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PubMed2002

Extraction solvent selection in environmental analysis.

A method for the prediction of a suitable solvent for the extraction of pesticides is outlined. The procedure is based on the Hildebrand solubility parameter, delta(t). The solubility parameter is broken down into three individual components, which are calculated by the addition of group contributions. To demonstrate the applicability of the approach pressurized fluid extraction was used to extract 4,4'-DDT [1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane] and its metabolites, 4,4'-DDD [1,1-dichloro-2,2-bis(p-chlorophenyl)ethane] and 4,4'-DDE [1,1-dichloro-2,2-bis(p-chlorophenyl)ethylene], from an historically contaminated soil from the United States and pentachlorophenol from a certified reference material (CRM524) using various solvents. Visual representation of the individual parameters predicted the ideal extraction solvent to be DCM for 4,4'-DDT and its metabolites and a mixture of acetonitrile and dichloromethane (1:1, v/v) for PCP. These findings were confirmed by the experimental results.

Environmental Pollutants↗
PubMed2004

Two trace analytical methods for determination of hydroxylated PCBs and other halogenated phenolic compounds in eggs from Norwegian birds of prey.

Two new trace analytical methods are presented for identification and quantification of phenolic compounds in complex biological matrixes such as bird of prey eggs. One method is based on derivatization with methyl chloroformate prior to GC/high-resolution MS (HRMS) analysis in electron impact ionization mode. Alternatively, the underivatized phenolic analytes were separated and detected by HPLC coupled to time-of-flight MS (TOF-MS) in the negative ion electrospray ionization mode. For both methods, the egg samples were homogenized and dried with acidified sodium sulfate, cold column-extracted, and cleaned up by gel permeation chromatography and subsequently a Florisil column. Recovery rates for pentachlorophenol (PCP), tetrabromobisphenol A (TBBPA), and selected hydroxylated PCBs (HO-PCBs) from spiked hen's eggs (spiking level 1 ng/g of wet weight (ww)) were in the range of 56-98% for the HPLC/MS method and 57-108% for GC/MS including derivatization. Typical detection limits of the HPLC/TOF-MS method were 5 pg/g ww (1-2 pg injected) for HO-PCBs and PCP and 20 pg/g ww (3 pg injected) for TBBPA. The GC/HRMS method achieved detection limits of approximately 1 pg/g ww in predatory bird eggs for all analytes (0.2 pg injected for derivatized TBBPA and 0.05 pg injected for derivatized HO-PCBs and PCP). Eight eggs from four different Norwegian predatory bird species were analyzed. The concentrations determined with the two different quantification methods corresponded well with each other. PCP and TBBPA were found in all samples at concentrations up to 1350 and 13 pg/g ww, respectively (GC/HRMS values). A total of 55 penta- to nonachloro-HO-PCB congeners were detected in the eight eggs, 10 of those could be structurally identified. The maximum HO-PCB congener concentration was found for 4-HO-CB 187 in a peregrine falcon egg with estimated 388 pg/g ww. Another peregrine falcon egg was highest contaminated with sum HO-PCBs (estimated 2.1 ng/g ww). This level was 1.2 per thousand of the sum PCBs value for the same egg. Furthermore, indications were found that the HO-PCB congener distribution pattern could be species specific for predatory birds.

Journal Article↗
PubMed2005

Chlorinated phenol analysis using off-line solid-phase extraction and capillary electrophoresis coupled with amperometric detection and a boron-doped diamond microelectrode.

The analysis of chlorinated phenols (2-chlorophenol, 3-chlorophenol, 4-chlorophenol, 2,4-dichlorophenol, 2,4,6-trichlorophenol, pentachlorophenol) in river water was accomplished using off-line solid-phase extraction (SPE) and capillary electrophoresis coupled with electrochemical detection. A key to the sensitive, reproducible, and stable detection of these pollutants was the use of a boron-doped diamond microelectrode in the amperometric detection mode. An off-line SPE procedure was utilized to extract and preconcentrate the pollutants prior to separation and detection, with ENVI-Chrom P, a highly cross-linked styrene-divinylbenzene copolymer, being employed as the sorbent. Pollutant recoveries in the 95-100% range with relative standard deviations of 1-4% were achieved. The diamond microelectrode provided a low and stable background current with low peak-to-peak noise. The oxidative detection of the pollutants was accomplished at +1.05 V vs Ag/AgCl without the need for electrode pretreatment. The method was evaluated in terms of the linear dynamic range, sensitivity, limit of quantitation, response precision, and response stability. A reproducible electrode response was observed during multiple injections of the chlorinated phenol solutions with a relative standard deviation of < or =5.4%. Good electrode response stability was observed over many days of continuous use with no significant electrode deactivation or fouling. The separation efficiencies for all six pollutants were greater than 170,000 plates/m. The minimum concentration detectable for all six ranged from 0.02 to 0.2 ppb (S/N > or = 3) using a 250:1 preconcentration factor.

Boron↗
PubMed2005

Light-assisted synthesis of Pt-Zn porphyrin nanocomposites and their use for electrochemical detection of organohalides.

Pt-Zn porphyrin nanocomposites have been synthesized using zinc porphyrin and dihydrogen hexachloroplatinate in the presence of light and ascorbic acid. TEM and AFM imaging revealed that Pt nanoparticles with an average diameter of approximately 3.5 nm were embedded within the Zn porphyrin matrix. The glassy carbon electrode was modified with Nafion-stabilized Pt-Zn porphyrin nanocomposites and used for dehalogenation of carbon tetrachloride, chloroform, pentachlorophenol, chlorobenzene, and hexachlorobenzene as five test models. The Pt-Zn porphyrin nanocomposite-modified electrode exhibited catalytic activity for the reduction of organohalides at -1.0 V versus Ag/AgCl. Raman signatures confirmed the dehalogenation of chlorobenzene by the nanocomposite-modified electrode. The above two aliphatic and three aromatic organohalides had detection limits of 0.5 microM with linearity up to 8 microM. The modified electrode was good for at least 80 repeated measurements of 4 microM chlorobenzene with a storage stability of 1 month at room temperature. The deactivation of the electrode activity was associated with the loss of platinum nanoparticles from the nanocomposite structure.

Electrochemistry↗
PubMed1986

Cytochrome P-450 mediated reductive dehalogenation of the perhalogenated aromatic compound hexachlorobenzene.

Hexachlorobenzene (HCB) elicits concentration-dependent and saturable type 1 binding spectra when added to oxidized (Fe3+) cytochrome P-450 (CYT P-450) in control, phenobarbital- (PB) induced, and beta-naphthoflavone- (BNF) induced male Sprague-Dawley rat liver microsomes. The spectral binding constants (Ks) for HCB in control and PB-induced microsomes are 180 microM and 83 microM, respectively, and correlate inversely with the specific content of CYT P-450 (0.9 and 2.1 nmol/mg) in the two microsomal preparations. BNF-induced microsomes show type 1 interaction only at low HCB concentration. Overall biotransformation of HCB, monitored by loss of [14C]HCB from the reaction medium, is dependent on NADPH and intact microsomes. Dimethyl sulfoxide (Me2SO), a potent hydroxyl radical scavenger and the solvent used for HCB dissolution, does not affect the biotransformation of HCB in aerobic reactions. Pentachlorobenzene (PCB) appears to be the initial and major isolatable CYT P-450 mediated dechlorination product of HCB with NADPH-fortified rat liver microsomes. Trace levels of pentachlorophenol (PCP) and an unidentified metabolite are also observed. PCB formation is enhanced under anaerobic conditions but is inhibited by metyrapone and carbon monoxide. PCB formation is also inhibited with aerobic reaction conditions, while PCP formation is observed. The data indicate that CYT P-450 in hepatic microsomes supports the reductive dechlorination of HCB to PCB.

Animals↗
PubMed2002

The reaction catalyzed by tetrachlorohydroquinone dehalogenase does not involve nucleophilic aromatic substitution.

Tetrachlorohydroquinone dehalogenase catalyzes the reductive dehalogenation of tetrachlorohydroquinone and trichlorohydroquinone during the biodegradation of the xenobiotic compound pentachlorophenol by Sphingobium chlorophenolicum. The mechanism of this transformation is of interest because it is unusual and difficult, and because aerobic microorganisms rarely catalyze reductive dehalogenation reactions. Tetrachlorohydroquinone dehalogenase is a member of the glutathione S-transferase superfamily. Many enzymes in this superfamily are capable of catalyzing nucleophilic aromatic substitution reactions. On the basis of this precedent, we have considered a mechanism for tetrachlorohydroquinone dehalogenase that involves a nucleophilic aromatic substitution reaction, either via an S(N)Ar mechanism or an S(RN)1-like mechanism, in the initial part of the reaction. Mechanistic studies were carried out with the wild type enzyme and with the C13S mutant enzyme, which catalyzes only the initial steps in the reaction. Three findings eliminate the possibility of a nucleophilic aromatic substitution reaction. First, the product of such a reaction, 2,3,5-trichloro-6-S-glutathionylhydroquinone, is not a kinetically competent intermediate. Second, the enzyme can carry out the reaction when the substrate is deprotonated at the active site. Nucleophilic aromatic substitution should not be possible when the substrate is negatively charged. Third, substantial normal solvent kinetic isotope effects on k(cat) and k(cat)/K(M,TriCHQ) are observed. Nonenzymatic and enzymatic nucleophilic S(N)Ar reactions typically show inverse solvent kinetic isotope effects.

Catalysis↗
PubMed2002

Characterization of the initial steps in the reductive dehalogenation catalyzed by tetrachlorohydroquinone dehalogenase.

Tetrachlorohydroquinone dehalogenase catalyzes the reductive dehalogenation of tetrachlorohydroquinone and trichlorohydroquinone during the degradation of pentachlorophenol by Sphingbium chlorophenolicum. Remarkably, the same active site catalyzes the glutathione-dependent isomerization of a double bond in maleylacetone (an analogue of maleylacetoacetate and maleylpyruvate) [Anandarajah, K. et al. (2000) Biochemistry 39, 5303-5311]. The mechanism of the initial steps in the reaction has been probed using the C13S mutant enzyme, which catalyzes the reaction only to the point at which Cys13 is required. The reaction proceeds by a rapid equilibrium random sequential kinetic mechanism. Substrate analogues that lack a second hydroxyl group cannot be turned over to products, although they can bind to the active site. The rate of the reaction is strongly influenced by the number of electron-withdrawing substituents on the substrate. These findings are consistent with a mechanism that begins with ketonization of the deprotonated substrate to form 2,3,5,6-tetrachloro-4-hydroxycyclohexa-2,4-dienone, followed by 1,4-elimination of HCl to from trichlorobenzoquinone. Subsequently, trichlorobenzoquinone is attacked by glutathione to form a glutathione conjugate that, in the absence of Cys13, decomposes to a mixture of products, either at the active site or after release into solution. Possible similarities between this mechanism and the mechanism for isomerization of maleylacetoacetate and maleylpyruvate are discussed.

Acetoacetates↗
PubMed2005

A mechanistic investigation of the thiol-disulfide exchange step in the reductive dehalogenation catalyzed by tetrachlorohydroquinone dehalogenase.

Tetrachlorohydroquinone dehalogenase catalyzes the reductive dehalogenation of tetrachloro- and trichlorohydroquinone to give 2,6-dichlorohydroquinone in the pathway for degradation of pentachlorophenol by Sphingobium chlorophenolicum. Previous work has suggested that this enzyme may have originated from a glutathione-dependent double bond isomerase such as maleylacetoacetate isomerase or maleylpyruvate isomerase. While some of the elementary steps in these two reactions may be similar, the final step in the dehalogenation reaction, a thiol-disulfide exchange reaction that removes glutathione covalently bound to Cys13, certainly has no counterpart in the isomerization reaction. The thiol-disulfide exchange reaction does not appear to have been evolutionarily optimized. There is little specificity for the thiol; many thiols react at high rates. TCHQ dehalogenase binds the glutathione involved in the thiol-disulfide exchange reaction very poorly and does not alter its pK(a) in order to improve its nucleophilicity. Remarkably, single-turnover kinetic studies show that the enzyme catalyzes this step by approximately 10000-fold. This high reactivity requires an as yet unidentified protonated group in the active site.

Amino Acid Sequence↗
PubMed1996

Exploration of the relationship between tetrachlorohydroquinone dehalogenase and the glutathione S-transferase superfamily.

Tetrachlorohydroquinone dehalogenase is found in Sphingomonas chlorophenolica, a soil bacterium that degrades pentachlorophenol, a widely used wood preservative. This enzyme converts tetrachlorohydroquinone (TCHQ) to trichlorohydroquinone (TriCHQ) and TriCHQ to dichlorohydroquinone (DCHQ) (Xun et al. (1992) J. Bacteriol. 174, 8003-8007). The reducing equivalents for each step are provided by two molecules of glutathione (Xun et al. (1992) Biochem. Biophys. Res. Commun. 182, 361-366). In addition to the expected TriCHQ and DCHQ products, the enzyme also produces substantial amounts of 2,3,5-trichloro-6-S-glutathionylhydroquinone (GS-TriCHQ) and an unidentified isomer of dichloro-S-glutathionylhydroquinone (GS-DCHQ). Treatment of the purified enzyme with dithiothreitol dramatically decreases the formation of GS-TriCHQ and GS-DCHQ. Furthermore, enzyme in freshly-prepared crude extracts forms only very small amounts of GS-TriCHQ and GS-DCHQ. We conclude that GS-TriCHQ and GS-DCHQ are produced by enzyme that has undergone some type of oxidative damage and are therefore not physiologically relevant products. The fact that the oxidative damage can be repaired by DTT suggests that a cysteine or methionine residue may be involved. We have created the C13S and C156S mutants of the enzyme. The C13S mutant converts TCHQ to GS-TriCHQ and GS-DCHQ, rather than to DCHQ. Thus, Cys13 is required for the reductive dehalogenation of TCHQ. A mechanism for the reaction which involves Cys13 is proposed.

Amino Acid Sequence↗
PubMed2001

Identifying sources and mass balance of dioxin pollution in Lake Shinji Basin, Japan.

On the basis of congener-specific analysis of dioxins in a dated sediment core, the sources and behavior of dioxins in Lake Shinji Basin, Japan, were estimated. The dioxins in the core showed that their deposition in the lake increased rapidly during the 1960s, peaked in the early 1970s, and then decreased gradually. Principal component analysis of the congener-specific data showed that three major sources existed: pentachlorophenol (PCP), chloronitrophen (CNP), and combustion. PCP and CNP are paddy field herbicides used extensively in the basin. The time trends of source contributions were estimated by multiple regression analysis using the source profiles. The results revealed that dioxin emission from PCP and CNP herbicides was high in the 1960s and the early 1970s, respectively. The contributions from PCP, CNP, and combustion in recent surface sediment were about 68, 16, and 16% in terms of total amount of dioxins. From the decreasing trend of dioxin deposition in the lake after extensive herbicide use, the amount of dioxins that accumulated in the agricultural soil in the basin was estimated to have decreased by about 2%/yr or a half-life of about 35 yr, indicating that dioxin runoff from agricultural fields would continue for a long time.

Agriculture↗
PubMed2002

Assessment of chlorinated dibenzo-p-dioxin and dibenzofuran trends in sediment and crab hepatopancreas from pulp mill and harbor sites using multivariate- and index-based approaches.

Mill process changes and source controls instituted in the late 1980s at pulp and paper mills along the British Columbia (BC) coast produced dramatic reductions in both the concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and the TEQ (2,3,7,8-TCDD toxic equivalents). Nevertheless, questions remained as to whether the sediments were acting as contaminant sources or sinks, whether crab uptake pathways have stayed the same since the mills ceased producing PCDD/Fs, and whether improvement was faster at some sites than others. To examine the processes governing the changes in PCDD/F composition, PCDD/F sources and compositional trends for the coastal BC sites were interpreted using sediment and crab PCA (principal components analysis) models and two indices based on the three main groups of PCDD/Fs that covary in all PCA models. One index measured the relative inputs of chlorine bleaching PCDFs and PCP (pentachlorophenol)-related PCDDs at each mill and harbor site whereas the other measured the relative inputs of PCP wood preservatives and pulp mill effluents. Results indicated that PCDFs produced during chlorine bleaching accumulate from sediments to crabs more readily than the PCDDs but that the chlorine bleaching TCDFs have generally decreased in importance at all mill sites. In the years just before 1995, little change was observed in either the proportion of toxic 2,3,7,8-chlorinated congeners or the PCDD/F concentrations, and the improvements seemed to have largely ceased by 1995. The lack of change in PCA composition for the harbors provided a further, disturbing indication that ecosystem recovery may have stalled. Results also implied that the main route of PCDD/Fs into crabs shifted from uptake via a pelagic food web incorporating effluent-borne PCDD/Fs associated with suspended particulate matter to uptake via a benthic food web.

Animals↗
PubMed2003

Formation of PCDDs, PCDFs, and coplanar PCBs from incineration of various woods in the presence of chlorides.

Exhaust gases from the combustion of woods (Japanese red pine, Japanese cedar, Siebold's beech, seawater-impregnated Japanese red pine and Japanese cedar, waste woods containing chlordane, and waste woods containing pentachlorophenol) were collected at the outlet of a combustion chamber. A small-scale incinerator with a stationary grate was used. The samples were analyzed for PCDDs, PCDFs, and coplanar PCBs by gas chromatography/ mass spectrometry (GC/MS). When the grate temperature of the combustion chamber was lower than 700 degrees C, the total amount of PCDDs, PCDFs, and coplanar PCBs formed was proportional to the chlorine content of the combustion samples. On the other hand, when the grate temperature of the combustion chamber was higher than 800 degrees C, there was only a slight formation of PCDDs, PCDFs, and coplanar PCBs regardless of the chlorine content of the combustion samples. When the grate temperature was low, nearly 90% of total PCDDs, PCDFs, and coplanar PCBs formed were PCDFs, whereas when the grate temperature was higher, 50-80% of total PCDDs, PCDFs, and coplanar PCBs formed was PCDFs. The total amount of PCDDs, PCDFs, and coplanar PCBs formed in a high-temperature condition was approximately 1/50 of that formed in a low-temperature condition. Coplanar PCBs tended to form less than PCDDs or PCDFs did. Mono-ortho-PCBs were formed several times more than nonortho-PCBs. PCDDs or PCDFs contributed significantly to the values of TEQ, while coplanar PCBs contributed only slightly.

Benzofurans↗
PubMed2002

Transformation processes, pathways, and possible sources of distinctive polychlorinated dibenzo-p-dioxin signatures in sink environments.

In recent years, studies on environmental samples with unusual dibenzo-p-dioxin (PCDD) congener profiles were reported from a range of countries. These profiles, characterized by a dominance of octachlorinated dibenzodioxin (OCDD) and relatively low in dibenzofuran (PCDF) concentrations, could not be attributed to known sources or formation processes. In the present study, the processes that result in these unusual profiles were assessed using the concentrations and isomer signatures of PCDDs from dated estuarine sediment cores in Queensland, Australia. Increases in relative concentrations of lower chlorinated PCDDs and a relative decrease of OCDD were correlated with time of sediment deposition. Preferred lateral, anaerobic dechlorination of OCDD represents a likely pathway for these changes. In Queensland sediments, these transformations result in a distinct dominance of isomers fully chlorinated in the 1,4,6,9-positions (1,4-patterns), and similar 1,4-patterns were observed in sediments from elsewhere. Consequently, these environmental samples may not reflect the signatures of the original source, and a reevaluation of source inputs was undertaken. Natural formation of PCDDs, which has previously been suggested, is discussed; however, based on the present results and literature comparisons, we propose an alternative scenario. This scenario hypothesizes that an anthropogenic PCDD precursor input (e.g. pentachlorophenol) results in the contamination. These results and hypothesis imply further investigations are warranted into possible anthropogenic sources in areas where natural PCDD formation has been suggested.

Benzofurans↗
PubMed2003

Plasma-associated halogenated phenolic contaminants in benthic and pelagic fish species from the Detroit River.

Halogenated phenolic contaminants (HPCs), polychlorinated biphenyls (PCBs), and other organochlorine (OC) contaminants (DDTs, chlordanes, HCH, and octachlorostyrene (OCS)) were determined (ng/g, wet wt basis) in the blood plasma of 6 piscivorous/pelagic- and 7 benthic-feeding fish species from the Detroit River. Seven to twelve hydroxylated (OH) PCB congeners with pentachloro- to nonachloro-substitution, pentachlorophenol (PCP) and 4-OH-heptachlorostyrene (4-OH-HpCS), as well as a number of other unidentified HPCs, were detected in all the fish species studied. The concentrations of sigma-OH-PCB (0.57-129.5 ng/ g), 4-OH-HpCS (0.02-0.31 ng/g), and PCP (0.05-3.42 ng/ g) in comparison to other major polychlorinated contaminants (sigma-PCB (10.4-909.0 ng/g), sigma-chlordane (0.72-8.68 ng/g), sigma-DDT (2.10-66.57 ng/g), and sigma-HCH (0.04-0.84 ng/g)) demonstrate the importance of HPCs, especially OH-PCBs, as plasma-associated contaminants. OH-PCBs are most likely metabolites of PCBs, and 4-OH-HpCS is a likely metabolite of OCS. Our findings indicate that metabolic biotransformation is a factor in the bioaccumulation, pharmacokinetics, and fate of OCS and highly chlorinated PCB congeners that are generally more recalcitrant in fish. Target tissue exposure to circulating OH-PCBs was variable, and thus potential OH-PCB-mediated toxicological activity and effects (e.g., endocrine-related) and health risks are different among the fish species.

Animals↗
PubMed2003

Hydroxylated PCBs and other chlorinated phenolic compounds in lake trout (Salvelinus namaycush) blood plasma from the Great Lakes region.

Recently, there has been an increase in studies focusing on an emerging class of organic contaminants, hydroxylated PCBs (OH-PCBs) and chlorinated phenolic compounds (CPCs) in the environment, particularly in northern regions of Europe and Canada. Since information for fish from the Great Lakes are scarce, we determined the blood plasma concentrations of OH-PCB congeners, pentachlorophenol (PCP), 2,3,4,5-tetrachlorophenol (TCP), and 4-hydroxyheptachlorostyrene (4-OH-HpCS) for lake trout (Savelinus namaycush) collected from two of the Great Lakes, Lake Ontario and Lake Superior, and two regional lakes, Lake Champlain and Lake Opeongo. PCP was the dominant CPC in lake trout (105-658 pg/g of plasma). Detectable concentrations of 2,3,4,5-TCP and 4-OH-HpCS were found in all lake trout (2.6-101 and 0.4-27 pg/g, respectively). Highest concentrations were found in trout from Lake Ontario and Lake Superior. Sixteen OH-PCBs were quantified, with 4-OH-CB187 having the highest concentration in all samples (10-173 pg/g of plasma). Unexpectedly, highly chlorinated OH-PCBs such as 4'-OH-CB199 (mean 21.4 and 74.4 pg/g), 4,4'-diOH-CB202 (18.3 and 27.7 pg/g), and 4'-OH-CB208 (24.5 and 34.7 pg/g) were found in lake trout from Lake Ontario and Lake Superior, respectively. Future studies to delineate the sources and impacts of CPCs in the Great Lakes catchment are needed.

Animals↗
PubMed2004

Electro-oxidation and amperometric detection of chlorinated phenols at boron-doped diamond electrodes: a comparison of microcrystalline and nanocrystalline thin films.

We report on the electro-oxidation and amperometric detection of phenol and chlorinated phenols, the latter coupled with flow injection analysis (FIA) and high performance liquid chromatography (HPLC), using boron-doped microcrystalline and nanocrystalline diamond thin-film electrodes. The low background current, good response without extensive pretreatment, and low susceptibility to fouling are properties that make diamond an attractive new electrode for monitoring this class of pollutants. Cyclic voltammetric studies were performed to evaluate the redox response of phenol, 2-chlorophenol, 3-chlorophenol,4-chlorophenol, and pentachlorophenol (PCP) in phosphate buffer, pH 3.5, as a function of the potential scan rate and cycle number. The diamond electrode performance for the amperometric detection of these contaminants in FIA-EC and HPLC-EC was evaluated in terms of the linear dynamic range, limit of quantitation, sensitivity, response precision, and response stability. Both diamond types yielded low mass limits of quantitation of 100-1000 pg for all the phenolic compounds in FIA-EC, except PCP which was 3 ng, and 100-600 pg for all the compounds in HPLC-EC. In all cases, the S/N was 3 or greater. Both electrode types also exhibited good sensitivity, excellent response reproducibility (av 2.7% for FIA-EC and av 4.2% for HPLC-EC), and superb response stability for all the analytes. The electrodes could be used from days to weeks in the measurement with only a periodic soak in distilled 2-propanol required to maintain optimum performance. Both types of diamond outperformed glassy carbon, which exhibited short-lived responsiveness as a consequence of fouling by reaction products and potential-dependent changes in the electrode's physiochemical properties. The use of the HPLC-EC assay for the determination of 2-chlorophenol in a contaminated soil sample is also demonstrated.

Boron↗
PubMed2004

Simulating the influence of snow on the fate of organic compounds.

Snow scavenging, a seasonal snowpack, and a dynamic water balance are incorporated in a non-steady-state generic multimedia fate model in order to investigate the effect of snow on the magnitude and temporal variability of organic contaminant concentrations in various environmental media. Efficient scavenging of large nonpolar organic vapors and particle-bound organic chemicals by snow can lead to reduced wintertime air concentrations and incorporation in the snowpack. The snow cover functions as a temporary storage reservoir that releases contaminants accumulating over the winter during a short melt period, resulting in temporarily elevated concentrations in air, water, and soil. The intensity of these peaks increases with the length of the snow accumulation period. Organic chemicals of sufficient volatility (log KOA < 9; e.g., light polychlorinated biphenyls) can volatilize from the snowpack, resulting in springtime concentration maxima in the atmosphere. The behavior of fairly water-soluble chemicals during snowmelt depends on their relative affinity for the newly formed liquid water phase and the rapidly diminishing ice surface-quantitatively expressed by their interface-water partition coefficient (KIW). Chemicals with a preference for the dissolved phase (low KIW; e.g., pentachlorophenol) can become enriched in the first meltwater fractions and experience a temporary concentration peak in lakes and rivers. Organic chemicals that are neither volatile enough to evaporate from the snowpack nor sufficiently water soluble to dissolve in the meltwater (e.g., polybrominated diphenyl ethers) sorb to the particles in the snowpack. These particles may be sufficiently contaminated to constitute the major input route to the terrestrial environment upon release during snowmelt. Because wintertime deposition to the snowpack may be higher than to a non-snow covered surface, this can result in higher soil concentrations of persistent organic contaminants in the long term. The potential ecotoxicological significance of peak exposures demands a better understanding of the role of snow in the fate of organic contaminants.

Environmental Monitoring↗
PubMed2005

Typical dioxin concentrations in agriculture soils of Washington state and potential sources.

Background or typical levels of polychlorinated dibenzo-p-dioxins and of polychlorinated dibenzo-p-furans in soils have become increasingly important in the regulatory community, as dioxins have come under increased scrutiny due to their toxicity and persistence. Knowing the typical levels of dioxin in soils is important to set regulatory levels, to prevent further contamination, and for setting cleanup levels. A random sample (n=54) of agricultural lands within Washington state revealed a typical concentration of "dioxin" of 0.14 ng/kg (toxicity equivalents, TEQ). For a comparison, residential urban areas, forested, and open areas were also investigated on a smaller scale (n=14, 8, and 8, respectively) with typical dioxin values of 4.1, 2.3, and 1.0 ng/kg (TEQs), respectively. A discriminant function analysis was used to examine soil dioxin profiles and associations with potential known dioxin sources in Washington state. Soil sample dioxin profiles could not be discriminated from those of biosolids and pentachlorophenol products.

Agriculture↗