Reductive dechlorination of polychlorinated biphenyls as affected by sediment characteristics

The effect of sediment sources on the selection of polychlorinated biphenyl (PCB) dechlorinating competence was investigated using sediments from two different locations, the Grasse River and Owasco Lake. These two sediments had a similar organic carbon content but different particle size distribution. The two PCB-free sediments were spiked with Aroclor 1248 and inoculated with microorganisms from the Reynolds and General Motors sites in the St. Lawrence River, which exhibited different dechlorination patterns. When each inoculum was serially transferred into fresh sediments four times (every 8-10 weeks), they still maintained the initial dechlorination patterns regardless, the source of sediments and the number of transfers, and dechlorination patterns of the two inocula in the same sediments did not converge. In a parallel approach, when the acclimated microorganisms from the Reynolds site were inoculated into fresh sediments from both sources as well as sediments enriched with organic carbon (2%, w/v), the dechlorination pattern remained unchanged after a 40-week incubation. These results suggest that the sediment characteristics or organic carbon content did not play a role in the selection of dechlorinating populations.     

Carbon/electron source dependence of polychlorinated biphenyl dechlorination pathways for anaerobic granules

The effect of acclimating anaerobic granules from commercial bioreactors with different carbon/electron sources on their ability to reductively dechlorinate a tri-(2,3,4-CB) and heptachlorobiphenyl (2,2',3,3',4,5,6-CB) was studied. The anaerobic granules were first grown in upflow anaerobic sludge blanket (UASB) reactors fed with two different mixtures of carbon/electron sources, i.e., propionate/butyrate/methanol and formate/methanol. Differences in dechlorination patterns for 2,2',3,3',4,5,6-CB were observed in batch experiments inoculated with granules from these two sets of UASB reactors. Variation of the carbon/electron source, during the dechlorination process, had no effect on the dechlorination pathway, but the extents and rates of dechlorination were highest for ethanol and formate and lowest for pyruvate fed batches. Pre-acclimation of different anaerobic sludges to polychlorinated biphenyls (PCBs) shortened the lag period, but did not influence the PCB dechlorination pathway. This is the first time that similar acclimation conditions for several anaerobic microbial communities prior to inoculation were reported to yield similar substrate specificities for the reductive dechlorination of specific PCB congeners. This research demonstrates a successful strategy for the development of biocatalysts to serve as the inoculum of partially decontaminated sites in order to provide microorganisms with specificities complementary to those of naturally occurring dechlorinators.     

A case of polychlorinated biphenyl contamination of water and sediment in the Slovenian karst region (Yugoslavia)

An incident is described in which polychlorinated biphenyls (PCBs) from an electro-industrial plant waste tip draining into ground-water channels in karst terrain have contaminated a potable water source. PCB composition data were obtained using quadropole GC-MS and capillary GC. The average level of PCBs determined in water was 0.3 μg 1^?1 and in sediment 55 μg g^?1     

Reductive dechlorination of polychlorinated dibenzo-p-dioxins by zerovalent iron in subcritical water

A new method for reductive dechlorination of polychlorinated dibenzo-p-dioxins (PCDDs) and remediation of contaminated soils is described that uses zerovalent iron as the dechlorination agent and subcritical water as reaction medium and extractive solvent. It is found that the zerovalent iron can be applied for stepwise dechlorination of octachlorinated dibenzo-p-dioxin (OCDD) on various matrixes in subcritical water. By using iron powder as matrix higher chlorinated congeners were practically completely reduced to less than tetra-substituted homologues. A significant part of residual OCDD, when it was spiked in to soils, and formed less chlorinated congeners are extracted with water in the given conditions. The solubility of OCDD was increased by a 4–6 orders over its solubility at ambient conditions. The new method of contentious-flow extraction is described.     

Microbial reductive dechlorination of polychlorinated biphenyls in heat treated and bromoethanesulfonate treated anaerobic sediment slurries

Anaerobic reductive dechlorination of polychlorinated biphenyls (PCBs) in heat treated, bromoethanesulfonate (BES) treated, and untreated slurries of PCB-contaminated upper Hudson River sediment was investigated to better understand the microorganisms that mediate this process. Extensive meta-and para-dechlorination of Aroclor 1242 and 2,3,4-trichlorobiphenyl (2,3,4-CB) occurred in both the untreated and heat treated slurries. Heat treatment of the slurries eliminated methanogenesis, enhanced 2,3,4-CB dechlorination, and caused extensive meta- and para-dechlorination of Aroclor 1242 earlier than in untreated slurries. BES treatment (1 mM) of the slurries caused a 90% reduction in methanogenesis and inhibited metadechlorination of PCB congeners containing 2,3- and 2,5-dichlorophenyl groups. The results suggest that there are at least two distinct microbial PCB reductive dechlorination activities in PCB-contaminated upper Hudson River sediment, a meta-dechlorination activity and a para-dechlorination activity on Aroclor 1242. Both of these microbial activities are apparently not methanogenic and are resistant to or activated by heat treatment. In addition, the meta- but not the para-dechlorinating activity is inhibited by BES treatment.     

Evaluation of bioaugmentation and biostimulation on arsenic remediation in soil through biovolatilization

Arsenic (As) removal through microbially driven biovolatilization can be explored as a potential method for As bioremediation. However, its effectiveness needs to be improved. Biostimulation with organic matter amendment and bioaugmentation with the inoculation of genetic engineered bacteria could be potential strategies for As removal and site remediation. Here, the experiments were conducted to evaluate the impacts of rice straw and biochar amendment, inoculation of genetic engineered Pseudomonas putida KT2440 (GE P. putida) with high As volatilization activity, on microbial mediated As volatilization and removal from three different arseniferous soils. In general, the addition of rice straw (5%) significantly enhanced As methylation and volatilization in comparison with corresponding non-amended soils. Biochar amendments and inoculation of the GE P. putida increased As methylation and volatilization, respectively, but less than that of rice straw addition. The effectiveness of As volatilizations are quite different in the various paddy soils. The combined amendments of rice straw and GE P. putida exhibited the highest As removal efficiency (483.2 μg/kg/year) in Dayu soil, with 1.2% volatilization of the total As annually. The highest water-soluble As concentration (0.73 mg/kg) in this soil could be responsible for highest As volatilization besides the rice straw and bacteria in this soil.     

Dechlorination of polychlorinated biphenyl congeners by anaerobic microorganisms from river sediment.

The microbial dechlorination of seven kinds of polychlorinated biphenyls (PCBs) by anaerobic microorganisms from river sediment was investigated. Dechlorination rates were found to be affected by the chlorine level of PCB congeners; dechlorination rates decreased as chlorine levels increased. Dechlorination rates were fastest under methanogenic conditions and slowest under nitrate-reducing conditions. The addition of individual electron donors (acetate, pyruvate, and lactate) enhanced the dechlorination of PCB congeners under methanogenic and sulfate-reducing conditions but delayed the dechlorination of PCB congeners under nitrate-reducing conditions. PCB congener dechlorination also was delayed by the addition of various polycyclic aromatic hydrocarbons (PAHs) under three reducing conditions and by surfactants, such as brij30, triton SN70, and triton N101. The results suggest that methanogen, sulfate-reducing bacteria, and nitrate-reducing bacteria all are involved in the dechlorination of PCB congeners.     

Spatial distribution and partitioning of polychlorinated biphenyl and organochlorine pesticide in water and sediment from Sarno River and Estuary,Southern Italy

The Sarno River is nicknamed “the most polluted river in Europe”. The main goal of this study is to enhance our knowledge on the Sarno River water and sediment quality and on its environmental impact on the gulf of Naples (Tyrrhenian Sea, Central Mediterranean Sea) in order to become a useful assessment tool for the regional administrations. For these reasons, 32 selected polychlorinated biphenyls (PCBs) and aldrin, α-BHC, β-BHC, δ-BHC, γ-BHC (lindane), 4,4′-DDD, 4,4′-DDE, 4,4′-DDT, dieldrin, endosulfan I, endosulfan II, endosulfan sulphate, endrin, endrin aldehyde, heptachlor, heptachlor epoxide (isomer B) and methoxychlor were determined in the water dissolved phase (DP), suspended particulate matter (SPM) and sediments. Total concentrations of PCBs ranged from 1.4 to 24.9 ng L^?1 in water (sum of DP and SPM) and from 1.01 to 42.54 ng g^?1 in sediment samples. The concentrations of total organochlorine pesticides (OCPs) obtained in water (sum of DP and SPM) ranged from 0.54 to 7.32 ng L^?1 and from 0.08 to 5.99 ng g^?1 in sediment samples. Contaminant discharges of PCBs and OCPs into the sea were calculated in about 1,247 g day^?1 (948 g day^?1 of PCBs and 326 g day^?1 of OCPs), showing that this river should account as one of the main contribution sources of PCBs and OCPs to the Tyrrhenian Sea.     

Enhanced 1,2-dichloroethane degradation in heavy metal co-contaminated wastewater undergoing biostimulation and bioaugmentation

Biostimulation, bioaugmentation and dual-bioaugmentation strategies were investigated in this study for efficient bioremediation of water co-contaminated with 1,2-dichloroethane (1,2-DCA) and heavy metals, in a microcosm set-up. 1,2-DCA concentration was periodically measured in the microcosms by gas chromatographic analysis of the headspace samples, while bacterial population and diversity were determined by standard plate count technique and Polymerase chain reaction and denaturing gradient gel electrophoresis (PCR–DGGE) analysis, respectively. Dual-bioaugmentation, proved to be most effective exhibiting 22.43%, 26.54%, 19.58% and 30.49% increase in 1,2-DCA degradation in microcosms co-contaminated with As³⁺, Cd²⁺, Hg²⁺ and Pb²⁺, respectively, followed by bioaugmentation and biostimulation. Dual-bioaugmented microcosms also exhibited the highest increase in the biodegradation rate constant (k₁) resulting in 1.76-, 2-, 1.7- and 2.1-fold increase in As³⁺, Cd²⁺, Hg²⁺ and Pb²⁺ co-contaminated microcosms respectively, compared to the untreated microcosms. Dominant bacterial strains obtained from the co-contaminated microcosms were found to belong to the genera Burkholderia, Pseudomonas, Bacillus, Enterobacter and Bradyrhizobium, previously reported for 1,2-DCA and other chlorinated compounds degradation. PCR–DGGE analysis revealed variation in microbial diversity over time in the different co-contaminated microcosms. Results obtained in this study have significant implications for developing innovative bioremediation strategies for treating water co-contaminated with chlorinated organics and heavy metals.     

Reductive dechlorination of polychlorinated dibenzo-p-dioxins by zerovalent iron in subcritical water

A new method for reductive dechlorination of polychlorinated dibenzo-p-dioxins (PCDDs) and remediation of contaminated soils is described that uses zerovalent iron as the dechlorination agent and subcritical water as reaction medium and extractive solvent. It is found that the zerovalent iron can be applied for stepwise dechlorination of octachlorinated dibenzo-p-dioxin (OCDD) on various matrixes in subcritical water. By using iron powder as matrix higher chlorinated congeners were practically completely reduced to less than tetra-substituted homologues. A significant part of residual OCDD, when it was spiked in to soils, and formed less chlorinated congeners are extracted with water in the given conditions. The solubility of OCDD was increased by a 4–6 orders over its solubility at ambient conditions. The new method of contentious-flow extraction is described.     

Formation and stability of polychlorinated biphenyl Pickering emulsions

An emulsion stabilized by colloidal suspensions of finely divided solids is known as a Pickering emulsion. The potential for polychlorinated biphenyls (PCBs) to form Pickering emulsions ex situ when in contact with powdered solids, such as clays and metal oxides, is investigated here. Bentonite, iron oxide and magnesium oxide dispersions proved to be robust Pickering emulsion stabilizers, whereas manganese oxide dispersions were not. Batch experiments revealed that emulsions can be formed using a moderately low energy input and can be stabilized with solid concentrations as low as 0.5 wt.%. For the base conditions (volumetric oil fraction (phi(oil))=30 vol.%; solid concentration (chi)=2 wt.%), the formed emulsions were indefinitely stable and the initial average droplet diameters varied from 80 to 258 mum, depending on the solid used in the colloidal dispersion. The average droplet size varied at early time, but for most conditions stabilized to a steady-state value 1 week after preparation. The effect of Ostwald ripening was limited. At greater than 0.5 wt.% concentration, the efficiency of the solid dispersion as a stabilizer was dependant on the volumetric oil fraction but not on the solid concentration. Generally, systems with volumetric oil fractions outside of the 20-70 vol.% range were unstable. The emulsions' droplet stability, average droplet size and size distribution were observed to vary as a function of the amount of energy provided to the system, the volumetric oil fraction, and the concentration of the solid in the aqueous dispersion. It is hypothesized that drilling through fractured rock in the immediate vicinity of dense, non-aqueous phase liquid (DNAPL) PCBs may provide both the energy and solid material necessary to form Pickering emulsions.     

Microbial dechlorination of polychlorinated biphenyls in anaerobic sewage sludge.

The potential of a chlorophenol (CP)-adapted consortium to dechlorinate polychlorinated biphenyls (PCBs) in sewage sludge was investigated. Results show that dechlorination rates differed significantly depending on sludge source and PCB congener. Higher total solid concentrations in sewage sludge and higher concentrations of chlorine in PCB resulted in slower dechlorination rates. No significant difference was found for 2,3,4,5-CB dechlorination from pH 6.0 to pH 8.0; however, dechlorination did not occur at pH 9.0 during a 41-day incubation period. Results show that at concentrations of 1 to 10 mg/L, the higher the PCB concentration, the faster the dechlorination rate. In addition, dechlorination rates were in the following order: methanogenic conditions > sulfate-reducing conditions > denitrifying conditions. The addition of acetate, lactate, pyruvate, and ferric chloride decreased lag times and enhanced dechlorination; however, the addition of manganese dioxide had an inhibitory effect. Dechlorination rates were also enhanced by the addition of PCB congeners, including 2,3,4-CB, 2,3,4,5-CB and 2,3,4,5,6-CB in mixture. Overall results show that the CP-adapted consortium has the potential to enhance PCB dechlorination. The optimal dechlorination conditions presented in this paper may be used as a reference for feasibility studies of PCB removal from sludge.     

Modeling polychlorinated biphenyl sorption isotherms for soot and coal

Sorption isotherms (pg-ng/L) were measured for 11 polychlorinated biphenyls (PCBs) of varying molecular planarity from aqueous solution to two carbonaceous geosorbents, anthracite coal and traffic soot. All isotherms were reasonably log-log-linear, but smooth for traffic soot and staircase-shaped for coal, to which sorption was stronger and more nonlinear. The isotherms were modeled using seven sorption models, including Freundlich, (dual) Langmuir, and Polanyi-Dubinin-Manes (PDM). PDM provided the best combination of reliability and mechanistically-interpretable parameters. The PDM normalizing factor Z appeared to correlate negatively with sorbate molecular volume, dependent on the degree of molecular planarity. The modeling results supported the hypothesis that maximum adsorption capacities (Q_max) correlate positively with the sorbent’s specific surface area. Q_max did not decrease with increasing sorbate molecular size, and adsorption affinities clearly differed between the sorbents. Sorption was consistently stronger but not less linear for planar than for nonplanar PCBs, suggesting surface rather than pore sorption.     

Phenanthrene partitioning in sediment–surfactant–fresh/saline water systems

The objective of this study was to investigate the influence of salinity on the effectiveness of surfactants in the remediation of sediments contaminated with phenanthrene (PHE). This is an example of a more general application of surfactants in removing hydrophobic organic compounds (HOCs) from contaminated soil/sediment in saline environments via in-situ enhanced sorption or ex-situ soil washing. Salinity effects on surfactant micelle formation and PHE partitioning into solution surfactant micelles and sorbed surfactant were investigated. The critical micelle concentration of surfactants decreased, and PHE partition between surfactant micelles and water increased with increasing salinity. Carbon-normalized partition coefficients (K_ss) of PHE onto the sorbed cationic surfactant increased significantly with increasing salinity, which illustrates a more pronounced immobilization of PHE by cationic surfactant in a saline system. Reduction of PHE sorption by anionic surfactant was more pronounced in the saline system, indicating that the anionic surfactant has a higher soil washing effectiveness in saline systems.     

Comparison of bioaugmentation and biostimulation for the enhancement of dense nonaqueous phase liquid source zone bioremediation.

Two 11.7-m(3) experimental controlled release systems (ECRS), packed with sandy model aquifer material and amended with tetrachloroethene (PCE) dense nonaqueous phase liquid (DNAPL) source zone, were operated in parallel with identical flow regimes and electron donor amendments. Hydrogen Releasing Compound (Regenesis Bioremediation Products, Inc., San Clemente, California), and later dissolved lactate, served as electron donors to promote dechlorination. One ECRS was bioaugmented with an anaerobic dechlorinating consortium directly into the source zone, and the other served as a control (biostimulated only) to determine the benefits of bioaugmentation. The presence of halorespiring bacteria in the aquifer matrix before bioaugmentation, shown by nested polymerase chain reaction with phylogenetic primers, suggests that dechlorinating catabolic potential may be somewhat widespread. Results obtained corroborate that source zone reductive dechlorination of PCE is possible at near field scale and that a system bioaugmented with a competent halorespiring consortium can enhance DNAPL dissolution and dechlorination processes at significantly greater rates than in a system that is biostimulated only.     

Mixture effects of 2,3,7,8-tetrachlorodibenzo-p-dioxin and polychlorinated biphenyl congeners in rats

Concern of the toxic effects and bioaccumulation of 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD) and polychlorinated biphenyls in the environment continues to be a focus of research in persistent organochlorine contaminants. Groups of five adult female S.D. rats were administered by gavage 0, 2.5, 25, 250 or 1000 ng TCDD/kg body weight/day or TCDD in combination with a mixture of PCB congeners (PCBs) at 2 or 20 microg/kg b.w./day for a period of 28 days. Growth suppression, increased absolute and relative liver weights, and decreased thymic weight were observed in either the 1000 ng TCDD group alone, or the groups receiving a mixture of 1000 ng TCDD + 2 microg PCBs. The TCDD induced increases in liver and thymic weights were not altered by co-administration with PCBs, however, growth suppression appeared to be more pronounced in the group receiving 1000 ng TCDD + 2 microg PCBs than with TCDD alone. Treatment with TCDD at 250 ng and 1000 ng/kg resulted in a significant increase in hepatic microsomal methoxy resorufin-O-demethylase and ethoxy resorufin-O-deethylase activities which were antagonized by co-administration with PCBs. Similarly, effects of 250 ng TCDD on serum cholesterol and liver UDP glucuronosyl transferase activity and ascorbic acid were significantly reduced by co-administration with 20 microg PCBs. Other biochemical effects elicited by treatment with 1000 ng TCDD, but not affected by co-administration with PCBs include the following: increased serum albumin, decreased liver vitamin A, and increased kidney vitamin A and liver microsomal glutathione-S-transferase activity. While decreased hemoglobin, platelet, packed cell volume and red cell indices were observed in TCDD treated rats, no interactive effects were seen. The above results indicate that the mixture effects of PCBs and TCDD may be additive or antagonistic depending on the dose level and endpoints measured. For the purpose of predicting mixture effects, knowledge of mechanisms of action and toxicokinetics is required.     

Atmospheric polychlorinated biphenyl concentrations and apparent degradation in coastal New Jersey

To characterize the atmospheric dynamics and behavior of organic compounds in the NY–NJ Harbor Estuary, atmospheric concentrations of polychlorinated biphenyls (PCBs) were measured at coastal, suburban and urban sites in New Jersey in 1997–1999. ∑PCB concentrations at the suburban site varied from 86 to 2300 pg m⁻³ and from 84 to 1100 pg m⁻³ at the coastal site. Although the temporal trends of total concentrations were significantly different at the three sites (p<0.01), PCB congener profiles revealed similar patterns (r²>0.90, p<0.001) implicating a dominant emission type and/or process. Temperature explained >50% of the total variability in ln[PCB] at both sites. Atmospheric concentrations at the suburban site increased when winds blew from an eastnortheast vector, while increased wind speeds led to a slight dilution. Wind speed and direction were not significantly correlated with the concentrations measured at the coastal site. Temporal changes in congener distribution at the suburban site are consistent with the preferential atmospheric removal of 3–5 Cl-biphenyls by hydroxyl radical attack with estimated half-lives of 0.7–1.8 years.     

Accumulation and tissue distribution of selected polychlorinated biphenyl congeners in chickens

During one to three consecutive periods of 2 weeks, broiler chickens (n = 108) received test dies to which different amount of PCBs (7 congeners) were added. The relationship between exposure time and accumulation of individual congeners in different chicken tissues, such as breast, thigh and abdominal fat tissue, was observed. In all tissues, the vast majority of the PCB accumulation occurred during the first 2 weeks of exposures. After that, PCB concentrations only increased in the abdominal fat tissue of the animals. The individual PCBs were distributed differently in the various tissues. While CBs 28, 118, 138, 153 and 180 accumulated in the chickens, CBs 52 and 101 were metabolized, but no methyl sulphone metabolites of these congeners could be detected. Our results provide information on the absorption, tissue distribution and biotransformation of the individual PCB congeners and confirm the structure-activity relationships for metabolism of PCBs in birds, which are different from those in fish or mammalian species.     

Selected organochlorine pesticide and polychlorinated biphenyl residues in house dust in Singapore

Although the use of organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) has been prohibited in Singapore since 1980, OCPs and PCBs still can be detected in the environment and represent a potential threat to public health. In this study, OCPs and PCBs were measured in house dust samples collected from 31 homes across the island-state of Singapore. Organochlorine pesticides, such as hexachlorocyclohexanes (HCHs), chlordanes and dichlorodiphenyltrichloroethanes (DDTs) were tested, with a range of 相似文献   

Serum polychlorinated biphenyl and organochlorine insecticide concentrations in a Faroese birth cohort

A prospective birth cohort of 1022 participants was established in the Faroe Islands over a 21-month period during 1986-1987. We collected questionnaire data on potential persistent organic pollutant (POP) concentration predictors, such as duration of breastfeeding and blubber consumption. To assess the participants' exposure from in utero to 14 years of age to polychlorinated biphenyls (PCBs) and the insecticide p,p'-DDT and its primary degradate p,p'-DDE, we measured 37 PCB congeners and pesticides in 316 umbilical cord samples taken from participants at birth, in 124 serum samples collected from participants at approximately 7 years of age, and in 795 serum samples collected from participants at 14 years of age. Measurements of higher chlorination PCB congeners made on individuals' serum samples collected at 7 years and 14 years were highly correlated (typically r > 0.5, p > 0.01), although their concentrations at 7 years were generally two to three times higher than at 14 years. Similarly, umbilical cord PCB concentrations were correlated with PCB concentrations in both 7- and 14-year serum samples. Sex-specific differences in higher chlorination PCB and p,p'-DDE concentrations were found at 14 years but not at 7 years, although a sex interaction with blubber consumption and nursing duration was observed at both ages. Both duration of breastfeeding and consumption of blubber were significant predictors of serum summationPCB concentrations at 7 and 14 years. Multivariate analyses showed that breastfeeding duration was the primary contributor to serum summationPCB concentrations at 7 years, and blubber consumption was the primary contributor at 14 years. These data suggest that infant exposures from breastfeeding were sufficiently large so that continued exposures to PCBs, p,p'-DDT, and p,p'-DDE through the diet have not fully diluted their contribution to the summationPCB and p,p'-DDE body burden of the children.