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PubMed2002

Disinfection by-products in Finnish drinking waters.

Disinfection by-products (DBPs) were measured in plant effluents of 35 Finnish waterworks, which utilized different treatment processes and raw water sources. DBPs were measured also from the distribution systems of three waterworks. Di- and trichloroacetic acids, and chloroform were the major DBPs found in treated water samples. The concentration of six haloacetic acids (HAA6) exceeded the concentrations of trihalomethanes (THMs). Chlorinated drinking waters (DWs) originating from surface waters contained the highest concentration of HAA6 and THMs: 108 and 26 microg/l, respectively. The lowest concentrations of DBPs were measured from ozonated and/or activated carbon filtrated and chloraminated DWs. Higher concentrations of HAA6, THMs, and adsorbable organic halogens were measured in summer compared to winter. The levels of chlorinated acetic acids, chloroform, and bromodichloromethane correlated positively with mutagenicity. Past mutagenicity levels of DWs were examined. A major reduction in the use of prechlorination, increased use of chloramine disinfection, and better removal of organic carbon were the most important reasons for the 69% decrease in mutagenicity from 1985 to 1994.

Chlorine Compounds↗
PubMed2002

Reductive dechlorination of chlorinated methanes in cement slurries containing Fe(II).

Degradative solidification/stabilization (DS/S) is a novel remediation technology that combines chemical degradation with conventional solidification/stabilization. The applicability of the Fe(II)-based DS/S to treating chlorinated alkanes was tested by characterizing degradation reactions of carbon tetrachloride (CT) and its daughter products in cement slurries containing Fe(II). Degradation kinetics of CT and chloroform (CF) were generally very rapid with reaction rates comparable to rates that can be obtained with zero-valent iron. Dechlorination reactions of CT proceeded primarily via a hydrogenolysis pathway, which yielded CF and methylene chloride (MC) as major products and chloromethane and methane as minor products. However, reaction pathways other than hydrogenolysis also appeared to be important at very high pH conditions. MC apparently was resistant to dechlorination reactions over a period of about two months. Kinetics of CT and CF transformation were strongly dependent on pH with an optimal value around 13, which was higher than found previously for PCE. When the initial CF concentration varied between 0.01 and 1 mM, and the Fe(II) dose was 104 mM, pseudo-first-order kinetics generally described the degradation reactions of CF. However, there was also some indication of substrate saturation kinetics in these experiments. This suggests that a saturation model would better describe the kinetics in systems with higher concentration of substrates or lower concentration of the reactive surfaces.

Carbon Tetrachloride↗
PubMed2002

Analysis of six relevant toxaphene congeners in biological samples using ion trap MS/MS.

The quantification of six polychlorinated bornanes (CHBs) was studied using ion trap MS/MS. The significance of the selection of parent ions (Ip) and daughter ions (Id) on the detection of these toxaphene congeners was assessed in standard solution and biological samples. Our results indicate that different Ip and Id, selected at either low or high mass-to-charge (m/z) ratios, influence drastically the response factor of the CHBs and the chemical noise observed. For the octachlorinated toxaphene congeners (Parlar-26 (P-26), Parlar-40/41 (P-40/41), Parlar-44 (P-44)), the detection performance of the ion trap MS/MS is similar whether Ip and Id were chosen at low or high m/z ratios. However, the selection of Ip and Id at high m/z ratios clearly enhances the detection of the nonachlorinated toxaphene congeners (Parlar-50 (P-50), Parlar-62 (P-62)). The improved method, which selects Ip and Id at low m/z ratios for P-26, P-40/41 and P-44 and at high m/z ratios for P-50 and P-62, permitted to obtain low detection limits as well as repeatable and accurate results.

Camphanes↗
PubMed2003

Hydrodehalogenation of chlorobenzene on activated carbon and activated carbon supported catalysts.

Chlorinated aromatic compounds in (waste) gases can be removed and/or dehalogenated by passing over a bed of activated carbon (AC) in a hydrogen containing atmosphere. Dehalogenation of the model compound chlorobenzene (PhCl) to HCl is complete at 490 degrees C--rather than the approximately 900 degrees C needed for the mere gas-phase reaction--but part of the benzene moieties is retained on the AC, resulting in its rather rapid deactivation, apparently due to a large decrease in surface area. Therefore, <1 mmol PhCl per gram of 'catalyst' could be processed. At 600 degrees C chlorobenzene yields 100% of both HCl and benzene, but still the AC lost most of its activity in time. Performances are compared of three different commercial ACs. As a HCl-washed AC is just as active, metals are not involved. This acid-washed AC was used as a support for 10 wt% Ni or Fe catalysts. While Fe did not show appreciable activity, results with Ni are promising. The yields of HCl and benzene from PhCl are approximately 100% already at T<400 degrees C, and T(50%) congruent with 260 degrees C, over 200 degrees C lower than with AC alone. There is no appreciable decrease of activity after having injected >20 mmol PhCl per gram of catalyst at partial conversion.

Benzene↗
PubMed2003

Interlaboratory study for the polychlorinated naphthalenes (PCNs): phase 1 results.

An interlaboratory study was initiated to investigate consistency in reported concentrations of polychlorinated naphthalenes (PCNs). Results are reported from the first phase of a study that examined the variability associated with different quantification methodologies, instrumentation and standards. Nine participating labs from seven countries quantified individual homolog groups, summation operator PCN (the sum of 2-8 chlorinated homologs), and selected congeners in two test solutions derived from Halowax 1014. The means of the reported summation operator PCN values were within less than 15% of the known concentrations of the two test solutions and the relative standard deviation among laboratories was 11%. However, the among laboratory variability was in the range 20-40% for individual PCN homologs and individual PCN congeners. These results suggest the need for additional interlaboratory studies and for the development of reference materials for PCN analysis. Future PCN interlaboratory comparison exercises are discussed that will utilize control materials and unknowns consisting of suitable environmental matrices.

Chlorine Compounds↗
PubMed2003

Chlorobenzenes removal from municipal solid waste incineration fly ash by surfactant-assisted column flotation.

The organic contaminants in municipal solid waste incineration (MSWI) fly ash, including chlorinated aromatic compounds and polycyclic aromatic hydrocarbons, have high toxicity and a potential negative impact on the environment. An effective and low energy consumption technique to remove the organic contaminants from MSWI fly ash is required urgently. Organic contaminants, such as chlorobenzenes (CBzs), in MSWI fly ash are known to become enriched in the unburnt carbon (UC) fraction. It is proposed that removal of UC from fly ash will result in the effective removal of most organic micropollutants. In this research, we use a technique of surfactant-assisted column flotation to decontaminate MSWI fly ash by removal of the CBzs-enriched UC from MSWI fly ash. We find that 39.8% of CBzs can be removed from fresh MSWI fly ash with 61.7% UC removal efficiency, whereas only 33.2% of CBzs can be removed from weathered MSWI fly ash with a low UC removal efficiency of 33.7%. By adding a mixture of two kinds of surfactants: sorbitan mono-oleate and polyoxyethylene (20) sorbitan mono-oleate to the weathered fly ash, 47.0% of CBzs were removed at the hydrophile lipophile balance value of 13.5, while the UC removal efficiency increased to 49.0%. The results show that surfactants can enhance CBzs and UC removal efficiencies during the column flotation process. Higher CBzs and UC removal efficiencies can be expected by further optimizing the conditions of surfactant-assisted column flotation.

Air Pollutants↗
PubMed2003

Soot sorption of non-ortho and ortho substituted PCBs.

Field-observations of distribution coefficients well above expectations from bulk organic-matter partitioning for several chlorinated aromatic compound classes have lead to the hypothesis that enhanced affinity to soot may not be limited to polycyclic aromatic hydrocarbons but may extend as a significant process for a wider range of hydrophobic organic compounds. This suggestion was here tested in soot-column sorption experiments with a series of ortho- and non-ortho substituted polychlorinated biphenyls (PCBs), using diesel particulate matter (NIST standard reference material SRM-1650) as model soot sorbent. For congeners of similar hydrophobicity, considerably higher affinities toward the soot sorbent were observed for the non-ortho substituted PCBs. Mono- to tetra-ortho substituted PCBs exhibited log-based soot-water distribution coefficients (K(sc)) from 5.25 to 5.51 l/kg(sc) at solute concentrations corresponding to 1-13 microg/l. In contrast, biphenyl, mono- and dichloro- non-ortho substituted PCBs yielded logK(sc) values between 5.09 and 6.35 l/kg(sc). These results are 20-50, and 75-110 times higher, respectively, than the corresponding K(ow)-predicted K(oc) numbers. This strong interaction with soot, particularly of non-ortho substituted PCBs, may fundamentally affect their environmental distribution and bioavailable exposure.

Adsorption↗
PubMed2003

Profile of persistent chlorinated contaminants, including selected chiral compounds, in wolverine (Gulo gulo) livers from the Canadian Arctic.

Wolverines (Gulo gulo) are circumpolar omnivores that live throughout the alpine and arctic tundra ecosystem. Wolverine livers were collected at Kugluktuk (Coppermine), NU (n=12) in the western Canadian Arctic to report, for the first time, the residue patterns of persistent organochlorine contaminants (OCs) in this species. The enantiomer fractions (EFs) of several chiral OCs, including PCB atropisomers, in wolverines were also determined. Results were compared to OC concentrations and EFs of chiral contaminants in arctic fox (Alopex lagopus) from Ulukhaqtuuq (Holman), NT (n=20); a closely related species that scavenges the marine and terrestrial arctic environment. The rank order of hepatic concentrations for sum ( summation operator ) OC groups in wolverines were polychlorinated biphenyls ( summation operator PCB)>chlordane-related components ( summation operator CHLOR)>DDT-related compounds ( summation operator DDT)>hexachlorocyclohexane isomers ( summation operator HCHs). The most abundant OC analytes detected in wolverine liver were PCB-153, PCB-180, and oxychlordane (OXY). Wolverine age and gender did not influence OC concentrations, which were comparable to lipid-normalized values in arctic fox. The EFs of several chiral OCs (alpha-HCH, cis- and trans-chlordane, OXY, heptachlor exo-epoxide) and PCB atropisomers (PCB-136, 149) were nonracemic in arctic fox and wolverine liver and similar to those previously calculated in arctic fox and polar bears from Iceland and the Canadian Arctic. Results suggest that these species have similar ability to biotransform OCs. As well, contaminant profiles suggest that terrestrial mammals do not represent the major source of OC exposure to wolverines and that wolverines are scavenging more contaminated prey items, such as marine mammals. While summation operator PCB did not exceed the concentrations associated with mammalian reproductive impairment, future research is required to properly evaluate the potential affect of other OCs on the overall health of wolverines.

Animals↗
PubMed2003

Relevance of coplanar PCBs for TEQ emission of fluidized bed incineration and impact of emission control devices.

Five fluidized bed incinerators combusting municipal solid waste were assessed for the impact of coplanar PCBs on total TEQ emission. In 17 stack measurements, the coplanar PCBs contributed on average less than 3% to total TEQ with a maximum contribution of 7.5% to total TEQ in one measurement. Differences in the design of the flue gas cooling section did not show an effect on the impact of coplanar PCBs on total TEQ. The effect of emission control devices on the impact of coplanar PCBs on the total TEQ was studied in more detail at one incinerator. The relative contribution of PCBs to total TEQ increased along the flue gas line. This was caused by a slightly higher removal efficiency for TEQ relevant PCDDs/PCDFs compared to coplanar PCBs by the bag filters and a higher destruction efficiency for PCDDs/PCDFs compared to PCBs by the SCR catalyst. Additionally, the removal efficiencies of the emission control devices (bag filters and catalyst) for other chlorinated aromatic compounds which have been proposed as TEQ indicator compounds (polychlorinated benzenes and polychlorinated phenols) were compared with those for PCDDs/PCDFs and coplanar PCBs. Removal efficiencies for polychlorinated benzenes or polychlorinated phenols considerably differed from those of PCDD/PCDF and coplanar PCBs. Implications for TEQ assessments using indicator compounds as proposed in the literature are discussed.

Air Pollution↗
PubMed2004

De novo formation characteristics of dioxins in the dry zone of an iron ore sintering bed.

The objectives of this work are to understand the details of the mechanism of dioxin formation in the part of a sintering bed termed the dry zone, and to obtain ideas on how to prevent their formation. Sinter mixtures of various composition types were heated in a packed bed reactor, and dioxins in the outlet gas and in the sinter mixture residue were measured. The dioxin formation potential of a simple sinter mixture composed of iron ore, coke and limestone was markedly lower than that of fly ash from a municipal solid waste incinerator (MSWI). In consideration of this result, a series of experiments were conducted using a sinter mixture impregnated with CuCl2. Experimental results showed that dioxin formation was temperature-dependent in the range of 300-550 degrees C, with the maximum observed at around 300 degrees C, which was quite similar to that of fly ash from the MSWI. The homologue distribution of PCDD/Fs in gas and solid reflected the possible difference in carbonaceous materials in coke and activated coke. Gaseous hydrogen chloride acted as a chlorinating reagent for dioxin formation.

Chlorine Compounds↗
PubMed1999

Advanced oxidation of a pulp mill bleaching wastewater.

The degradation, by several advanced oxidation reactions, of a pulp mill ECF bleaching effluent, was studied. The initial biodegradability of the organic matter present in the effluent, estimated as the BOD5/COD, was low (0.3). When the effluent was submitted to ozonation and to five different advanced oxidation systems (O3/UV, O3/UV/ZnO, O3/UV/TiO2, O2/UV/ZnO, O2/UV/TiO2), the biodegradability increase significantly. After five minutes of reaction, the O3/UV system appears as the most efficient in to transform the organic matter to more biodegradable forms. A similar effect was observed when the effluent was submitted to an activated sludge treatment. The COD, TOC and toxicity reduction correlated well with the biodegradability enhancement after AOPs treatments.

Biodegradation, Environmental↗
PubMedDate not supplied

Search for chlorobornanes in river sediments and in influents and effluents.

In 1997, we collected nine river sediment samples, including one duplicate, from above and below three pulp and paper mills on the Wisconsin River in Wisconsin, USA, and one mill on Beaver Dam Creek in Ontario, Canada. We also obtained twenty split sediment samples from the Wisconsin River that were collected by the US EPA in collaboration with Indiana University. Finally, we collected influent and effluent samples from eight pulp and paper related industries in the US and Canada. We analyzed all sediment and water samples for hexa- through decachlorobornanes. We did not detect any chlorobornanes in most of the sediments. When chlorobornanes were detected, the concentration in sediments below pulp mills were similar to or less than in those from above the same mills. Chlorobornanes could not be detected in any of the influent or effluent samples. Thus, pulp and paper mills and relate facilities are not a source of chlorobornanes.

Camphanes↗
PubMed2000

Chloroperoxidase-mediated chlorination of aromatic groups in fulvic acid.

The aim of the present study is to investigate whether exo-enzymatically mediated chlorination of fulvic acid (FA) results in the formation of chlorinated groups within the macromolecules which correspond to those which were previously detected in soil and surface water samples. The chlorination was carried out by exposing FA to a commercial chloroperoxidase (CPO) in the presence of chloride and hydrogen peroxide. The exposed FA was then chemically degraded using an oxidative technique and finally analysed for four different aromatic groups and their chlorinated analogues. The particular aromatic groups included were the methyl esters of 4-ethoxybenzoic acid, 3-methoxy-4-ethoxybenzoic acid, 3,4-diethoxybenzoic acid, and 3,5-dimethoxy-4-ethoxybenzoic acid, along with their mono- and dichlorinated analogues. Prior to the chemical degradation procedure, the FA was analysed for AOX (adsorbable organic halogens) and chlorinated acetic acids. The original FA contained 1.4 mg Cl(org) g(-1) and detectable amounts of two chlorinated aromatic groups. After exposure to the enzyme, the concentration of AOX increased to 44.3 mg Cl(org) g(-1) and detectable amounts of four chlorinated aromatic groups as well as di- and trichloroacetic acid were found.

Acetates↗
PubMed2000

Thermal remediation of PCDD/Fs contaminated soil by zone combustion process.

A new thermal process has been proposed for remediating soils contaminated by chlorinated organic compounds, e.g., PCDD/Fs and PCBs. This is to apply the "zone combustion process" which utilizes stable combustion of coke particles in the packed bed to soils with air flow across the bed. The usefulness and validity were obtained the results showing that more than 98.9% of PCDD/Fs in the soil was successfully removed in a laboratory-scale experiment. Some pretreatment of the soil sample, such as drying, pre-granulation and addition of limestone was found to make the removal efficiency better. Although, some fundamentals on the behavior of PCDD/Fs, e.g., decomposition/vaporization ratios and formation of other compounds cannot be certainly identified yet, the present results clearly show a way to remediate the contaminated soils and solid wastes.

Benzofurans↗
PubMed2000

Photocatalytic oxidation of gaseous chlorinated organics over titanium dioxide.

The photocatalytic oxidation of high levels of volatile chlorinated organic compounds in gas phase has been studied using a specially designed photoreactor. The influence of light intensity, initial water vapour concentration, temperature, inlet contaminant concentration and flow rate on destruction efficiency has been investigated. The performance of the titanium catalyst was strongly affected by the presence of water in the air stream. Experiments have been most successfully conducted at room temperature, low initial contaminant concentrations, low flow rates and high light intensities. Several by-products have been detected performing photocatalytic degradation of trichloroethylene (TCE) and tetrachloroethylene (PCE). No catalyst deactivation was observed.

Catalysis↗
PubMed1981

Advantages and disadvantages of chemical oxidation and disinfection by ozone and chlorine dioxide.

Ozone and chlorine dioxide present definite advantages and disadvantages over chlorination. Chlorination, particularly for the removal of ammonia and the maintenance of a disinfectant residual in the distribution system has decisive advantages and will be difficult to replace. Ozone and chlorine dioxide seem to produce fewer carcinogenic by-products but the risk for acute toxicity, especially from the chlorites which follow chlorine dioxide, is higher than with chlorine. Chlorine dioxide and more particularly ozone should be considered as useful complements to chlorination, but no strong oxidative treatment should be applied before most of the organic matter has been removed.

Bacteria↗
PubMed1997

A review of dioxin releases to land and water in the UK.

UK government policy is to identify and control the sources of some chlorinated organic compounds including polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs), often known collectively as dioxins. This requires the gathering of information on the scale of releases of PCDD/PCDFs to all environmental media. While a number of recent studies have produced inventories of PCDD/PCDF emissions to air, this study, commissioned by Her Majesty's Inspectorate of Pollution (HMIP--now part of the Environment Agency), is the first attempt at producing a comprehensive UK inventory of emissions of dioxins to land and water from industrial and non-industrial processes. Release of PCDD/PCDFs in wastes taken to landfill are included under the definitions or releases to land used by the Environment Agency. Assembly of the inventory, particularly for releases to water, was severely hampered by lack of data from the UK or overseas; further work is required to remedy the data gaps and deficiencies revealed. The inventory puts total quantified releases to land at 1500-12,000 g toxic equivalent quantities (TEQ) per year--significantly more than releases to air or water. This is as expected, given the nature of the processes that form PCDD/PCDFs and their propensity to bind tightly to solid materials. The bulk of releases to land are to landfills rather than the open environment. From the data available, the open use of chemicals (including the disposal of wood treated with PCP), the manufacture of pesticides, the incineration of municipal solid waste (MSW) and accidental fires appear to be the largest contributors. The processes with greatest potential for releases to water appear to be the open use of chemicals, sewage treatment, disposal of waste oil, accidental fires, production of pesticides and chlorophenols and chemical waste incineration. In addition, the run-off from roads may be a significant source of releases as this is untreated. For the majority of processes studied, the trend is towards reduced releases to land and water, but improvements in the control of releases to air may lead to increased quantities of PCDD/PCDFs in some wastes and thus to increased releases to land. One exception may be from increasing quantities of sewage sludge disposed of to farm land. Changes in waste disposal practice--for example, use of wastes for soil improvement--may also inadvertently increase the probability of human exposure to PCDD/PCDF releases to land. The study did not attempt to assess the risks to humans and ecosystems from releases of PCDD/PCDFs to land and water: it recommends the development of an appropriate risk-assessment methodology.

Benzofurans↗