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1.
As an active metabolite of venlafaxine and emerging antidepressant, O-desmethylvenlafaxine (ODVEN) was widely detected in different water bodies, which caused potential harm to human health and environmental safety. In this study, the comparative work on the ODVEN degradation by UV (254 nm) and UV-LED (275 nm) activated sodium percarbonate (SPC) systems was systematically performed. The higher removal rate of ODVEN can be achieved under UV-LED direct photolysis (14.99%) than UV direct photolysis (4.57%) due to the higher values of photolysis coefficient at the wavelength 275 nm. Significant synergistic effects were observed in the UV/SPC (80.38%) and UV-LED/SPC (53.57%) systems and the former exhibited better performance for the elimination of ODVEN. The degradation of ODVEN all followed the pseudo-first-order kinetics well in these processes, and the pseudo-first-order rate constant (kobs) increased with increasing SPC concentration. Radicals quenching experiments demonstrated that both ·OH and CO3· were involved in the degradation of ODVEN and the second-order rate constant of ODVEN with CO3· (1.58 × 108 (mol/L)−1 sec−1) was reported for the first time based on competitive kinetic method. The introduction of HA, Cl, NO3 and HCO3 inhibited the ODVEN degradation to varying degrees in the both processes. According to quantum chemical calculation, radical addition at the ortho-position of the phenolic hydroxyl group was confirmed to be the main reaction pathways for the oxidation of ODVEN by ·OH. In addition, the oxidation of ODVEN may involve the demethylation, H-abstraction, OH-addition and C-N bond cleavage. Eventually, the UV-LED/SPC process was considered to be more cost-effective compared to the UV/SPC process, although the UV/SPC process possessed a higher removal rate of ODVEN.  相似文献   

2.
In the oxidation treatment of textile dyeing sludge, the quantitative and transformation laws of organic chlorine are not clear enough. Thus, this study mainly evaluated the treatment of textile dyeing sludge by Fenton and Fenton-like system from the aspects of the influence of Cl, the removal of polycyclic aromatic hydrocarbons (PAHs) and organic carbon, and the removal and formation mechanism of organic chlorine. The results showed that the organic halogen in sludge was mainly hydrophobic organic chlorine, and the content of adsorbable organic chlorine (AOCl) was 0.30 mg/g (dry sludge). In the Fenton system with pH=3, 500 mg/L Cl, 30 mmol/L Fe2+ and 30 mmol/L H2O2, the removal of phenanthrene was promoted by chlorine radicals (•Cl), and the AOCl in sludge solid phase increased to 0.55 mg/g (dry sludge) at 30 min. According to spectral analysis, it was found that •Cl could chlorinate aromatic and aliphatic compounds (excluding PAHs) in solid phase at the same time, and eventually led to the accumulation of aromatic chlorides in solid phase. Strengthening the oxidation ability of Fenton system increased the formation of organic chlorines in liquid and solid phases. In weak acidity, the oxidation and desorption of superoxide anion promoted the removal and migration of PAHs and organic carbon in solid phase, and reduced the formation of total organic chlorine. The Fenton-like system dominated by non-hydroxyl radical could realize the mineralization of PAHs, organic carbon and organic chlorines instead of migration. This paper builds a basis for the selection of sludge conditioning methods.  相似文献   

3.
Cu-Co multiple-oxides modified on HNO3-pretreated activated coke (ACN) were optimized for the simultaneous removal of gaseous CO and elemental mercury (Hg0) at low temperature (< 200 °C). It was found that 2%CuOx-10%CoOx/ACN catalyst calcined at 400°C resulted in the coexistence of complex oxides including CuO, Cu2O, Co3O4, Co2O3 and CoO phases, which might be good for the simultaneous catalytic oxidation of CO by Co-species and removal of Hg0 by Cu-species, benefiting from the synergistic catalysis during the electro-interaction between Co and Cu cations (CoO ? Co3O4 and Cu2O ? CuO). The catalysis removal of CO oxidation was obviously depended on the reaction temperature obtaining 94.7% at 200 °C, while no obvious promoting effect on the Hg0 removal (68.3%-78.7%). These materials were very substitute for the removal of CO and Hg° from the flue gas with the conditions of 8–20 vol.% O2 and flue-gas temperature below 200 °C. The removal of Hg° followed the combination processes of adsorption and catalytic oxidation reaction via Langmuir-Hinshelwood mechanism, while the catalysis of CO abided by the Mars-van Krevelen mechanism with lattice oxygen species.  相似文献   

4.
To achieve advanced nitrogen removal from actual municipal sewage, a novel multistage anoxic/aerobic process with sludge regeneration zone (R-MAO) was developed. The reactor was used to treat actual domestic sewage and the nitrogen removal capacity of the sludge regeneration zone (R zone) was investigated during the long-term operation. The best performance was obtained at the R zone's Oxidation-Reduction Potential (ORP) of -50±30 mV and hydraulic residence times (HRT) of 1.2 hr. The average effluent COD, TN, NH4+-N and NO3-N of the R-MAO process were 18.0±2.3, 7.5±0.6, 1.0±0.5 and 4.6±0.4 mg/L, respectively, with the corresponding removal efficiency of COD, TN and NH4+-N were 92.9%±1.0%, 84.1%±1.5% and 97.5%±1.1%. Compared to the sole MAO system, the TN removal efficiency of the R-MAO increased by 10.1%. Besides, under the optimal conditions, the contribution of the R zone in the R-MAO that removal COD, TN, NH4+-N and NO3-N were 0.36, 0.15, 0.032 and 0.82 g/day. High-throughput sequencing results showed that uncultured_bacterium_f_Burkholderiaceae (5.20%), OLB8 (1.04%) and Ottowia (1.03%) played an important role in denitrification in the R zone. This study provided effective guidance for the design and operation of the R-MAO process in domestic sewage treatment.  相似文献   

5.
Herein, we found that anthraquinone (AQ) acted as a catalyst for the rapid and effective removal of triphenylmethane dye containing tertiary amino group (TDAG). Results showed that AQ had an enhanced catalytic reactivity towards the removal of TDAG compared to hydro-quinone, which was further proved and explained using density functional theory (DFT) calculations. AQs could achieve a TDAG removal efficiency and rate of approximately 100% and 0.3583 min−1, respectively, within 20 min. Quenching experiments and electron paramagnetic resonance (EPR) tests indicated that the superoxide radical (O2•−) generated through the catalytic reduction of an oxygen molecule (O2) by AQ contributed to the effective removal of the TDAG. In addition, it was found that the electrophilic attack of the O2•− radical on the TDAG was the driving force for the dye degradation process. Decreasing the pH led to protonation of the substituted group of AG, which resulted in formation of an electron deficient center in the TDAG molecule (TDAG-EDC+) through delocalization of the π electron. Therefore, the possibility of the electrophilic attack for the dye by the negative O2•- radical was significantly enhanced. This study revealed that the H+ and the O2•− generated by the catalytic reduction of O2 have synergistic effects that led to a significant increase in the dye removal rate and efficiency, which were higher than those obtained through persulfate oxidation.  相似文献   

6.
Recycling strongly acidic wastewater as diluted H2SO4 after contaminants contained being removed was previously proposed, however, Cl(-I), a kind of contaminant contained in strongly acidic wastewater, is difficult to remove, which severely degrades the quality of recycled H2SO4. In this study, the removal of Cl(-I) using PbO2 was investigated and the involved mechanisms were explored. The removal efficiency of Cl(-I) reached 93.38% at 50℃ when PbO2/Cl(-I) mole ratio reached 2:1. The identification of reaction products shows that Cl(-I) was oxidized to Cl2, and PbO2 was reduced to PbSO4. Cl2 was absorbed by NaOH to form NaClO, which was used for the regeneration of PbO2 from the generated PbSO4. Cl(-I) was removed through two pathways, i.e., surface oxidation and •OH radical oxidation. •OH generated by the reaction of PbO2 and OH plays an important role in Cl(-I) removal. The regenerated PbO2 had excellent performance to remove Cl(-I) after six-time regeneration. This study provided an in-depth understanding on the effective removal of Cl(-I) by the oxidation method.  相似文献   

7.
In order to enhance the removal performance of graphitic carbon nitride (g-C3N4) on organic pollutant, a simultaneous process of adsorption and photocatalysis was achieved via the compounding of biochar and g-C3N4. In this study, g-C3N4 was obtained by a condensation reaction of melamine at 550°C. Then the g-C3N4/biochar composites were synthesized by ball milling biochar and g-C3N4 together, which was considered as a simple, economical, and green strategy. The characterization of resulting g-C3N4/biochar suggested that biochar and g-C3N4 achieved effective linkage. The adsorption and photocatalytic performance of the composites were evaluated with enrofloxacin (EFA) as a model pollutant. The result showed that all the g-C3N4/biochar composites displayed higher adsorption and photocatalytic performance to EFA than that of pure g-C3N4. The 50% g-C3N4/biochar performed best and removed 45.2% and 81.1% of EFA (10 mg/L) under darkness and light with a dosage of 1 mg/mL, while g-C3N4 were 19.0% and 27.3%, respectively. Besides, 50% g-C3N4/biochar showed the highest total organic carbon (TOC) removal efficiency (65.9%). Radical trapping experiments suggested that superoxide radical (?O2?) and hole (h+) were the main active species in the photocatalytic process. After 4 cycles, the composite still exhibited activity for catalytic removal of EFA.  相似文献   

8.
Triphenylmethane (tpm) derivatives (e.g. tpmCV) have threatened the safety of the aquatic environment due to the potential toxicity and carcinogenicity. In this study, the novel ultrasonic/persulfate/chlorite (US/S2O82−/ClO2) oxidation process was developed for the effective removal of tpmCV in wastewater. The apparent non-integer kinetics (n around 1.20) of tpmCV degradation under different factors (R2Adj > 0.990) were investigated, respectively. Inhibiting effects of anions were greater than those of cations (except Fe(II/III)). The adding of micromolecule organic acids could regulate degradation towards positive direction. The double response surface methodology (RSM) was designed to optimize tpmCV removal process, and the acoustic-piezoelectric interaction was simulated to determine the propagation process of acoustic wave in the reactor. The possible degradation pathway was explored to mainly include carbonylation, carboxylation, and demethylation. The estimated effective-mean temperature at the bubble-water interface was calculated from 721 to 566 K after introducing the ClO2, however, the adsorption or partitioning capacity of tpmCV in the reactive zone was widened from 0.0218 to 0.0982. The proposed co-catalysis of US/S2O82−/ClO2 was based on the determined active species mainly including ClO2, SO4, and OH. Compared with other US-based processes, the operating cost (3.97 $/m3) of US/S2O82−/ClO2 with the EE/O value (16.8 kWh/m3) was relatively reduced.  相似文献   

9.
This study investigated the enhancement effects of dissolved carbonates on the peroxymonosulfate-based advanced oxidation process with CuS as a catalyst. It was found that the added CO32− increased both the catalytic activity and the stability of the catalyst. Under optimized reaction conditions in the presence of CO32−, the degradation removal of 4-methylphenol (4-MP) within 2 min reached 100%, and this was maintained in consecutive multi-cycle experiments. The degradation rate constant of 4-MP was 2.159 min−1, being 685% greater than that in the absence of CO32− (0.315 min−1). The comparison of dominated active species and 4-MP degradation pathways in both CO32−-free and CO32−-containing systems suggested that more CO3/1O2 was produced in the case of CO32−deducing an electron transfer medium, which tending to react with electron-rich moieties. Meanwhile, Characterization by X-ray photoelectron spectroscopic and cyclic voltammetry measurement verified CO32− enabled the effective reduction of Cu2+ to Cu+. By investigating the degradation of 11 phenolics with different substituents, the dependence of degradation kinetic rate constant of the phenolics on their chemical structures indicated that there was a good linear relationship between the Hammett constants σp of the aromatic phenolics and the logarithm of k in the CO32−-containing system. This work provides a new strategy for efficient removal of electron-rich moieties under the driving of carbonate being widely present in actual water bodies.  相似文献   

10.
Single particle-inductively coupled plasma mass spectrometry (SP-ICP-MS) is a powerful tool for size-characterization of metal-containing nanoparticles (MCNs) at environmentally relevant concentrations, however, coexisting dissolved metal ions greatly interfere with the accuracy of particle size analysis. The purpose of this study is to develop an online technique that couples hollow fiber ultrafiltration (HFUF) with SP-ICP-MS to improve the accuracy and size detection limit of MCNs by removing metal ions from suspensions of MCNs. Through systematic optimization of conditions including the type and concentration of surfactant and complexing agent, carrier pH, and ion cleaning time, HFUF completely removes metal ions but retains the MCNs in suspension. The optimal conditions include using a mixture of 0.05 vol.% FL-70 and 0.5 mmol/L Na2S2O3 (pH = 8.0) as the carrier and 4 min as the ion cleaning time. At these conditions, HFUF-SP-ICP-MS accurately determines the sizes of MCNs, and the results agree with the size distribution determined by transmission electron microscopy, even when metal ions also are present in the sample. In addition, reducing the ionic background through HFUF also lowers the particle size detection limit with SP-ICP-MS (e.g., from 28.3 to 14.2 nm for gold nanoparticles). This size-based ion-removal principle provided by HFUF is suitable for both cations (e.g., Ag+) and anions (e.g., AuCl4) and thus has good versatility compared to ion exchange purification and promising prospects for the removal of salts and macromolecules before single particle analysis.  相似文献   

11.
Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis (DGGE) and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity (both in gene richness and diversity index values) and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor (50 mg/kg) recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos (150 mg/kg) caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos (250 mg/kg) produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes (bands) responded differently to the impact of agrochemicals: four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.  相似文献   

12.
Phytoremediation is a potential cleanup technology for the removal of heavy metals from contaminated soils.Bidens maximowicziana is a new Pb hyperaccumulator,which not only has remarkable tolerance to Pb but also extraordinary accumulation capacity for Pb.The maximum Pb concentration was 1509.3 mg/kg in roots and 2164.7 mg/kg in overground tissues.The Pb distribution order in the B. maximowicziana was:leaf>stem>root.The effect of amendments on phytoremediation was also studied.The mobility of soil Pb and the Pb concentrations in plants were both increased by EDTA application.Compared with CK(control check),EDTA application promoted translocation of Pb to overground parts of the plant.The Pb concentrations in overground parts of plants was increased from 24.23-680.56 mg/kg to 29.07-1905.57 mg/kg.This research demonstrated that B.maximowicziana appeared to be suitable for phytoremediation of Pb contaminated soil,especially,combination with EDTA.  相似文献   

13.
Laogang landfill near Shanghai is the largest landfill in China, and receives about 10000 t of daily garbage per day, Samples of topsoil and plants were analyzed to evaluate mercury pollution from the landfill. For topsoil samples, there were significant correlations among total mercury (HgT), combinative mercury (Hgc) and gaseous mercury (HgG), and content of total organic carbon (TOC), but, no significantly relationship was found between Hg content and filling time. Hg content changes in vertical profiles with time showed that the average Hgv of profiles 1992, 1996, and 2000 was similar, but their average HgG was quite different. HgT was significantly correlated with Hgc in profile 1992 and 2000, and Hgv was significantly correlated with Hg6 in profile 1996. HgG/Hgv ratio in profile samples decreased in the order of (HgG,/HgT)1992〉(HgG/HgT)1996〉〉(HgG/HgT)2000. A simple outline of Hg release in landfill could be drawn: with increasing of filling time, degradation undergoes different biodegradation, accordingly, gaseous mercury goes through small, more, and small proportion to total mercury. Distribution of Hg in plants was inhomogeneous, following the order of leaf〉root〉stem. The highest value of leaf may be associated with higher atmospheric Hg from landfill. Ligneous plants (e.g. Phyllostachys glanca, Prunus salicina and Ligustrum lucidum) are capable of enriching more Hg than herbaceous plants.  相似文献   

14.
The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.  相似文献   

15.
The influence of the nonionic surfactant Tween 80 on pentachlorophenol (PCP) oxidation catalyzed by horseradish peroxidase was studied. The surfactant was tested at concentrations below and above its critical micelle concentration (CMC). Enhancement of PCP removal was observed at sub-CMCs. The presence of Tween 80 in the reaction mixture reduced enzyme inactivation which occurred through a combination of free radical attack and sorption by precipitated products. A simple first-order model was able to simulate time profiles for enzyme inactivation in the presence or absence of Tween 80. At supra-CMCs, the surfactant caused noticeable reductions in PCP removal, presumably through micelle partitioning of PCP which precluded the hydrophobic PCP molecule from interacting with the enzyme.  相似文献   

16.
Decomposition of alachlor by ozonation and its mechanism   总被引:1,自引:0,他引:1  
Decomposition and corresponding mechanism of alachlor, an endocrine disruptor in water by ozonation were investigated. Results showed that alachlor could not be completely mineralized by ozone alone. Many intermediates and final products were formed during the process, including aromatic compounds, aliphatic carboxylic acids, and inorganic ions. In evoluting these products, some of them with weak polarity were qualitatively identified by GC-MS. The information of inorganic ions suggested that the dechlorination was the first and the fastest step in the ozonation of alachlor.  相似文献   

17.
Several main metabolites of benzo[a]pyrene (BaP) formed by Penicillium chrysogenum, Benzo[a]pyrene-1,6-quinone (BP 1,6- quinone), trans-7,8-dihydroxy-7,8-dihydrobenzo[a]pyrene (BP 7,8-diol), 3-hydroxybenzo[a]pyrene (3-OHBP), were identified by high-performance liquid chromatography (HPLC). The three metabolites were liable to be accumulated and were hardly further metabolized because of their toxicity to microorganisms. However, their further degradation was essential for the complete degradation of BaP. To enhance their degradation, two methods, degradation by coupling Penicillium chrysogenum with KMnO4 and degradation only by Penicillium chrysogenum, were compared; Meanwhile, the parameters of degradation in the superior method were optimized. The results showed that (1) the method of coupling Penicillium chrysogenum with KMnO4 was better and was the first method to be used in the degradation of BaP and its metabolites; (2) the metabolite, BP 1,6-quinone was the most liable to be accumulated in pure cultures; (3) the effect of degradation was the best when the concentration of KMnO4 in the cultures was 0.01% (w/v), concentration of the three compounds was 5 mg/L and pH was 6.2. Based on the experimental results, a novel concept with regard to the bioremediation of BaP-contaminated environment was discussed, considering the influence on environmental toxicity of the accumulated metabolites.  相似文献   

18.
Sorption of chlorotoluron in ammonium sulfate, urea and atrazine multi-solutes system was investigated by batch experiments. The results showed application of nitrogen fertilizers to the soil could affect the behavior of chlorotoluron. At the same concentration of N, sorption of chlorotoluron decreased as the concentration of atrazine increased on the day 0 and 6 in soil, respectively. The sorption of chlorotoluron increased from 0 to 6 d when soils were preincubated with deionized water, ammonium sulfate and urea solution for 6 d. That indicated incubation time was one of the most important factors for the sorption of chlorotoluron in nitrogen fertilizers treatments. The individual sorption isotherms of chlorotoluron in rubbery polymer and silica were strictly linear in single solute system, but there were competition sorption between pesticides or between pesticides and nitrogen fertilizers. That indicated the sorption taken place by concurrent solid-phase dissolution mechanism and sorption on the interface of water-organic matter or water-mineral matter.  相似文献   

19.
以三峡大学的校园河道求索溪为研究对象,利用综合水质标识指数法确定求索溪水质类别,分析其水质时空变化规律,并利用对应分析法得出求索溪中不同监测点的主要污染因子.研究结果表明:求索溪整体的综合水质标识指数为7.423,整体水质为劣V类(地表水环境质量标准GB 3838-2002)且黑臭.从时间变化来看,求索溪4月份的水质最差,5月份次之,4、5月份所有监测点的水质都劣于V类且黑臭;8月份水质最好,水质为Ⅳ类;从空间分布来看,8个监测点综合水质标识指数均超过6.0,水质为劣V类,其中6号监测点的水质相对最好,监测点3号的水质相对最差;对应分析法得出求索溪的整体水体污染程度受总氮因子的影响最大,其次为总磷.该研究拟为求索溪及类似校园河道的水环境治理研究提供基础依据和参考.  相似文献   

20.
In this study an effort has been made to use plant polyphenol oxidases; potato (Solanum tuberosum) and brinjal (Solanum melongena), for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.  相似文献   

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