Laboratory studies were conducted to find out the efficacy of uniquely prepared zero valent iron impregnated silica in transforming xenobiotic chlorophenols namely 4-chlorophenol, 2,4-dichlorophenol and 2,4,6-trichlor...Laboratory studies were conducted to find out the efficacy of uniquely prepared zero valent iron impregnated silica in transforming xenobiotic chlorophenols namely 4-chlorophenol, 2,4-dichlorophenol and 2,4,6-trichlorophenol. Continuous mode column experiments were performed to investigate the transformation of chlorophenols by varying pH, column height, flow rate and initial chlorophenol concentration. Reusability study of the zero valent iron impregnated silica was studied as well as the morphological changes and the chemical composition of the catalyst medium were also investigated. Dechlorination kinetic studies were conducted and the order of dechlorination of chlorophenols was found to be 2,4,6-trichlorophenol 〉 2,4-dichlorophenol 〉 4-chlorophenol. The optimum pH, column height and flow rate were found to be 7, 20 cm and 0.75 L/hr respectively for all chlorophenols in the reaction duration of 4 hr. Intermediates formed during dechlorination study were identified by gas chromatography-mass spectroscopy analysis. This method was applied to real pulp and paper wastewater and was found satisfactory.展开更多
20 Quantum chemical parameters of chlorophenol compounds were fully optimized by using B3LYP method on both 6-31G^＊ and 6-311G^＊ basis sets. These structural parameters are taken as theoretical descriptors, and the ...20 Quantum chemical parameters of chlorophenol compounds were fully optimized by using B3LYP method on both 6-31G^＊ and 6-311G^＊ basis sets. These structural parameters are taken as theoretical descriptors, and the experimental data of 20 compounds＇ aquatic photogen toxicity（-lgEC50） are used to perform stepwise regression in order to obtain two predicted -lgEC50 correlation models whose correlation coefficients R^2 are respectively 0.9186 and 0.9567. In addition, parameters of chlorine atom＇s substitutive positions and their correlations （NPCs） are taken as descriptors to obtain another predicted -lgEC50 model with the correlation coefficient R2 of 0.9444. Correlation degree of each independent variable in the three models is verified by using variance inflation factors （VIF） and t value. In the cross-validation method, cross-validation coefficients q^2 of 3 models are respectively 0.8748, 0.9119 and 0.8993, which indicates that the relativity and prediction ability of this model are superior to those of the model obtained by topological and BLYP methods.展开更多
Individual and combined assessment of risks of adverse effects to aquatic ecosystems of three chlorophenols（CPs）,including 2,4dichlorophenol（2,4-DCP）,2,4,6-trichlorophenol（2,4,6-TCP） and pentachlorophenol（PCP）...Individual and combined assessment of risks of adverse effects to aquatic ecosystems of three chlorophenols（CPs）,including 2,4dichlorophenol（2,4-DCP）,2,4,6-trichlorophenol（2,4,6-TCP） and pentachlorophenol（PCP）,were conducted.A probabilistic approach based on the concentrations of CPs in surface waters of China was used to determine the likelihood of adverse effects.The potential risk of CPs in surface waters of China was determined to be of concern,especially PCP and mixtures of CPs.The risks of adverse effects were examined as the joint probabilities of exposure and response.The joint probability for PCP was 0.271 in the worst case and 0.111 in the median case,respectively.Based on the cumulative probability,5% of aquatic organisms included in the assessment would be affected 21.36% of the time in the worst case and 5.99% of the time in median case,respectively.For the mixtures of CPs,the joint probability were 0.171 in the worst case and 0.503 in median case,respectively and 5% of species would be affected 49.83% of the time for the worst case and 12.72% in the median case,respectively.Risks of effects of the individual CPs,2,4-DCP and 2,4,6-TCP were deemed to be acceptable with a overlapping probability of 0.1 with 5% of species being affected less than 4% of the time.展开更多
Ti/Sb-SnO2 anodes were prepared by thermal decomposition to examine the influence of the amount of Sb dopant on the structure and electrocatalytic capability of the electrodes in the oxidation of 4-chlorophenol. The p...Ti/Sb-SnO2 anodes were prepared by thermal decomposition to examine the influence of the amount of Sb dopant on the structure and electrocatalytic capability of the electrodes in the oxidation of 4-chlorophenol. The physicochemical properties of the Sb-SnO2 coating were markedly influenced by different amounts of Sb dopant. The electrodes, which contained 5% Sb dopant in the coating, presented a much more homogenous surface and much smaller mud-cracks, compared with Ti/Sb-SnO2 electrodes containing 10% or 15% Sb dopant, which exibited larger mud cracks and pores on the surface. However, the main microstructure remained unchanged with the addition of the Sb dopant. No new crystal phase was observed by X-ray diffraction （XRD）. The electrochemical oxidation of 4-chlorophenol on the Ti/SnO2 electrode with 5% Sb dopant was inclined to electrochemical combustion; while for those containing more Sb dopant, intermediate species were accumulated. The electrodes with 5% Sb dopant showed the highest efficiency in the bulk electrolysis of 4-chlorophenol at a current density of 20 mA/cm^2 for 180 min; and the removal rates of 4-chlorophenol and COD were 51.0% and 48.9%, respectively.展开更多
A series of phosphorus-modified titanium dioxide samples with varying P/Ti atomic ratio were conveniently prepared via a conventional solgel route. The effects of phosphorus content and calcination temperature on the ...A series of phosphorus-modified titanium dioxide samples with varying P/Ti atomic ratio were conveniently prepared via a conventional solgel route. The effects of phosphorus content and calcination temperature on the crystalline structure, grain growth, surface area, and the photocatalytic activity of P-modified TiO2 were investigated. The XRD results showed that P species slow down the particle growth of anatase and increase the anatase-to-rutile phase transformation temperature to more than 900°C. Kinetic studies on the P-modified TiO2 to degraded 4-chlorophenol had found that the TP5500 prepared by adopting a P/Ti atomic ratio equal to 0.05 and calcined at 500°C had an apparent rate constant equal to 0.0075 min 1, which is superior to the performance of a commercial photocatalyst Degussa P25 Kapp = 0.0045 min 1 and of unmodified TiO2 （TP0500） Kapp = 0.0022 min 1. From HPLC analyses, various hydroxylated intermediates formed during oxidation had been identified, including hydroquinone （HQ）, benzoquinone （BQ） and （4CC） 4-chlorocatechol as main products. Phytotoxicity was assessed before and after irradiation against seed germination of tomato （Lycopersicon esculentum） whereas acute toxicity was assessed by using Folsomia candida as the test organism. Intermediates products were all less toxic than 4-chlorophenol and a significant removal of the overall toxicity was accomplished展开更多
A hypercrosslinked polymeric adsorbent （ZH-03） for adsorbing and removing chlorophenolic compounds from their aqueous solutions was studied, including the static adsorption. The equilibrium adsorption data were fit ...A hypercrosslinked polymeric adsorbent （ZH-03） for adsorbing and removing chlorophenolic compounds from their aqueous solutions was studied, including the static adsorption. The equilibrium adsorption data were fit to Freundlich adsorption isothermic models to evaluate the model parameters. Thermodynamic studies on the adsorption of chlorophenolic compounds on ZH-03 indicated that there were chemisorption transitions for 2,4,6-trichlorophenol and physical adsorption processes for 2-chlorophenol and 2,6-chlorophenol, and ZH-03 showed the homogeneous nature of the adsorbent surface. Column adsorption for chlorophenols wastewater shows the advantages of the ZH-03 adsorbent for adsorbing the following chlorophenolic compounds as 2-chlorophenol, 2,6-dichlorophenol and 2,4,6-trichlorophenol. Sodium hydroxide was used for desorpting chlorophenols from ZH-03 and showed excellent performance.展开更多
A novel self-assembled pure and Mg doped ZnO nano-particles （NPs） were successfully synthesized by a simple low temperature co-precipitation method. The prepared photocatalysts were characterized by X-ray diffractio...A novel self-assembled pure and Mg doped ZnO nano-particles （NPs） were successfully synthesized by a simple low temperature co-precipitation method. The prepared photocatalysts were characterized by X-ray diffraction, high resolution scanning electron mi- croscopy, high resolution transmission electron microscopy, diffuse reflectance spectroscopy and photoluminescence （PL） spectroscopy. The results indicated that the prepared photocatalysts showed high crystallinity with a uniform size distribution of the NPs. The degradation of cholorphenols is highly mandatory in today＇s scenario as they are affecting the environment adversely. Thus, the photocatalytic degradation of 4-chlorophenol （4-CP）, a potent endocrine disrupting chemical in aqueous medium was investigated by both pure and Mg-doped ZnO NPs under UV-light irradiation in the present study. The influence of the Mg content on the structure, morphology, PL character and photocatalytic activity of ZnO NPs were investigated systematically. Furthermore,the effect of different parameters such as 4-CP concentration, photocatalyst amount, pH and UV-light wavelength on the resulting photocatalytic activity was investigated.展开更多
A new cell immobilization method based on the replacement of KCl by KCl+chitosan as the gelling agent was developed. The experimental results showed that through addition of chitosan into gelling agent, the mechanica...A new cell immobilization method based on the replacement of KCl by KCl+chitosan as the gelling agent was developed. The experimental results showed that through addition of chitosan into gelling agent, the mechanical strength and the thermal stability of the carrageenan gel were greatly improved. The new immobilization method was used to entrap a chlorophenol degrading microorganism. The immobilized microbial cells were applied for chlorophenol biodegradation. The experiments demonstrated that immobilized cells exhibit a higher bioactivity in the degradation of chlorophenol than free cells.展开更多
To better understand the interaction mechanisms of plant surfaces with polar organic compounds, sorption of 4-chlorophenol, 2,4- dichlorophenol, and 2,4,6-trichlorophenol by fruit cuticles （i.e., tomato, apple, and p...To better understand the interaction mechanisms of plant surfaces with polar organic compounds, sorption of 4-chlorophenol, 2,4- dichlorophenol, and 2,4,6-trichlorophenol by fruit cuticles （i.e., tomato, apple, and pepper）, and potato tuber periderm were investigated. The roles of cuticular components （waxes, cutin, cutan and sugar） on sorption of chlorophenols are quantitatively compared. Cutin and waxes govern the sorption capacity of bulk apple cuticle by hydrophobic interactions. Potato periderm with highest sugar content exhibits the lowest sorption capability for the chlorophenols. With the increase of hydrophobicity （i.e., Kow ） of sorbate, the relative contribution of lipophilic components （wax, cutin and cutan） on total sorption increases, however, the ratios of Koc to Kow decreases due to increasing ionization degree of sorbates.展开更多
The electrochemical treatment of wastewater containing chlorophenols （2-monochlorophenol, 4-monochlorophenol, 2,4-dichlorophenol, 2,4,6-trichlorophenol） was carried out experimentally with synthetic boron-d0ped diam...The electrochemical treatment of wastewater containing chlorophenols （2-monochlorophenol, 4-monochlorophenol, 2,4-dichlorophenol, 2,4,6-trichlorophenol） was carried out experimentally with synthetic boron-d0ped diamond （BDD） thin film electrodes. Current vs time curves under different cell voltages were measured. Removal rate of COD, instant current efficiency （ICE） and energy consumption were investigated under different current densities. The influence of supporting media is reported, which plays an important role in determining the global oxidation rate. The oxidative chloride is stronger than peroxodisulphate. The electrochemical characteristics of boron-doped diamond electrodes were investigated in comparison with active coating Ti substrate anode （ACT）. The experimental results show that BDD is markedly superior to ACT due to its different absorption properties.展开更多
Nanoscale Pd/Fe bimetallic particles were synthesized with an efficient method to dechlorinate o-chlorophenol. The nanoscale Pd/Fe particles were determined by transmission electron microscopy and BET specific surface...Nanoscale Pd/Fe bimetallic particles were synthesized with an efficient method to dechlorinate o-chlorophenol. The nanoscale Pd/Fe particles were determined by transmission electron microscopy and BET specific surface area analysis. Most of the particles are in the size range of 20—100 nm. The BET specific surface area of synthesized nanoscale Pd/Fe particles is 12.4 m 2/g. In contrast, a commercially available fine iron powder(<100 mesh) has a specific surface area of 0.49 m 2/g. Batch studies demonstrated that the nanoscale particles can effectively dechlorinate o-chlorophenol. The dechlorination reaction takes place on the surface of synthesized nanoscale Pd/Fe bimetallic particles in a pseudo-first order reaction. The surface-area-normalized rate coefficients(k_ SA) are comparable to those reported in the literature for chlorinated ethenes. The observed reaction rate constants(k_ obs) are dominated by the mass fraction of Pd and the mass concentration of the nanoscale Pd/Fe particles.展开更多
Candida albicans PDY-07 was isolated from activated sludge under anaerobic conditions and identified as a member belonging to the genus Candida. Pure culture of C. albicans PDY-07, biodegradation of 4-chlorophenol (4-...Candida albicans PDY-07 was isolated from activated sludge under anaerobic conditions and identified as a member belonging to the genus Candida. Pure culture of C. albicans PDY-07, biodegradation of 4-chlorophenol (4-CP) was carried out under anaerobic conditions in Erlenmeyer flasks at 35°C, with an initial pH of 7.0–7.2 and a starting inoculum of 10%(by volume). The results showed that, under the above-mentioned conditions, C. albicans PDY-07 could thoroughly biodegrade 4-CP up to a concentration of 300mg·L?1 within 244h and that it had a high tolerance potential of up to 440mg·L?1 for 4-CP. With the increase in the initial concentrations of 4-CP, substrate inhibition was obviously enhanced. There was increased consumption of 4-CP, which was not assimilated by the cell for growth but was used to counteract the strong substrate inhibition. In addition, the cell growth and substrate-degradation kinetics of 4-CP as the sole source of carbon and energy for the strain in batch cultures were also investigated over a wide range of substrate concentrations (2.2–350mg·L?1), using the proposed cell growth and degradation kinetic models. The results recorded from these experiments showed that the proposed kinetic models adequately described the dynamic behavior of 4-CP biodegradation by C. albicans PDY-07.展开更多
Chlorophenols, typically 4-chlorophenols are highly toxic and non-biodegradable organic contaminants which pose serious threat to the environment, particularly when released into aqueous medium. The removal of these p...Chlorophenols, typically 4-chlorophenols are highly toxic and non-biodegradable organic contaminants which pose serious threat to the environment, particularly when released into aqueous medium. The removal of these pollutants by efficient method has received worldwide concern in recent past. A new Fe3O4–Cr2O3 magnetic nanocomposite was synthesized by wet chemical method under ultrasonic irradiation. Microstructure and morphology of the nanocomposite were characterized by powder X-ray diffraction（XRD）,Fourier transform infrared（FT-IR）, and a transmission electron microscope（TEM）. Magnetic and optical properties were studied by a vibrating sample magnetometer（VSM） and an ultraviolet–visible（UV–Vis） spectrophotometer respectively. The magnetic nanocomposite（MNC） was used as photocatalyst for effective decomposition of 4-chlorophenol in water under ultraviolet（UV） irradiation.展开更多
In this paper, a novel magnetic solid-phase extraction method using three-dimensional graphene-based magnetic nanocomposite as adsorbent for the preconcentration of several chlorophenols from water samples prior to hi...In this paper, a novel magnetic solid-phase extraction method using three-dimensional graphene-based magnetic nanocomposite as adsorbent for the preconcentration of several chlorophenols from water samples prior to high-performance liquid chromatography analysis was developed. Various experimental parameters were investigated. Under the optimum conditions, the enrichment factors of the method were in the range of 186–312, and the limit of detection（S/N = 3） was 0.10 ng/mL. The recoveries of the method were in the range between 85.1% and 101.2%. The developed method has been successfully applied to the determination of chlorophenols in environmental water samples.展开更多
The oxidative degradation of 4-chlorophenol （4-CP） in aqueous solution induced by plasma with submersed glow discharge has been investigated. The concentration of 4-CP and the reaction intermediates were determined ...The oxidative degradation of 4-chlorophenol （4-CP） in aqueous solution induced by plasma with submersed glow discharge has been investigated. The concentration of 4-CP and the reaction intermediates were determined by high performance liquid chromatography （HPLC）. Various influencing factors such as the initial pH, the concentration of 4-CP and the catalytic action of Fe^2＋ were examined. The results indicate that 4-CP is eventually degraded into inorganic ion, dioxide carbon and water. The attack of hydroxyl radicals on the benzene rings of 4-CP in the initial stage of oxidative reactions is presumed to be a key step. They also suggest that the reaction is of a pseudo-first order kinetic reaction and the proposed method is an efficient way for the 4-CP degradation,展开更多
Chlorophenols(CPs)are significant refractory pollutants that are highly toxic to humans and other organ-isms.Reactive electrode membranes(REMs)show considerable potential in the electrochemical removal of refractory p...Chlorophenols(CPs)are significant refractory pollutants that are highly toxic to humans and other organ-isms.Reactive electrode membranes(REMs)show considerable potential in the electrochemical removal of refractory pollutants by allowing flow-through operations with convection-enhanced mass transfer.However,relevant studies are commonly performed on the laboratory scale,and there is no straightfor-ward method that guarantees success in scaling up engineered REM reactors.In this study,we demon-strated that a tubular concentric electrode(TCE)configuration with a titanium suboxide ceramic anode and a stainless-steel cathode is suitable for large-scale CPs removal.Both theoretical and experi-mental results showed that the TCE configuration not only allows the electrode surface to be orthogonal to electric field lines everywhere,but also has an ohmic resistance that is inversely proportional to the length of the electrode.In addition,the TCE configuration can be operated in either the anode-to-cathode(AC)or the cathode-to-anode(CA)mode based on the flow direction,creating adjustable condi-tions for selective degradation of CPs.This was confirmed by 98%removal of 2,4-dichlorophenol(2,4-DCP)and 72.5%removal of chemical oxygen demand(COD)in the CA mode,in which the kinetic constant was one order of magnitude higher than that for the AC mode under flow-through single-pass operations.This can be explained by the lower activation energy and free energy in the CA mode,as revealed by the-oretical calculations and experimental measurements.The TCE configuration is also suitable for a numbering-up strategy to scale up the electrochemical reactor without increasing the ohmic resistance or decreasing the specific electrode area,achieving 99.4%removal of 2,4-DCP with an energy consump-tion of 1.5 kW·h·m^(-3) when three TCE modules were employed.This study presents a suitable electrode design configuration for the REM reactor,offering effective strategies to bridge the“Valley of Death”encountered when scaling up the electrochemical removal of CP pollutants.展开更多
Experimental data are presented to test and validate a kinetic model for the oxidation of 2 chlorophenol wastewater by photo assisted Fenton process. The data showed that this process had produced good effects under a...Experimental data are presented to test and validate a kinetic model for the oxidation of 2 chlorophenol wastewater by photo assisted Fenton process. The data showed that this process had produced good effects under acidic conductions. Up to 90% 2 chlorophenol was removed after 90 minute reaction time with H 2O 2 of 25% COD Cr, in , while in UV/H 2O 2 system only 16 8% 2 chlorophenol was removed after one hour treatment. The optimal pH in this reaction occurred between pH 3 0 and pH 4.0. The reaction kinetics for photo assisted Fenton process experimented in this research was investigated. Kinetic models were proposed for the treatment of 2 chlorophenol wastewater. The reaction was found to follow the 2nd order. The equations of reaction kinetics are as follows:-d[RH]d t = K RH [RH][H 2O 2] 0exp (-K H 2O 2 t );-d[COD Cr ]d t = K COD Cr [COD Cr ][H 2O 2] 0exp(-K′ t ). The prediction of the models was found to be in a good agreement with experimental results, thus confirming the proposed reaction mechanism.展开更多
This paper provides evidence for the degradation of organic pollutant by the photo-Fenton complex mechanism. Both the complex oxidation and HO. oxidation mechanisms were verified by p-chlorophenol degradation, UV/Vis ...This paper provides evidence for the degradation of organic pollutant by the photo-Fenton complex mechanism. Both the complex oxidation and HO. oxidation mechanisms were verified by p-chlorophenol degradation, UV/Vis spectra anaylsis, and quantum yield. The hydroxyl radical involved in the photo-Fenton process can also be generated from the decomposition of H2O2, photolysis of Fe^3＋ and degradation of hydrated Fe（Ⅵ）-complex, excepting the traditional Fenton reaction.展开更多
Studies on the effect of the chlorine content of chlorophenols （CPs） on their adsorption from aqueous solution by mesoporous SBA-15 are important in understanding the mechanisms of CP adsorption. In this study, thre...Studies on the effect of the chlorine content of chlorophenols （CPs） on their adsorption from aqueous solution by mesoporous SBA-15 are important in understanding the mechanisms of CP adsorption. In this study, three CPs with different degrees of chlorine content （i.e., 2-chlorophenol, 2,6-dichlorophenol and 2,4,6-trichlorophenol） were investigated. The effects of parameters such as temperature and solution pH were studied. The results showed that CP adsorption by SBA- 15 increased with increasing number of chlorine substituents and depended strongly on the temperature and solution pH. Thermodynamic parameters such as Gibbs free energy change （AGO）, enthalpy change （△H^0） and entropy change （△S^0） were also calculated. By comparison of the adsorption coefficient of CPs with varying physical-chemical properties （size, hydrophobicity and electron density）, we propose that hydrophobic interactions between CPs and the SBA-15 surface, as well as electron donor-acceptor （EDA） complexes between oxygen of the siloxane surface of SBA-15 （e--donor） and the n-system of the CPs （e--acceptor）, were dominant adsorption mechanisms.展开更多
A novel in-situ electrochemical oxidation method was applied to the degradation of wastewater containing chlorophenol. Under oxygen sparging, the strong oxidant, hydrogen dioxide, could be in-situ generated through th...A novel in-situ electrochemical oxidation method was applied to the degradation of wastewater containing chlorophenol. Under oxygen sparging, the strong oxidant, hydrogen dioxide, could be in-situ generated through the reduction of oxygen on the surface of the cathode. The removal rate ofchlorophenol could be increased 149% when oxygen was induced in the electrochemical cell. The promotion factor was estimated to be about 82.63% according to the pseudo-first-order reaction rate constant (min^-1). Important operating parameters such as current density, sparged oxygen rate were investigated. Higher sparged oxygen rate could improve the degradation of chlorophenol. To make full use of oxygen, however, sparged oxygen rate of 0.05 m3/h was adopted in this work. Oxidation-reduction potential could remarkably affect the generation of hydrogen peroxide. It was found that the removal rate of chlorophenol was not in direct proportion to the applied current density. The optimum current density was 3.5 mA/cm^2 when initial chlorophenol concentration was 100 mg/L and sparged oxygen rate was 0.05 m^3/h.展开更多
文摘Laboratory studies were conducted to find out the efficacy of uniquely prepared zero valent iron impregnated silica in transforming xenobiotic chlorophenols namely 4-chlorophenol, 2,4-dichlorophenol and 2,4,6-trichlorophenol. Continuous mode column experiments were performed to investigate the transformation of chlorophenols by varying pH, column height, flow rate and initial chlorophenol concentration. Reusability study of the zero valent iron impregnated silica was studied as well as the morphological changes and the chemical composition of the catalyst medium were also investigated. Dechlorination kinetic studies were conducted and the order of dechlorination of chlorophenols was found to be 2,4,6-trichlorophenol 〉 2,4-dichlorophenol 〉 4-chlorophenol. The optimum pH, column height and flow rate were found to be 7, 20 cm and 0.75 L/hr respectively for all chlorophenols in the reaction duration of 4 hr. Intermediates formed during dechlorination study were identified by gas chromatography-mass spectroscopy analysis. This method was applied to real pulp and paper wastewater and was found satisfactory.
基金973 National Basic Research Program of China (2003CB415002)
文摘20 Quantum chemical parameters of chlorophenol compounds were fully optimized by using B3LYP method on both 6-31G^＊ and 6-311G^＊ basis sets. These structural parameters are taken as theoretical descriptors, and the experimental data of 20 compounds＇ aquatic photogen toxicity（-lgEC50） are used to perform stepwise regression in order to obtain two predicted -lgEC50 correlation models whose correlation coefficients R^2 are respectively 0.9186 and 0.9567. In addition, parameters of chlorine atom＇s substitutive positions and their correlations （NPCs） are taken as descriptors to obtain another predicted -lgEC50 model with the correlation coefficient R2 of 0.9444. Correlation degree of each independent variable in the three models is verified by using variance inflation factors （VIF） and t value. In the cross-validation method, cross-validation coefficients q^2 of 3 models are respectively 0.8748, 0.9119 and 0.8993, which indicates that the relativity and prediction ability of this model are superior to those of the model obtained by topological and BLYP methods.
基金supported by the National Natural Science Foundation of China(No.20737001,20977047)the Major State Basic Research Development Program (No.2008CB418102)+3 种基金the Specialized Research Fund for the Doctoral Program of Higher Education(No. 200802841030)the National Major Project of Science & Technology Ministry of China(No.2008ZX08526-003)supported by the Canada Research Chair Program,and is at-large Chair Professor at the Department of Biology and Chemistry and State Key Laboratory in Marine Pollution,City University of Hong Kongthe Einstein Professor Program of the Chinese Academy of Sciences and the Visiting Professor Program of King Saud University
文摘Individual and combined assessment of risks of adverse effects to aquatic ecosystems of three chlorophenols（CPs）,including 2,4dichlorophenol（2,4-DCP）,2,4,6-trichlorophenol（2,4,6-TCP） and pentachlorophenol（PCP）,were conducted.A probabilistic approach based on the concentrations of CPs in surface waters of China was used to determine the likelihood of adverse effects.The potential risk of CPs in surface waters of China was determined to be of concern,especially PCP and mixtures of CPs.The risks of adverse effects were examined as the joint probabilities of exposure and response.The joint probability for PCP was 0.271 in the worst case and 0.111 in the median case,respectively.Based on the cumulative probability,5% of aquatic organisms included in the assessment would be affected 21.36% of the time in the worst case and 5.99% of the time in median case,respectively.For the mixtures of CPs,the joint probability were 0.171 in the worst case and 0.503 in median case,respectively and 5% of species would be affected 49.83% of the time for the worst case and 12.72% in the median case,respectively.Risks of effects of the individual CPs,2,4-DCP and 2,4,6-TCP were deemed to be acceptable with a overlapping probability of 0.1 with 5% of species being affected less than 4% of the time.
基金Project supported by the Institute of Environmental Engineering,Peking University and China Postdoctoral Science Foundation(No.2005037032)
文摘Ti/Sb-SnO2 anodes were prepared by thermal decomposition to examine the influence of the amount of Sb dopant on the structure and electrocatalytic capability of the electrodes in the oxidation of 4-chlorophenol. The physicochemical properties of the Sb-SnO2 coating were markedly influenced by different amounts of Sb dopant. The electrodes, which contained 5% Sb dopant in the coating, presented a much more homogenous surface and much smaller mud-cracks, compared with Ti/Sb-SnO2 electrodes containing 10% or 15% Sb dopant, which exibited larger mud cracks and pores on the surface. However, the main microstructure remained unchanged with the addition of the Sb dopant. No new crystal phase was observed by X-ray diffraction （XRD）. The electrochemical oxidation of 4-chlorophenol on the Ti/SnO2 electrode with 5% Sb dopant was inclined to electrochemical combustion; while for those containing more Sb dopant, intermediate species were accumulated. The electrodes with 5% Sb dopant showed the highest efficiency in the bulk electrolysis of 4-chlorophenol at a current density of 20 mA/cm^2 for 180 min; and the removal rates of 4-chlorophenol and COD were 51.0% and 48.9%, respectively.
文摘A series of phosphorus-modified titanium dioxide samples with varying P/Ti atomic ratio were conveniently prepared via a conventional solgel route. The effects of phosphorus content and calcination temperature on the crystalline structure, grain growth, surface area, and the photocatalytic activity of P-modified TiO2 were investigated. The XRD results showed that P species slow down the particle growth of anatase and increase the anatase-to-rutile phase transformation temperature to more than 900°C. Kinetic studies on the P-modified TiO2 to degraded 4-chlorophenol had found that the TP5500 prepared by adopting a P/Ti atomic ratio equal to 0.05 and calcined at 500°C had an apparent rate constant equal to 0.0075 min 1, which is superior to the performance of a commercial photocatalyst Degussa P25 Kapp = 0.0045 min 1 and of unmodified TiO2 （TP0500） Kapp = 0.0022 min 1. From HPLC analyses, various hydroxylated intermediates formed during oxidation had been identified, including hydroquinone （HQ）, benzoquinone （BQ） and （4CC） 4-chlorocatechol as main products. Phytotoxicity was assessed before and after irradiation against seed germination of tomato （Lycopersicon esculentum） whereas acute toxicity was assessed by using Folsomia candida as the test organism. Intermediates products were all less toxic than 4-chlorophenol and a significant removal of the overall toxicity was accomplished
基金This work was funded by the Educational Bureau of Jiangsu Province, China (Grant Code 04KJB150153 and 05KJD610250).
文摘A hypercrosslinked polymeric adsorbent （ZH-03） for adsorbing and removing chlorophenolic compounds from their aqueous solutions was studied, including the static adsorption. The equilibrium adsorption data were fit to Freundlich adsorption isothermic models to evaluate the model parameters. Thermodynamic studies on the adsorption of chlorophenolic compounds on ZH-03 indicated that there were chemisorption transitions for 2,4,6-trichlorophenol and physical adsorption processes for 2-chlorophenol and 2,6-chlorophenol, and ZH-03 showed the homogeneous nature of the adsorbent surface. Column adsorption for chlorophenols wastewater shows the advantages of the ZH-03 adsorbent for adsorbing the following chlorophenolic compounds as 2-chlorophenol, 2,6-dichlorophenol and 2,4,6-trichlorophenol. Sodium hydroxide was used for desorpting chlorophenols from ZH-03 and showed excellent performance.
基金the financial support rendered by University Grants Commission(UGC)(Ref.F.No.38-118/2009(SR)),New Delhi
文摘A novel self-assembled pure and Mg doped ZnO nano-particles （NPs） were successfully synthesized by a simple low temperature co-precipitation method. The prepared photocatalysts were characterized by X-ray diffraction, high resolution scanning electron mi- croscopy, high resolution transmission electron microscopy, diffuse reflectance spectroscopy and photoluminescence （PL） spectroscopy. The results indicated that the prepared photocatalysts showed high crystallinity with a uniform size distribution of the NPs. The degradation of cholorphenols is highly mandatory in today＇s scenario as they are affecting the environment adversely. Thus, the photocatalytic degradation of 4-chlorophenol （4-CP）, a potent endocrine disrupting chemical in aqueous medium was investigated by both pure and Mg-doped ZnO NPs under UV-light irradiation in the present study. The influence of the Mg content on the structure, morphology, PL character and photocatalytic activity of ZnO NPs were investigated systematically. Furthermore,the effect of different parameters such as 4-CP concentration, photocatalyst amount, pH and UV-light wavelength on the resulting photocatalytic activity was investigated.
文摘A new cell immobilization method based on the replacement of KCl by KCl+chitosan as the gelling agent was developed. The experimental results showed that through addition of chitosan into gelling agent, the mechanical strength and the thermal stability of the carrageenan gel were greatly improved. The new immobilization method was used to entrap a chlorophenol degrading microorganism. The immobilized microbial cells were applied for chlorophenol biodegradation. The experiments demonstrated that immobilized cells exhibit a higher bioactivity in the degradation of chlorophenol than free cells.
基金supported by the National Natural Science Foundation of China (No. 20977081)the Foundation forthe Author of National Excellent Doctoral Dissertation of China (No. 200765)+1 种基金the Zhejiang Provincial Natural Science Foundation of China (No. R5100105)the Doctoral Fund of Ministry of Education of China (No.J20091588)
文摘To better understand the interaction mechanisms of plant surfaces with polar organic compounds, sorption of 4-chlorophenol, 2,4- dichlorophenol, and 2,4,6-trichlorophenol by fruit cuticles （i.e., tomato, apple, and pepper）, and potato tuber periderm were investigated. The roles of cuticular components （waxes, cutin, cutan and sugar） on sorption of chlorophenols are quantitatively compared. Cutin and waxes govern the sorption capacity of bulk apple cuticle by hydrophobic interactions. Potato periderm with highest sugar content exhibits the lowest sorption capability for the chlorophenols. With the increase of hydrophobicity （i.e., Kow ） of sorbate, the relative contribution of lipophilic components （wax, cutin and cutan） on total sorption increases, however, the ratios of Koc to Kow decreases due to increasing ionization degree of sorbates.
基金Project(20113282241450) supported by the Science and Technology Program from Ministry of Transport of China
文摘The electrochemical treatment of wastewater containing chlorophenols （2-monochlorophenol, 4-monochlorophenol, 2,4-dichlorophenol, 2,4,6-trichlorophenol） was carried out experimentally with synthetic boron-d0ped diamond （BDD） thin film electrodes. Current vs time curves under different cell voltages were measured. Removal rate of COD, instant current efficiency （ICE） and energy consumption were investigated under different current densities. The influence of supporting media is reported, which plays an important role in determining the global oxidation rate. The oxidative chloride is stronger than peroxodisulphate. The electrochemical characteristics of boron-doped diamond electrodes were investigated in comparison with active coating Ti substrate anode （ACT）. The experimental results show that BDD is markedly superior to ACT due to its different absorption properties.
文摘Nanoscale Pd/Fe bimetallic particles were synthesized with an efficient method to dechlorinate o-chlorophenol. The nanoscale Pd/Fe particles were determined by transmission electron microscopy and BET specific surface area analysis. Most of the particles are in the size range of 20—100 nm. The BET specific surface area of synthesized nanoscale Pd/Fe particles is 12.4 m 2/g. In contrast, a commercially available fine iron powder(<100 mesh) has a specific surface area of 0.49 m 2/g. Batch studies demonstrated that the nanoscale particles can effectively dechlorinate o-chlorophenol. The dechlorination reaction takes place on the surface of synthesized nanoscale Pd/Fe bimetallic particles in a pseudo-first order reaction. The surface-area-normalized rate coefficients(k_ SA) are comparable to those reported in the literature for chlorinated ethenes. The observed reaction rate constants(k_ obs) are dominated by the mass fraction of Pd and the mass concentration of the nanoscale Pd/Fe particles.
基金Supported by the National Natural Science Foundation of China (No.20336030) and the Natural Science Foundation of Tianjin(No.05YFJZJC 00500).
文摘Candida albicans PDY-07 was isolated from activated sludge under anaerobic conditions and identified as a member belonging to the genus Candida. Pure culture of C. albicans PDY-07, biodegradation of 4-chlorophenol (4-CP) was carried out under anaerobic conditions in Erlenmeyer flasks at 35°C, with an initial pH of 7.0–7.2 and a starting inoculum of 10%(by volume). The results showed that, under the above-mentioned conditions, C. albicans PDY-07 could thoroughly biodegrade 4-CP up to a concentration of 300mg·L?1 within 244h and that it had a high tolerance potential of up to 440mg·L?1 for 4-CP. With the increase in the initial concentrations of 4-CP, substrate inhibition was obviously enhanced. There was increased consumption of 4-CP, which was not assimilated by the cell for growth but was used to counteract the strong substrate inhibition. In addition, the cell growth and substrate-degradation kinetics of 4-CP as the sole source of carbon and energy for the strain in batch cultures were also investigated over a wide range of substrate concentrations (2.2–350mg·L?1), using the proposed cell growth and degradation kinetic models. The results recorded from these experiments showed that the proposed kinetic models adequately described the dynamic behavior of 4-CP biodegradation by C. albicans PDY-07.
基金support from Central Instruments Facility and Department of Chemistry of Indian Institute of Technology Guwahati for extending various analytical facilities during the course of investigation
文摘Chlorophenols, typically 4-chlorophenols are highly toxic and non-biodegradable organic contaminants which pose serious threat to the environment, particularly when released into aqueous medium. The removal of these pollutants by efficient method has received worldwide concern in recent past. A new Fe3O4–Cr2O3 magnetic nanocomposite was synthesized by wet chemical method under ultrasonic irradiation. Microstructure and morphology of the nanocomposite were characterized by powder X-ray diffraction（XRD）,Fourier transform infrared（FT-IR）, and a transmission electron microscope（TEM）. Magnetic and optical properties were studied by a vibrating sample magnetometer（VSM） and an ultraviolet–visible（UV–Vis） spectrophotometer respectively. The magnetic nanocomposite（MNC） was used as photocatalyst for effective decomposition of 4-chlorophenol in water under ultraviolet（UV） irradiation.
基金Financial supports from the National Natural Science Foundation of China (No. 31171698)the Scientific and Technological Research Foundation of Department of Education of Hebei Province (No. ZD20131033)the Natural Science Foundations of Hebei (No. B2012204028)
文摘In this paper, a novel magnetic solid-phase extraction method using three-dimensional graphene-based magnetic nanocomposite as adsorbent for the preconcentration of several chlorophenols from water samples prior to high-performance liquid chromatography analysis was developed. Various experimental parameters were investigated. Under the optimum conditions, the enrichment factors of the method were in the range of 186–312, and the limit of detection（S/N = 3） was 0.10 ng/mL. The recoveries of the method were in the range between 85.1% and 101.2%. The developed method has been successfully applied to the determination of chlorophenols in environmental water samples.
基金The project partially supported by the Project of Key Science and Technology of Education Ministry (00250), the Natural ScienceFoundation of Gansu Province (3ZS041-A25-028), and the Project of KJCXGC-01, NWNU, China
文摘The oxidative degradation of 4-chlorophenol （4-CP） in aqueous solution induced by plasma with submersed glow discharge has been investigated. The concentration of 4-CP and the reaction intermediates were determined by high performance liquid chromatography （HPLC）. Various influencing factors such as the initial pH, the concentration of 4-CP and the catalytic action of Fe^2＋ were examined. The results indicate that 4-CP is eventually degraded into inorganic ion, dioxide carbon and water. The attack of hydroxyl radicals on the benzene rings of 4-CP in the initial stage of oxidative reactions is presumed to be a key step. They also suggest that the reaction is of a pseudo-first order kinetic reaction and the proposed method is an efficient way for the 4-CP degradation,
基金supported by the National Natural Science Foun-dation of China(U21A20161 and 51822806)State Key Laboratory of Urban Water Resource and Environment,China(Harbin Institute of Technology)(2020DX07)Heilongjiang Touyan Innovation Team Program,China(HIT-SE-01).
文摘Chlorophenols(CPs)are significant refractory pollutants that are highly toxic to humans and other organ-isms.Reactive electrode membranes(REMs)show considerable potential in the electrochemical removal of refractory pollutants by allowing flow-through operations with convection-enhanced mass transfer.However,relevant studies are commonly performed on the laboratory scale,and there is no straightfor-ward method that guarantees success in scaling up engineered REM reactors.In this study,we demon-strated that a tubular concentric electrode(TCE)configuration with a titanium suboxide ceramic anode and a stainless-steel cathode is suitable for large-scale CPs removal.Both theoretical and experi-mental results showed that the TCE configuration not only allows the electrode surface to be orthogonal to electric field lines everywhere,but also has an ohmic resistance that is inversely proportional to the length of the electrode.In addition,the TCE configuration can be operated in either the anode-to-cathode(AC)or the cathode-to-anode(CA)mode based on the flow direction,creating adjustable condi-tions for selective degradation of CPs.This was confirmed by 98%removal of 2,4-dichlorophenol(2,4-DCP)and 72.5%removal of chemical oxygen demand(COD)in the CA mode,in which the kinetic constant was one order of magnitude higher than that for the AC mode under flow-through single-pass operations.This can be explained by the lower activation energy and free energy in the CA mode,as revealed by the-oretical calculations and experimental measurements.The TCE configuration is also suitable for a numbering-up strategy to scale up the electrochemical reactor without increasing the ohmic resistance or decreasing the specific electrode area,achieving 99.4%removal of 2,4-DCP with an energy consump-tion of 1.5 kW·h·m^(-3) when three TCE modules were employed.This study presents a suitable electrode design configuration for the REM reactor,offering effective strategies to bridge the“Valley of Death”encountered when scaling up the electrochemical removal of CP pollutants.
文摘Experimental data are presented to test and validate a kinetic model for the oxidation of 2 chlorophenol wastewater by photo assisted Fenton process. The data showed that this process had produced good effects under acidic conductions. Up to 90% 2 chlorophenol was removed after 90 minute reaction time with H 2O 2 of 25% COD Cr, in , while in UV/H 2O 2 system only 16 8% 2 chlorophenol was removed after one hour treatment. The optimal pH in this reaction occurred between pH 3 0 and pH 4.0. The reaction kinetics for photo assisted Fenton process experimented in this research was investigated. Kinetic models were proposed for the treatment of 2 chlorophenol wastewater. The reaction was found to follow the 2nd order. The equations of reaction kinetics are as follows:-d[RH]d t = K RH [RH][H 2O 2] 0exp (-K H 2O 2 t );-d[COD Cr ]d t = K COD Cr [COD Cr ][H 2O 2] 0exp(-K′ t ). The prediction of the models was found to be in a good agreement with experimental results, thus confirming the proposed reaction mechanism.
文摘This paper provides evidence for the degradation of organic pollutant by the photo-Fenton complex mechanism. Both the complex oxidation and HO. oxidation mechanisms were verified by p-chlorophenol degradation, UV/Vis spectra anaylsis, and quantum yield. The hydroxyl radical involved in the photo-Fenton process can also be generated from the decomposition of H2O2, photolysis of Fe^3＋ and degradation of hydrated Fe（Ⅵ）-complex, excepting the traditional Fenton reaction.
基金supported by the Postdoctoral Fund of Southeast Universitythe Natural Science Foundation of Jiangsu Province (No. BK2009294)
文摘Studies on the effect of the chlorine content of chlorophenols （CPs） on their adsorption from aqueous solution by mesoporous SBA-15 are important in understanding the mechanisms of CP adsorption. In this study, three CPs with different degrees of chlorine content （i.e., 2-chlorophenol, 2,6-dichlorophenol and 2,4,6-trichlorophenol） were investigated. The effects of parameters such as temperature and solution pH were studied. The results showed that CP adsorption by SBA- 15 increased with increasing number of chlorine substituents and depended strongly on the temperature and solution pH. Thermodynamic parameters such as Gibbs free energy change （AGO）, enthalpy change （△H^0） and entropy change （△S^0） were also calculated. By comparison of the adsorption coefficient of CPs with varying physical-chemical properties （size, hydrophobicity and electron density）, we propose that hydrophobic interactions between CPs and the SBA-15 surface, as well as electron donor-acceptor （EDA） complexes between oxygen of the siloxane surface of SBA-15 （e--donor） and the n-system of the CPs （e--acceptor）, were dominant adsorption mechanisms.
基金Project supported partially by the Hi-Tech Research and Devel-opment Program (863) of China (No. 2002AA529182) and the Foundation of Education Ministry of China (No. 98679) andZhejiang Provincial Natural Science Foundation of China (No. 200043)
文摘A novel in-situ electrochemical oxidation method was applied to the degradation of wastewater containing chlorophenol. Under oxygen sparging, the strong oxidant, hydrogen dioxide, could be in-situ generated through the reduction of oxygen on the surface of the cathode. The removal rate ofchlorophenol could be increased 149% when oxygen was induced in the electrochemical cell. The promotion factor was estimated to be about 82.63% according to the pseudo-first-order reaction rate constant (min^-1). Important operating parameters such as current density, sparged oxygen rate were investigated. Higher sparged oxygen rate could improve the degradation of chlorophenol. To make full use of oxygen, however, sparged oxygen rate of 0.05 m3/h was adopted in this work. Oxidation-reduction potential could remarkably affect the generation of hydrogen peroxide. It was found that the removal rate of chlorophenol was not in direct proportion to the applied current density. The optimum current density was 3.5 mA/cm^2 when initial chlorophenol concentration was 100 mg/L and sparged oxygen rate was 0.05 m^3/h.
