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PubMed2004

Degradation of 2-chlorophenol via a hydrogenotrophic biofilm under different reductive conditions.

This research studies the 2-chlorophenol (2-CP) degradation by the hydrogenotrophic biofilm cultivated in three silicone-tube membrane bioreactors under the conditions of denitrification (DN), sulfate-reduction (DS) and dechlorination (DC). Experimental results showed that after acclimation for more than four months with 2-CP, the respective 2-CP removal efficiency was 95% in DN, 94% in DS and 95% in DC reactors, under the condition of influent 2-CP 25 mg/l with hydraulic retention time (HRT) of 15 h. The metabolic pathway of 2-CP was different in different reactors. The 2-CP was thought to be utilized as carbon and energy source in DN and DS reactors, while the dechlorination occurred in the DC reactor in lack of nitrate and sulfate. The pH dramatically affected the 2-CP degradation in all reactors. Experimental results showed that the optimal pH range was around 6+/-0.2 in DN, 7+/-0.2 in DS, and 5.8-7.2 in DC reactors. Both nitrate and sulfate inhibited the 2-CP dechlorination, but the inhibition levels were different. Nitrate completely inhibited the dechlorination at once, while sulfate took a longer time to reach complete inhibition, only after the bacteria were adapted to the sulfate-reducing condition. Both inhibitions were accomplished by taking the place of 2-CP as electron acceptors. H2 served as an electron donor for dechlorination of 2-CP. The dechlorination was apparently stopped when lacking H2 and another pathway was responsible for the 2-CP degradation.

Biofilms↗
PubMed2005

Characterization and microbial utilization of dissolved organic carbon in groundwater contaminated with chlorophenols.

The aim of this study was to characterize the labile part of dissolved organic carbon (DOC) present in groundwater by identification of natural organic carbon substrates and to assess their microbial utilization during aeration of the groundwater. The studied chlorophenol (CP) contaminated groundwater contained 60-2650 micromoll(-1) of DOC of which up to 98.0% were CPs; 1.7% were low-molecular weight organic acids and 0.2% were dissolved free amino acids. Traces of following natural organic carbon substrates were identified: L-alanine, L-isoleucine, L-leucine, L-serine, L-threonine, L-tyrosine, L-valine, L-aspartic, acetic, citric, formic, lactic, malic and oxalic acid. Dissolved oxygen concentration inside the CP-plume was lower (mean 25 micromoll(-1)) than outside of the plume (mean 102 micromoll(-1)). Over a monitoring period of four years the concentrations of CPs, Fe(II) and NH4+ were higher inside than outside of the CP-plume. Oxygen availability within the CP-plume limits in situ biological oxidation of CPs, DOC, NH4+ and Fe(II). The microbial enzymatic hydrolysis rates of 4-methylumbelliferyl and 7-amino-4-methylcoumarin-linked substrates varied from 0.01 to 52 micromoll(-1)h(-1) and was slightly higher inside than outside the plume. Microbial uptake rates of 14C-acetate, 14C-glucose and 14C-leucine were on average 28, 4 and 4 pmoll(-1)h(-1) outside and 17, 25 and 8 pmoll(-1)h(-1) inside the plume, respectively. The indigenous microorganisms were shown able of hydrolysis of dissolved organic matter, uptake and utilization of natural organic carbon substrates. Therefore, the labile part of DOC serves as a pool of secondary substrates beside the CP-contaminants in the groundwater and possibly help in sustaining the growth of CP-degrading bacteria.

Bacteria↗
PubMed2005

Degradation of 4-chlorophenol by microwave irradiation enhanced advanced oxidation processes.

In this work the synergistic effects of several microwave assisted advanced oxidation processes (MW/AOPs) were studied for the degradation of 4-chlorophenol (4-CP). The efficiencies of the degradation of 4-CP in dilute aqueous solution for a variety of AOPs with or without MW irradiation were compared. The results showed that the synergistic effects between MW and H2O2, UV/H2O2, TiO2 photocatalytic oxidation (PCO) resulted in a high degradation efficiency for 4-CP. The potential of MW/AOPs for treatment of industrial wastewater is discussed.

Chlorophenols↗
PubMed2005

Experimental study on the thermal oxidation of 2-chlorophenol in air over the temperature range 450-900 degrees C.

The thermal oxidation of 2-chlorophenol (2-CP) in air was investigated using a perfectly stirred reactor at 1 atm over the temperature range 450-900 degrees C. The relative concentration of 2-CP was 1,000 ppm V (equivalence ratio Phi=0.03). About fifty organic products were identified as trace species. The concentration profiles of 2-CP, carbon oxides as well as those of seventeen major organic intermediates and six non-to-lower chlorinated dioxins and furans were presented as a function of temperature for a residence time of 2s. The most abundant intermediate products were carbon monoxide, 2H-pyran-2-one, chlorobenzene, 4-cyclopenten-1,3-dione, phenol, benzofuran, 2-chlorohydroquinone and 2-indanone. These concentration profiles have revealed that temperatures of at least 900 degrees C were needed to completely oxidize 2-CP, CO and all other organic byproducts to carbon dioxide. Reaction pathways accounting for the formation of most observed products are proposed.

Air↗
PubMed2006

2-chlorophenol induced ROS generation in fish Carassius auratus based on the EPR method.

In the present study, a secondary spin trapping technique was used followed by electron paramagnetic resonance (EPR) analysis, to study the potential of reactive oxygen species (ROS) production after fish (Carassius auratus) were injected i.p. with different doses (50, 100, 200, 250, 500mgkg(-1)) of 2-chlorophenol (2-CP). The ROS signal intensity of the EPR spectrum showed a significant increase (p<0.05, compared with the control) when the 2-CP dose was as low as 50mgkg(-1). There is a good relationship between the 2-CP administered doses and ROS generation. Based on the hyperfine splitting constants and shape of the EPR spectrum, the ROS which was generated in fish liver after intraperitoneal (i.p.) injection of 2-CP was identified as ()OH. SOD and CAT activities were found to be induced at lower doses of 2-CP. GSH levels fell below the control level following all treatments with 2-CP, and GSSG levels changed along with those of GSH. These observations indicated that the fish experienced oxidative stress. The strong positive correlation (r=0.966, p<0.005) between ()OH radical and lipid peroxidation suggested that lipid peroxidation was possibly induced by ()OH. The phase II detoxification enzyme glutathione-S-transferase (GST) may play an important role in 2-CP metabolism or excretion and, consequently, reduce ROS production. This study provides strong evidence that level of ROS is significantly increased in 2-CP stressed fish, and ROS may serve as a potential biomarker to indicate 2-CP contamination.

Animals↗
PubMed2006

Effects of potassium alkalis and sodium alkalis on the dechlorination of o-chlorophenol in supercritical water.

Effects of potassium alkalis and sodium alkalis on the dechlorination of o-chlorophenol (o-CP) in supercritical water (SCW) were studied in this paper under the conditions of 450 degrees C and 25 MPa. Experimental results indicated that the dechlorination of o-CP can be accelerated significantly by all alkalis investigated. The dechlorination of o-CP proceeded mainly via two pathways: hydrodechlorination and hydrolysis. Both of the two pathways can be promoted by alkalis, and the dechlorination of o-CP can be accelerated by both the cations and hydroxide ion dissociated from alkalis. The overall dechlorination of o-CP can be accelerated by cations via promoting the hydrodechlorination pathway, while, hydroxide ion via promoting the hydrolysis pathway. In addition, the hydrodechlorination can be accelerated faster by sodium alkalis than that by potassium ones, while, the hydrolysis can be promoted faster by potassium alkalis. This difference may be caused by the different charge density between potassium ion and sodium ion, and the different solubility and dissociation constant between potassium alkalis and sodium alkalis in SCW. Dechlorination of o-CP with addition of alkalis prior to supercritical water oxidation (SCWO) process not only can avoid the reactor corrosion caused by the generated hydrochloric acid in direct SCWO of o-CP, but also can reduce the formation of toxic chlorinated byproducts compared with direct SCWO process or SCWO of o-CP with addition of alkali.

Alkalies↗
PubMed2006

The QSPR (quantitative structure-property relationship) study about the anaerobic biodegradation of chlorophenols.

In this study, based on quantum chemical and physicochemical descriptors, by the use of partial least squares analysis, a good prediction quantitative structure-property relationship for the disappearance rate constant (logK) of chlorophenols (CPs) in the anaerobic culture was obtained. It was found that the resonance energy of the two-center term (J), which described the character of the weakest carbon-chlorine bond, played an important role in the reductive chlorine processes, the greater the sizes of CPs molecules, the higher the logK values. Increasing energy of the lowest unoccupied molecular orbital (E(lumo)) values of the CPs lead to decreasing logK values, and CPs with large absolute hardness values tended to have big logK values.

Anaerobiosis↗
PubMed2006

Electrochemical degradation of 4-chlorophenol at nickel-antimony doped tin oxide electrode.

The effectiveness of a novel nickel-antimony doped tin oxide electrode for electrochemical degradation of organic pollutants was investigated using 4-chlorophenol (4-CP) as a model toxic organic. The experimental results demonstrate that the optimal Ni content was at Ni:Sn=1:500 in atomic ratio in the precursor coating solution, whereas the Sb:Sn ratio was set at 8:500. Using the electrode prepared with the optimal Ni doping ratio for 4-CP degradation, the charge-based efficiencies were up to 89 microg C(-1) for 4-CP destruction and 15 microg C(-1) for TOC removal, which were considerably higher than the efficiencies observed for other electrodes. It is suggested that the enhancement of the electrode for electrochemical oxidation of organics could be attributed to the production of hydroxyl radicals in anodic water electrolysis.

Antimony↗
PubMed2006

Pulsed discharge plasma induced Fenton-like reactions for the enhancement of the degradation of 4-chlorophenol in water.

To sufficiently utilize chemically active species and enhance the degradation rate and removal efficiency of toxic and biorefractory organic pollutant para-chlorophenol (para-CP), the introductions of iron metal ions (Fe2+/Fe3+) into either pulsed discharge plasma (PDP) process or the PDP process with TiO2 photo-catalyst were tentatively performed. The experimental results showed that under the same experimental condition, the degradation rate and removal efficiency of para-CP were greatly enhanced by the introduction of iron ions (Fe2+/Fe3+) into the PDP process. Moreover, when iron ions and TiO2 were added together in the PDP process, the degradation rate and removal energy of para-CP further improved. The possible mechanism was discussed that the obvious promoting effects were attributed to ferrous ions via plasma induced Fenton-like reactions by UV light irradiation excited and hydrogen peroxide formed in pulsed electrical discharge, resulting in a larger amount of hydroxyl radicals produced from the residual hydrogen peroxide. In addition, the regeneration of ferric ions to ferrous ions facilitates the progress of plasma induced Fenton-like reactions by photo-catalytic reduction of UV light, photo-catalytic reduction on TiO2 surface and electron transfer of quinone intermediates, i.e. 1,4-hydroquinone and 1,4-benzoquinone.

Catalysis↗
PubMed2006

Degradation mechanisms of 4-chlorophenol in a novel gas-liquid hybrid discharge reactor by pulsed high voltage system with oxygen or nitrogen bubbling.

The effect of gas bubbling on the removal efficiency of 4-chlorophenol (4-CP) in aqueous solution has been investigated using a novel pulsed high voltage gas-liquid hybrid discharge reactor, which generates gas-phase discharge above the water surface simultaneously with the spark discharge directly in the liquid. The time for 100% of 4-CP degradation in the case of oxygen bubbling (7 min) was much shorter than that in the case of nitrogen bubbling (25 min) as plenty of hydrogen peroxide and ozone formed in oxygen atmosphere enhanced the removal efficiency of 4-CP. Except for the main similar intermediates (4-chlorocatechol, hydroquinone and 1,4-benzoquinone) produced in the both cases of oxygen and nitrogen bubbling, special intermediates (5-chloro-3-nitropyrocatechol, 4-chloro-2-nitrophenol, nitrate and nitrite ions) were produced in nitrogen atmosphere. The reaction pathway of 4-CP in the case of oxygen bubbling was oxygen/ozone attack on the radical hydroxylated derivatives of 4-CP. However, in the case of nitrogen bubbling, hydroxylation was the main reaction pathway with effect of N atom on degradation of 4-CP.

Chlorophenols↗
PubMed2005

Multi-walled carbon nanotubes as a solid-phase extraction adsorbent for the determination of chlorophenols in environmental water samples.

Multi-walled carbon nanotubes (MWCNs) are used as adsorbent for solid-phase extraction (SPE) of several chlorophenols (CPs). CPs were adsorbed on MWCNs cartridge, then desorbed with pH 10.0 methanol, finally determined by HPLC. Under the optimized conditions, detection limits of 0.08-0.8 ng mL(-1) were obtained. The method had been applied to analyze the five CPs in tap water and river water.

Adsorption↗
PubMed2005

Multiple solid-phase microextraction in a non-equilibrium situation. Application in quantitative analysis of chlorophenols and chloroanisoles related to cork taint in wine.

Multiple HS-solid-phase microextraction (MHS-SPME) is a modification of SPME developed for quantitative analysis that avoids possible matrix effects based on an exhaustive analyte extraction from the sample. In this paper, the theory of this process associated with a non-equilibrium situation has been presented. The application of an optimised HS-SPME-based method in the analysis of chloroanisoles and chlorophenols, previously acetylated, associated with the occurrence of cork taint in different red, white and rosé wine samples, has revealed the existence of matrix effects. This fact determines the choice of standard addition as the adequate technique for the quantification of these compounds in real samples. MHS-SPME is proposed as a good alternative technique with respect to HS-SPME because it avoids matrix effects, simplifies the quantification of these compounds in real samples and reduces analysis time, providing sensitivity below chloroanisole sensory threshold with acceptable precision.

Anisoles↗
PubMed2005

Vial position in the determination of chlorophenols in water by solid phase microextraction.

The extraction of chlorophenol from water by headspace solid phase microextraction (HS-SPME) in vials located both vertically and horizontally is compared. The results obtained show that kinetic parameters are clearly affected by how the vial is placed in the analysis of semivolatile compounds. Extraction time for reach the equilibrium was three times lower in the horizontal configuration. An on-line extraction unit coupled to a continuous flow system is used to analyse unmodified ground water samples. In order to increase the high throughput, the analysis time is reduced and the sensitivity increased by making the extraction simultaneously with two fibres. The proposed method is applied to the analysis of spiked river water samples. The precision expressed as relative standard deviation ranges from 3.5 to 4.8%, and the recoveries from 94 to 105%.

Chemical Fractionation↗
PubMed2006

Assays on the simultaneous determination and elimination of chloroanisoles and chlorophenols from contaminated cork samples.

A method for the simultaneous determination of the chloroanisoles and chlorophenols in cork samples with gas chromatography has been evaluated in view to its application. All the stages of the suggested procedure have been submitted to an in-depth examination using spiked ground corks. The recoveries of the method, which involves a simultaneous extraction with n-pentane followed by a second extraction using an aqueous basic solution where the phenolic derivates are transferred and, subsequently, derivatised, have been satisfactory for the all analytes at the studied spiking concentration levels. Good precision data and limits of detection between 1 ng/g and 2 ng/g were obtained for almost all compounds. As real samples, naturally contaminated cork slabs taken from different sources have been analysed, showing the presence of 2,4,6-trichloroanisole (TCA) and, in lesser extent, its direct precursor, 2,4,6-trichlorophenol (TCP). Removal studies have been performed by washing these tainted cork slabs with different solutions: Milli-Q water, sodium hydroxide and commercial products. Sodium hydroxide solutions have led to better analyte elimination, and the complete removal of TCP from the cork has been accomplished together with 72% of TCA reduction has been achieved.

Anisoles↗
PubMed2006

Rapid, one-pot derivatization and distillation of chlorophenols from solid samples with their on-line enrichment.

A microwave-assisted steam distillation (MASD) sample preparation technique for extracting chlorophenols from solid samples was studied. This open vessel microwave system based study developed as an integrated method since it has incorporated extractive distillation, derivatization and on-line enrichment. Gas chromatography (GC) with electron-capture detection was used for the analysis. The study involved optimization of MASD parameters and on-line enrichments using spiked solid samples. MASD achieved recoveries for spiked soil samples in the range of 94-101% within 20min with a collection of only 20ml distillate facilitating on-line enrichment. Some real samples were analyzed that included soil, wood, leather, textiles, dyes and certified reference materials of soil and wood samples. Limit of detection values of 12ng/g for pentachlorophenol and 194ng/g for monochlorophenol were found. Recoveries of 96.6% in the case of soil certified reference material (CRM) with RSD 2.7% and 80.6% in the case of wood CRM with RSD 3.3% were observed in this study. MASD studied found to produce very clean extracts in comparison to reference techniques.

Chemical Fractionation↗
PubMed2005

Bioconcentration of atrazine and chlorophenols into roots and shoots of rice seedlings.

Accumulation of o-chlorophenol (CP), 2,4-dichlorophenol (DCP), and atrazine (ATR), as single and mixed contaminants, from hydroponic solutions into roots and shoots of rice seedlings was studied following 48-h exposure of the plant roots. As single contaminants at low levels, the observed bioconcentration factors (BCFs) of CP and DCP with roots approximated the equilibrium values according to the partition-limited model. The BCF of atrazine with roots was about half the partition limit for unknown reasons. The BCFs of CP and ATR with shoots also approximated the partition limits, while the BCF for more lipophilic DCP with shoots was about half the estimated limit, due to insufficient water transport into plants for DCP. As mixed contaminants at low levels, the BCFs with both roots and shoots were comparable with those for the single contaminants; at high levels, the BCFs generally decreased because of the enhanced mixed-contaminant phytotoxicity, as manifested by the greatly reduced plant transpiration rate.

Anthelmintics↗
PubMed2005

Biodegradation of 4-chlorophenol by acclimated and unacclimated activated sludge--evaluation of biokinetic coefficients.

Unacclimated and acclimated activated sludges were examined for their ability to degrade 4-CP (4-chlorophenol) in the presence and absence of a readily growing substrate using aerobic batch reactors. The effects of 4-CP on the micro (specific growth rate), COD removal efficiency, Y (yield coefficient), and q (specific substrate utilization rate) were investigated. It was observed that the toxicity of 4-CP on the culture decreased remarkably after acclimation. For example, the IC(50) value on the basis of micro was found to increase from 130 to 218 mg/L with the acclimation of the culture. Although an increase in 4-CP concentration up to 300 mg/L has no adverse effect on the COD removal efficiency of the acclimated culture, a considerable decrease was observed in the case of an unacclimated culture. Although 4-CP removal was not observed with an unacclimated culture, almost complete removal was achieved with the acclimated culture, up to 300 mg/L. The Haldane kinetic model adequately predicted the biodegradation of 4-CP and the kinetic constants obtained were q(m)=41.17 mg/(gMLVSSh), K(s)=1.104 mg/L, and K(i)=194.4 mg/L. The degradation of 4-CP led to formation of 5-chloro-2-hydroxymuconic semialdehyde, which was further metabolized, indicating complete degradation of 4-CP via a meta-cleavage pathway.

Adaptation, Physiological↗
PubMed2004

Capability of coupled CdSe/TiO(2) for photocatalytic degradation of 4-chlorophenol.

The photocatalytic process using TiO(2) and coupled semiconductor in the photodegradation reaction of 4-chlorophenol (4-CP) was investigated. Nanosized titanium dioxide powder was synthesized via the sol-gel procedure and modified via the coupled photocatalysts. The microstructural and chemical properties of TiO(2) and coupled CdSe/TiO(2) were also examined. For CdSe/TiO(2) samples, the specific surface area was 7.0 m(2)/g and the deposition proportion of CdSe was approximately 27.6%. In the photocatalysis results, higher photodegradation efficiency of 4-CP was observed at higher pH values. In the UV 254 nm system, the degradation efficiency of 4-CP and TOC with sol-gel produced TiO(2) (TiO(2)(SG)) powder was higher than with commercial TiO(2)(RdH) powder. For the coupled semiconductor system (CdSe/TiO(2)), the apparent first-order rate constants were 1.35 x 10(-2), 4.33 x 10(-2), 2.0 x 10(-3) and 1.9 x 10(-3)min(-1) at the conditions of pH 7 (254 nm), pH 11 (254nm), pH 7 (365 nm), and pH 11 (365 nm). The disappearance of 4-CP under CdSe/TiO(2)(RdH) photoreaction at pH 7 and 365 nm condition is better than that of TiO(2)(RdH) system, with 30% versus 22% 4-CP reduction in 180 min. In the same condition, CdSe/TiO(2)(RdH) provided more photomineralization efficiency than that of TiO(2)(RdH) in terms of TOC reduction. Both 4-CP and TOC reduction were significant for systems illuminated at 254 nm. Considering the direct photolysis effect at 254 nm where 4-CP reduction is near 100% and TOC removal is nil, CdSe/TiO(2)(RdH) exhibits a 50% photomineralization efficiency and a nearly four times faster reaction rate than the single TiO(2)(RdH) semiconductor.

Cadmium Compounds↗