and Development Program of China (No. 2020YFA0211004)Key Grant of Nation Science Funding of China (No. 22236005)+5 种基金Nation Science Funding of China (No. 22376141)Ministry of Education of China (No. PCSIRT_IRT_16R49)“111” Innovation and Talent Recruitment Base (D18020)Shanghai Government (No. 20ZR1440700)Shanghai Engineering Research Center of Green Energy Chemical Engineering (No. 18DZ2254200)Scientific and Technological Innovation Team for Green Catalysis and Energy Materialien Yunnan Institutions of Higher Learning, and Surface project of Yunnan Province science and technology Department (No. 20210 A070001-050).
文摘Deep degradation of organic pollutants by sunlight-induced coupled photocatalytic and Fenton (photo-Fenton) reactions is of immense importance for water purification. In this work, we report a novel bifunctional catalyst (Fe-PEI-CN) by codoping graphitic carbon nitride (CN) with polyethyleneimine ethoxylated (PEI) and Fe species, which demonstrated high activity during p-chlorophenol (p-ClPhOH) degradation via H_(2)O_(2) from the photocatalytic process. The relationship between the catalytic efficiency and the structure was explored using diff erent characterization methods. The Fe modification of CN was achieved through Fe-N coordination, which ensured high dispersion of Fe species and strong stability against leaching during liquid- phase reactions. The Fe modification initiated the Fenton reaction by activating H_(2)O_(2) into ·OH radicals for deep degradation of p-ClPhOH. In addition, it eff ectively promoted light absorption and photoelectron-hole (e-h ^(+) ) separation, corresponding to improved photocatalytic activity. On the other hand, PEI could significantly improve the ability of CN to generate H_(2)O_(2) through visible light photocatalysis. The maximum H_(2)O_(2) yield reached up to 102.6 μmol/L, which was 22 times higher than that of primitive CN. The cooperation of photocatalysis and the self-Fenton reaction has led to high-activity mineralizing organic pollutants with strong durability, indicating good potential for practical application in wastewater treatment.
文摘TiO_(2) nanobelts and Co_(3)O_(4)/TiO_(2) catalytic materials were prepared using the hydrothermal method.The cat-alyst was characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,X-ray electron spectroscopy,and fluorescence spectroscopy.At room temperature,with a relative humidity of 50.0%,the total gas flow rate of 1.0 L·min-1,the space velocity of 1.05×10^(4) h^(-1),and toluene volume concentration of 25.0µL·L^(-1),two 6 W vacuum ultraviolet lamps were used as light sources to catalyze,degrade,and mineralize toluene.The results show that the prepared catalyst is in the shape of nano-ribbons.The loading of Co_(3)O_(4) inhibits the recombina-tion of photogenerated electrons and holes and can effectively improve the catalytic performance.The Co_(3)O_(4)/TiO_(2) with a load of 6.0%Co_(3)O_(4) has the best catalytic effect.When N2 was used as a carrier gas,the degradation rate of tol-uene was only 34.7%.The toluene degradation is mainly due to the photolysis of vacuum ultraviolet light.When air was used as a carrier gas,O_(3) was produced.The Co_(3)O_(4)/TiO_(2) with a load of 6.0%and vacuum ultraviolet synergistical-ly promote toluene degradation.The highest degradation rate of toluene was 91.7%and the mineralization rate was 74.6%.The degradation rate of toluene was 2.6 times that of nitrogen as a carrier gas.
基金supported by the National Natural Science Foundation of China(21421001,21276116,21477050,21301076,21303074)Natural Science Foundation of Jiangsu Province(BK20140530,BK20150482)+5 种基金China Postdoctoral Science Foundation(2015M570409)Chinese-German Cooperation Research Project(GZ1091)Program for High-Level Innovative and Entrepreneurial Talents in Jiangsu ProvinceProgram for New Century Excellent Talents in University(NCET-13-0835)Henry Fok Education Foundation(141068)Six Talents Peak Project in Jiangsu Province(XCL-025)~~
文摘With the significant discharge of antibiotic wastewater into the aquatic and terrestrial ecosystems, antibiotic pollution has become a serious problem and presents a hazardous risk to the environment. To address such issues, various investigations on the removal of antibiotics have been undertaken. Photocatalysis has received tremendous attention owing to its great potential in removing antibiotics from aqueous solutions via a green, economic, and effective process. However, such a technology employing traditional photocatalysts suffers from major drawbacks such as light absorption being restricted to the UV spectrum only and fast charge recombination. To overcome these issues, considerable effort has been directed towards the development of advanced visible light-driven photocatalysts. This mini review summarises recent research progress in the state-of-the-art design and fabrication of photocatalysts with visible-light response for photocatalytic degradation of antibiotic wastewater. Such design strategies involve the doping of metal and non-metal into ultraviolet light-driven photocatalysts, development of new semiconductor photocatalysts, construction of heterojunction photocatalysts, and fabrication of surface plasmon resonance-enhanced photocatalytic systems. Additionally, some perspectives on the challenges and future developments in the area of photocatalytic degradation of antibiotics are provided.
基金The Priority Academic Program Development of Jiangsu Higher Education Institutions (No. 1105007001 )the Ph. D. Programs Foundation of Ministry of Education of China (No. 20100092120018)the Natural Science Foundation of Jiangsu Province (No. BK2009453)
文摘In order to explore the reaction mechanism of Fe^3+ and the mineralization effect of the micropollutant, Fe^3+ assisted photocatalytic oxidation of sulfadiazine (SD) in the TiO2 suspended solution is investigated. The effect of Fe^3+ participation, the degradation kinetics of SD, the effect of SD mineralization and the possible mechanism of Fe^3+ participation in TiO2 suspension are analyzed by adding FeCl3, taking samples at a given time and determining the SD concentration. Results indicate that the degradation of SD catalyzed by TiO2/ Fe^3+ is faster than that catalyzed by TiO2 or Fe^3+ separately. The photocatalytic degradation of SD follows the pseudo-first- order kinetics model in a range of 20 to 80 mg/L of initial concentration. The mineralization rate of SD can be enhanced by the addition of Fe^3+ in the TiO2 suspended solution. The mechanism of the rapid degradation of SD is proposed, which indicates that Fe^3+ adsorbed on the surface of TiO2 particles acts as an electron acceptor. The amount of recombining electronhole pairs decreases, and the amount of hydroxyl radicals increases. The increased hydroxyl radical strengthens the degradation of SD in the TiO2/Fe^3+ suspended solution.
基金Project(21271071)supported by the National Natural Science Foundation of ChinaProject(21306041)supported by the National Natural Science Young Foundation of China
文摘ZnO/Znml2O4 nanocomposites with heteronanostructures were successfully prepared by co-precipitation method. The as-prepared samples were characterized by HRTEM, TEM, XRD, BET, TG-DTA, and UV-Vis spectra techniques. The photoeatalytic activities of the as-prepared samples were evaluated by the photocatalytic degradation of methyl orange and inactivation of Escherichia coli in suspension under the irradiation of the simulated sunlight. The effects of compositions, calcination temperatures, concentration ofphotocatalysts and light source on the photocatalytic activities were systematically studied. The results show that when the concentration of ZnO/ZnA1204 photocatalyst with the starting Zn to Al molar ratio of 1:1.5 calcined at 600 ℃ is 1.0 g/L, the maximum photocatalytic degradation rate of 98.5% can be obtained in 50 min under the irradiation of the simulated sunlight. Under the same conditions, an inactivation rate of 99.8% for E.coli is achieved in 60 min.
基金NationalNaturalScienceFoundationofChina (No .59772 0 1 9)
文摘Pervoskite type oxides LaCoO 3 was prepared by citrate method with the granula of 20 nm-30 nm. With a fluorescent Hg lamp or sunlight as irradiator, the degradation experiments of various water soluble dyes were carried out in the suspension system of LaCoO 3 . The results show that the pervoskite type oxide LaCoO 3 has good photocatalytic activity.Studied by X ray photoelectron spectroscopy and photoacoustic spectra, its photocatalytic activity is found to be related with factors such as the d electron structure of ion Co 3+ ,Co—O binding energy and adsorbed oxygen on the surface etc.
基金This work was supported by tile Key Projects of Natural Science Research of Universities in Anhui Province (No.KJ2015A183, No.KJ2015A201) and Talents Foundation of Hefei University (No.15RC05), Anhui Province Natural Science Foundation (No.1608085MD78), the Key Projects of Anhui Province University Outstanding Youth Talent Support Program (gxyqZD2016274), the National Natural Science Foundation of China (No.21305142, No.51403048).
文摘A multifunctional Cu2O/Ag micro-nanocomposite, which has the characteristics of high cat- alytic activities under the visible light and high surface-enhanced Raman scattering (SERS) activity, was fabricated via a facile method and employed for the in situ SERS monitoring of the photocatalytic degradation reaction of crystal violet. Through the variation of the AgNO3 concentration, Ag content on the Cu2O template can be controllably tuned, which has great influence on the SERS effect. The results indicate that Ag nanopartieles form on the Cu2O nanoframes to obtain the Cu2O/Ag nanoeomposite, which can act as an excellent bifunetional platform for in situ monitoring of photocatalytic degradation of organic pollutions by SERS.
基金ACKNOWLEDGMENT This work was supported Science Foundation of China by the National Natural (No.20703042).
文摘Titania-based composite catalysts were prepared through a sol-gel route employing multi-walled carbon nanotubes with different diameters. The materials were characterized using thermogravimetric analysis, nitrogen adsorption-desorption isotherm, powder X-ray diffraction, scanning electron microscopy, and diffuse reflectance UV-Vis absorption spectra. The application of the catalysts to photocatalytic degradation of phenol was tested under UV-Vis irradiation. A synergetic effect on phenol removal was observed in case of composite catalysts, which was evaluated in terms of apparent rate constant, total organic carbon removal and photonic efficiency.
基金supported by the National Natural Science Foundation of China (31901462 and 31671613).
文摘Bacillus thuringiensis(Bt)cotton production is challenged by two main problems,i.e.,the low concentration of Bt protein at the boll setting stage and the lowest insect resistance in bolls among all the cotton plant’s organs.Therefore,increasing the Bt protein concentration at the boll stage,especially in bolls,has become the main goal for increasing insect resistance in cotton.In this study,two protein degradation inhibitors(ethylene diamine tetra acetic acid(EDTA)and leupeptin)were sprayed on the bolls,subtending leaves,and whole cotton plants at the peak flowering stage of two Bt cultivars(medium maturation Sikang 1(SK1))and early maturation Zhongmian 425(ZM425)in 2019 and 2020.The Bt protein content and protein degradation metabolism were assessed.The results showed that the Bt protein concentrations were enhanced by 21.3 to 38.8%and 25.0 to 38.6%in the treated bolls of SK1 and ZM425 respectively,while they were decreased in the subtending leaves of these treated bolls.In the treated leaves,the Bt protein concentrations increased by 7.6 to 23.5%and 11.2 to 14.9%in SK1 and ZM425,respectively.The combined application of EDTA and leupeptin to the whole cotton plant increased the Bt protein concentrations in both bolls and subtending leaves.The Bt protein concentrations in bolls were higher,increasing by 22.5 to 31.0%and 19.6 to 32.5%for SK1 and ZM425,respectively.The organs treated with EDTA or/and leupeptin showed reduced free amino acid contents,protease and peptidase activities and significant enhancements in soluble protein contents.These results indicated that inhibiting protein degradation could improve the protein content,thus increasing the Bt protein concentrations in the bolls or/and leaves of cotton plants.Therefore,the increase in the Bt protein concentration without yield reduction suggested that these two protein degradation inhibitors may be applicable for improving insect resistance in cotton production.
基金TheNationalNaturalScienceFoundationofChina (No .2 0 1760 5 3 )
文摘The degradation of phenol was carried out using heterogeneous Fenton-type catalysts in the presence of H_2O_2 and UV. Catalysts were prepared by exchanging and immobilizing Fe 2+ in zeolite 13X, silica gel or Al_2O_3. The concentration of phenol solution was 100 mg/L. The amount of H_2O_2 added was the stoichiometric amount of H_2O_2 required for the total oxidation of phenol. Under the irradiation of medium pressure light (300 W) phenol was mineralized within 1 h in the presence of Fe 2+/zeolite 13X. The COD removal rate was enhanced in the presence of Fe 2+/zeolite 13X compared to that of Fe 2+/silica gel or Fe 2+/Al_2O_3. Analogous homogenous photo-Fenton reaction with equivalent Fe 2+ was also carried out to evaluate the catalysis efficiency of Fe 2+/zeolite 13X. Results showed that the COD removal rate was near to that of homogeneous Fenton, while heterogeneous Fe 2+/zeolite 13X catalyst could be recycled.
文摘Photocatalytic degradation of phenol selected as model compound of organic pollutant had been investigated in aqueous titanium dioxide (TiO2) dispersion under UV irradiation. The effects of various parameters such as pH, catalyst concentration, phenol concentration, anions, metal ions, electron acceptors, and surfactants on the photocatalytic degradation of phenol were investigated. The degradation kinetics was determined by the change in phenol concentration employing UV-Vis spectrometry as a function of irradiation time. The degradation kinetics of phenol follows pseudo first-order kinetics. The results showed a significant dependence of the photocatalytic degradation of phenol on the functional parameters. The probable promising roles of the additives on the degradation process were discussed.
基金supported by the National Natural Science Foundation of China (No. 20707009)the Jiangsu Province Social Development Foundation (No.BS2007051)+1 种基金the Opening Foundation (WTWER0713) of Engineering Research Center for Water Treatment and Water Remediation of the Ministry of Education of Chinathe State Key Laboratory of Pollution Control and Resource Reuse Opening Foundation (No. PCRRCF07003).
文摘The photocatalytic degradation of Rhodamine B (RhB) was carried out using TiO2 supported on activated carbon (TiO2-AC) under microwave irradiation. Composite catalyst TiO2-AC was prepared and characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM) and Brunauer-Emmett-Teller (BET). In the process of microwave-enhanced photocatalysis (MPC), RhB (30 mg/L) was almost completely decoloured in 10 min, and the mineralization efficiency was 96.0% in 20 min. The reaction rate constant of RhB in MPC using TiO2-AC by pseudo first-order reaction kinetics was 4.16 times of that using Degussa P25. Additionally, according to gas chromatography/mass spectrometry (GC/MS) and liquid chromatography/mass spectrometry (LC/MS) identification, the major intermediates of RhB in MPC included two kinds of N-de-ethylation intermediates (N,N-diethyl-N'-ethyl-rhodamine (DER)), oxalic acid, malonic acid, snccinic acid, and phthalic acid, maleic acid, 3-nitrobenzoic acid, and so on. The degradation of RhB in MPC was mainly attributed to the destruction of the conjugated structure, and then the intermediates transformed to acid molecules which were mineralized to water and carbon dioxide.
基金TheNationalNaturalScienceFoundationofChina (No .396 70 42 0 )
文摘Kinetic processes of a-naphthaleneacetic acid (NAA) photolysis were studied under different conditions. The results showed that the ultraviolet light was more effective than fluorescent light in promoting degradation, and the degradation of NAA under ultraviolet light followed the first order kinetics with the photolysis rate constant of 1.15 x 10-2 min-1 and half-life time (t1/2) of 60 min. Further, it was proved that the photolysis rate was higher in the presence of oxygen, titanium dioxide (TiO2), and low pH (acidic solution). At last, two photolysis intermediates were identified by GC-MS and possible photolysis pathways were proposed.
基金Project supported by the Special Foundation of Nanometer Technology from Shanghai Municipal Science and Technology Commis-sion(STCSM) (No. 0552nm002).
文摘Anatase TiO2 films were successfully prepared on foam nickel substrates by sol-gel technique using tetrabutyl titanate as precursor. The characteristics of the TiO2 films were investigated by XPS, XRD, FE-SEM, TEM and UV-Vis absorption spectra. The photocatalytic activities of TiO2 films were investigated by photocatalytic degradation reactions of gaseous acetaldehyde, an indoor pollutant, under ultraviolet light irradiation. It was found that Ni^2+ doping into TiO2 films due to the foam nickel substrates resulted in the extension of absorption edges of TiO2 films from UV region to visible light region. The pre-heating for foam nickel substrates resulted in the formation of NiO layer, which prevented effectively the injection of photogenerated electrons from TiO2 films to metal nickel. The TiO2 films displayed high photocatalytic activity for the degradation of acetaldehyde, and were enhanced by calcining the substrates and coating TiO2 films repeatedly. The high activity was mainly attributed to the improvement of the characteristics of substrate surface and the increase of active sites on photocatalyst.
基金Project supported by the National Natural Science Foundation of China (No. 20373074) the National Basic Research Programme (973) of China (No. 2003CB415006-3).
文摘The photocatalytic degradation of dye pollutant sulforhodamine-B (SRB) in aqueous titanium dioxide (TiO2) dispersions was examined under three lighting regimes: UV light (330 nm〈λ〈 380 nm), sunlight, and visible light (λ〉450 nm), all investigated at pH=2.5. Total organic carbon (TOC) and chemical oxygen demand (CODer) assays show that the degradation rate of SRB is much higher when irradiated with UV and sunlight compared with visible light. The temporal concentration changes of SRB illustrated a first-order reaction and the rate constant, k, is 0.197 min^-1, 0.152 min^-1, 0.027 min^-1, respectively, under the three lighting conditions. The final mineralized products were amine compounds identified by infrared spectrophotometry. When irradiated with visible light, the photocatalytic degradation rate could be improved by lowering the H2O2 concentration and inhibited by increasing the H2O2 concentration, but results contrary to the above were obtained when UV light was used for irradiation.