Introductory remarks to the Special Issue.
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Biological Availability↗
Biomedical subjects
Kevin C Jones
Publications and source records attributed to Kevin C Jones.
Influence of plants on the chemical extractability and biodegradability of 2,4-dichlorophenol in soil.
This study investigated the fate and behaviour of [UL-(14)C] 2,4-dichlorophenol (DCP) in planted (Lolium perenne L.) and unplanted soils over 57 days. Extractability of [UL-(14)C] 2,4-DCP associated activity was measured using calcium chloride (CaCl(2)), acetonitrile-water and dichloromethane (DCM) extractions. Biodegradability of [UL-(14)C] 2,4-DCP associated activity was assessed through measurement of (14)CO(2) production by a degrader inoculum (Burkholderia sp.). Although extractability and mineralisation of [UL-(14)C] 2,4-DCP associated activity decreased significantly in both planted and unplanted soils, plants appeared to enhance the sequestration process. After 57 days, in unplanted soil, 27% of the remaining [UL-(14)C] 2,4-DCP associated activity was mineralised by Burkholderia sp., and 13%, 48%, and 38% of (14)C-activity were extracted by CaCl(2), acetonitrile-water and DCM, respectively. However, after 57 days, in planted soils, only 10% of the [UL-(14)C] 2,4-DCP associated activity was available for mineralisation, whilst extractability was reduced to 2% by CaCl(2), 17% by acetonitrile-water and 11% by DCM. This may be due to the effect of plants on soil moisture conditions, which leads to modification of the soil structure and trapping of the compound. However, the influence of plants on soil biological and chemical properties may also play a role in the ageing process.
Biodegradation, Environmental↗
Formation of non-extractable pesticide residues: observations on compound differences, measurement and regulatory issues.
Six major use pesticides (Atrazine, Dicamba, Isoproturon, Lindane, Paraquat and Trifluralin) with differing physico-chemical properties were evaluated for the significance of 'bound' or non extractable residue formation. Investigations were carried out in purpose-built microcosms where mineralization, volatilisation, 'soil water' extractable and organic solvent extractable residues could be quantified. Extractable residues were defined as those accessible by sequential extraction where the solvent used became increasingly non-polar. Dichloromethane was the 'harshest' solvent used at the end of the sequential extraction procedure. (14)C-labelled volatilised and (14)CO(2) fractions were trapped on exit from the microcosm. The pesticides were categorised into 3 classes based on their behaviour. (i) Type A (Atrazine, Lindane and Trifluralin) in which ring degradation was limited as was the formation of non-extractable residues; the remainder of the (14)C-activity was found in the extractable fraction. (ii) Type B (Dicamba and Isoproturon) in which approximately 25% of the (14)C-activity was mineralised and a large portion was found in the non-extractable fraction after 91 days. Finally, Type C (Paraquat) in which almost all of the (14)C-activity was quickly incorporated into the non-extractable fraction. The implications of the data are discussed, with respect to the variability and significance of regulatory aspects of non-extractable residues.
Atrazine↗
Prediction of polycyclic aromatic hydrocarbon biodegradation in contaminated soils using an aqueous hydroxypropyl-beta-cyclodextrin extraction technique.
This study investigated the use of an aqueous hydroxypropyl-beta-cyclodextrin (HPCD) shake extraction to predict the degree of microbial degradation of polycyclic aromatic hydrocarbons (PAHs) in soils. Three different aged PAH-contaminated soils were studied: A soil from a former coke works (CW) and two artificially contaminated soils (AC1 and AC2). First, the catabolic activity of the indigenous soil microflora was assessed with 14C-respirometry, using a range of 14C-labeled aromatic compounds. Extensive mineralization of several compounds occurred in the CW and the AC2 soils, suggesting that both soils contained catabolically active microorganisms. No significant mineralization occurred in the AC1 soil, implying that either it did not contain an indigenous PAH-degrading microbial population or that degradation, but not mineralization, occurred. The soils then were subjected to three sets of analyses: dichloromethane (DCM) soxhlet extraction, six-week biodegradation assay followed by DCM extraction, and extraction with HPCD followed by DCM extraction. A general decrease in PAHs present in the soils occurred after the biodegradation assay. In the CW and the AC1 soils, strong correlations were observed between the amount of PAHs biodegraded and the fraction of PAHs removed from the soils using the HPCD extraction. However, the AC2 soil showed a more modest correlation between the biodegradable fraction and the HPCD extractable fraction, with the HPCD extraction slightly underestimating the extent of PAH biodegradation. The results of this study indicated that an aqueous HPCD extraction may be a useful tool in assessing the microbial availability of aged contaminant mixtures in soils, although further validation is required.
2-Hydroxypropyl-beta-cyclodextrin↗
Effect of cyclodextrin and transformer oil amendments on the chemical extractability of aged [14C]polychlorinated biphenyl and [14C]polycyclic aromatic hydrocarbon residues in soil.
Sequestration of hydrophobic organic contaminants (HOCs) in soils limits chemical and biological availability. Concerns exist regarding the long-term stability of sequestered contaminants in the environment, and stability needs to be demonstrated if bioavailability considerations are to be adopted into the risk assessment and remediation of contaminated land. The aim of the present study was to test the short-term influence of two organic amendments on the chemical extractability of HOC residues that had been present in soils for more than 12 years. The amendments investigated were cyclodextrin and transformer oil (a light, nonaqueous phase liquid [LNAPL]). The contaminants investigated were fluoranthene and benzo[a]pyrene in one soil and the polychlorinated biphenyls (PCBs) 28 and 52 in a second soil. The addition of cyclodextrin to the soils did not result in a significant increase in chemical extractability of the residues after a 36-d contact time. The addition of transformer oil resulted in an increase in chemical extractability of the PCBs after a 14-d soil-LNAPL contact time and a further increase after a 36-d contact time. The present study demonstrates that the chemical availability of aged HOCs in soil may be influenced by the presence of other chemicals and has implications for the long-term management of contaminated land.
Absorption↗
Atmospheric dry deposition of persistent organic pollutants to the Atlantic and inferences for the global oceans.
Atmospheric deposition to the oceans is a key process affecting the global dynamics and sinks of persistent organic pollutants (POPs). A new methodology that combines aerosol remote sensing measurements with measured POP aerosol-phase concentrations is presented to derive dry particulate depositional fluxes of POPs to the oceans. These fluxes are compared with those due to diffusive air-water exchange. For all polychlorinated biphenyl (PCB) congeners and lower chlorinated dibenzo-p-dioxins and furans (PCDD/Fs), air-water exchange dominates the dry deposition mechanism. However, this tendency reverses in some areas, such as in marine aerosol influenced areas and dust outflow regions, consistent with the important variability encountered for the depositional fluxes. Seasonal variability is mainly found in mid-high latitudes, due to the important influence of wind speed enhancing dry deposition fluxes and temperature as a driver of the gas-particle partitioning of POPs. The average dry aerosol deposition flux of sigmaPCBs and sigmaPCDD/Fs to the Atlantic Ocean is calculated to be in the order of 66 ng m(-2) yr(-1) and 9 ng m(-2)yr(-1) respectively. The total dry aerosol deposition of sigmaPCBs and sigmaPCDD/Fs to the Atlantic Ocean is estimated to be 2200 kg yr(-1) and 500 kg yr(-1), respectively, while the net air-water exchange is higher, 22000 kg sigmaPCBs yr(-1) for PCBs and 1300 kg sigmaPCDD/Fs yr(-1). Furthermore, it is suggested that marine aerosol plays an important role in scavenging atmospheric contaminants.
Aerosols↗
Passive sampling survey of polybrominated diphenyl ether flame retardants in indoor and outdoor air in Ottawa, Canada: implications for sources and exposure.
The polybrominated diphenyl ethers (PBDEs) are widely used as flame retardants in plastics of soft furnishings, TV sets and computers, and insulation in the indoor environment. The penta-BDEs--now banned in most parts of Europe but still used in North America--are additive flame retardants that may be released to the indoor environment via volatilization or as dusts. In this study, to investigate general population PBDE exposure, air was sampled in 74 randomly selected homes in Ottawa, Canada and at seven outdoor sites during the winter of 2002--3, using polyurethane foam (PUF) disk passive air samplers. The passive sampling rate (2.5 m3 day(-1)) was determined through a pilot study employing active and passive samplers side-by-side at selected indoor locations. Indoor air concentrations of PBDEs were log-normally distributed with a geometric mean of 120 pg m(-3) and a median of 100 pg m(-3), approximately 50 times higher than the range of outdoor air concentrations (<0.1-4.4 pg m(-3)). The maximum daily human exposure via the inhalation pathway based on median PBDE levels found in this survey was estimated to be 1.9 ng day(-1) (female) and 2.0 ng day(-1) (male), representing 4.1% (f) and 4.4% (m) of overall daily intake.
Air Pollutants↗
A novel analytical approach for visualizing and tracking organic chemicals in plants.
Vegetation plays a key role in the environmental fate of many organic chemicals, from pesticides applied to plants, to the air-vegetation exchange and global cycling of atmospheric organic contaminants. Our ability to locate such compounds in plants has traditionally relied on inferences being made from destructive chemical extraction techniques or methods with potential artifacts. Here, for the first time, two-photon excitation microscopy (TPEM) is coupled with plant autofluorescence to visualize and track trace levels of an organic contaminant in living plant tissue, without any form of sample modification or manipulation. Anthracene-a polynuclear aromatic hydrocarbon (PAH)-was selected for study in living maize (Zea mays) leaves. Anthracene was tracked over 96 h, where amounts as low as approximately 0.1-10 pg were visible, as it moved through the epicuticular wax and plant cuticle, and was observed reaching the cytoplasm of the epidermal cells. By this stage, anthracene was identifiable in five separate locations within the leaf: (1) as a thin (approximately 5 microm) diffuse layer, in the upper surface of the epicuticular wax; (2) as thick (approximately 28 microm) diffuse bands extending from the epicuticular wax through the cuticle, to the cell walls of the epidermal cells; (3) on the external surface of epidermal cell walls; (4) on the internal surface of epidermal cell walls; and (5) within the cytoplasm of the epidermal cells. This technique provides a powerful nonintrusive tool for visualizing and tracking the movement, storage locations, and degradation of organic chemicals within vegetation using only plant and compound autofluorescence. Many other applications are envisaged for TPEM, in visualizing organic chemicals within different matrixes.
Air Pollutants↗
Potential contamination of shipboard air samples by diffusive emissions of PCBs and other organic pollutants: implications and solutions.
Air samples were taken onboard the RRS Bransfield on an Atlantic cruise from the United Kingdom to Halley, Antarctica, from October to December 1998, with the aim of establishing PCB oceanic background air concentrations and assessing their latitudinal distribution. Great care was taken to minimize pre- and post-collection contamination of the samples, which was validated through stringent QA/QC procedures. However, there is evidence that onboard contamination of the air samples occurred,following insidious, diffusive emissions on the ship. Other data (for PCBs and other persistent organic pollutants (POPs)) and examples of shipboard contamination are presented. The implications of these findings for past and future studies of global POPs distribution are discussed. Recommendations are made to help critically appraise and minimize the problems of insidious/diffusive shipboard contamination.
Air↗
Exchange of polychlorinated biphenyls (PCBs) and polychlorinated naphthalenes (PCNs) between air and a mixed pasture sward.
To improve understanding of air-to-vegetation transfer of persistent organic pollutants (POPs), uptake and depuration of polychlorinated biphenyls (PCBs) and polychlorinated naphthalenes (PCNs) between grass sward and air was investigated. Pasture swards were placed in fanned (2 m s(-1) wind speed) and unfanned conditions for a period of 20 days and sampled at intervals. Depuration was carried out after a short (4 days) and a long (14 days) exposure period. Prior to contamination, a mixed pasture sward at a semi-rural location contained sigmaPCN concentrations 15-20% of the sigmaPCB concentration. Uptake of both PCBs and PCNs was broadly linear in fanned and unfanned conditions over the 20-day period, i.e., the pasture did not reach equilibrium with the air. Uptake rates (fluxes) were greater under the fanned conditions. The difference in uptake rates between fanned and unfanned conditions increased with degree of chlorination for both PCBs and PCNs, ranging between a factor of 2 for tri-chlorinated PCBs and PCNs and a factor 5 for octa-chlorinated PCBs. Depuration results over the first hours were very scattered, showing an initial period of loss, followed by an increase in concentrations, possibly as a result of re-volatilization of PCBs from the soil in the trays, with consequent recapture by the overlying sward. Rapid clearance was observed over the following days, but depuration of PCBs and PCNs was still incomplete after 14 days, with 20% of the initial concentration of the sigmaPCBs and 10% of the sigmaPCNs retained by the sward. There was no difference in the proportion of POPs retained in the sward between the 4- and 14-day contamination treatments. POP-specific differences in the amount of compound "trapped" in leaves after contamination were observed. The results show that, although changes in the rate of air movement around a pasture have an effect on the uptake rate of POPs into the vegetation, plant-side resistance controls both the air-to-pasture and pasture-to-air exchange of gas-phase PCBs and PCNs; i.e., differences between plant species in cuticle composition and/or structure affecting the permeability of the cuticle are of greater importance than differences in leaf morphology affecting aerodynamic roughness.
Air↗
Inter-individual differences in the ability of human milk-fat extracts to enhance the genotoxic potential of the procarcinogen benzo[a]pyrene in MCF-7 breast cells.
Environmental factors are believed to play an important role in cancer aetiology. Whether environmental pollutants act in isolation or in combination within mixtures remains unclear. Four human milk-fat extracts (from resident U.K. women) were screened for levels of organochlorinated and brominated compounds prior to being tested (1-50 mg-equiv) for micronucleus (MN)-forming activity in MCF-7 cells. Using the cytokinesis-block micronucleus assay, micronuclei (MNi) were scored in 1000 binucleate cells per treatment. Cell viability (% plating efficiency) and immunohistochemical detection of p53 induction were also measured. The effects of treatment with 1 mg-equiv of extract in combination with benzo[a]pyrene (BP) were also examined. BP-DNA adducts were detected and quantified by 32P-postlabeling analysis. Dose-related increases in MNi independent of pollutant concentrations were induced by milk-fat extracts. All four extracts elevated the percentage of p53 positive cells, although not always in a dose-related fashion. Some combinations resulted in profound low-dose-induced increases in MNi and significant elevations in the percentage of p53 positive cells, which occurred without further reduction in cell viability or mitotic rate. When one particular extract was combined with BP, a 100-fold increase in BP-DNA adducts was detected as compared with the levels induced by BP alone; an effect not induced by other extracts. This adduct-enhancing extract was fractionated into 14 fractions that were subsequently tested (1 mg-equiv of original extract) in combination with 0.01 microM BP. Fraction 1, into which nonpolar pollutants mostly eluted, enhanced MN-forming activity with BP. Surprisingly, the more polar and less likely to contain fat-soluble pollutants fractions 5 and 8 also enhanced MN-forming activity. No identifiable pollutants were present in these fractions. The results suggest that different environmental pollutants present in human tissue may influence the susceptibility of target cells to initiating events.
Benzo(a)pyrene↗
Analytical challenges hamper perfluoroalkyl research.
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Chemistry Techniques, Analytical↗
Defining bioavailability and bioaccessibility of contaminated soil and sediment is complicated.
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Animals↗
Further studies on the latitudinal and temporal trends of persistent organic pollutants in Norwegian and U.K. background air.
Data are presented for PBDEs, PCBs, and selected organochlorine compounds, measured at background locations by passive air samplers (semipermeable membrane devices, SPMDs) along a latitudinal transect from the south of the U.K. to the north of Norway during 2000-2002. This work is part of an ongoing air sampling campaign in which PCB data were previously obtained in 1994-1996 and 1998-2000. Comparisons of the masses of chemicals sequestered by the SPMDs during these different time intervals are used to investigate spatial and temporal trends. The study yielded examples of compounds that increase, decrease, or remain uniform with latitude, suggestive of differences in the relative importance of deposition versus atmospheric reaction in controlling their long-range atmospheric transport potential. The main constituents of the penta-BDE product were detected at amounts equivalent to 2.0 (range 1.1-2.5) and 1.1 (0.8-1.6) pg m(-3) for the U.K. and Norway background sites, respectively. Fractionation of PBDEs was observed, because the amounts of lighter BDEs decreased with latitude, while the heavier molecular weight congeners were quite uniformly distributed. In contrast, the sequestered amounts of the lighter PCBs were uniformly distributed with latitude, with heavier PCBs decreasing. Sequestered amounts of hexachlorobenzene increased with latitude. Preliminary PCB atmospheric clearance rates were derived using the 1994-1996, 1998-2000, and 2000-2002 data. They averaged ca. 3.5 years for all congeners/locations. No systematic differences in congeners or locations were noted, supporting the hypothesis that the underlying trends in European background air are still controlled by primary, rather than secondary, sources.
Air Pollutants↗
Evidence for dynamic air-water coupling and cycling of persistent organic pollutants over the open Atlantic Ocean.
Ship-board air samples collected between The Netherlands and South Africa in January-February 2001 were analyzed for PCBs and selected organochlorine compounds. Broad latitudinal trends in compound concentrations were influenced by proximity to source areas, land, and air mass origin. Lowest concentrations were observed in the remote south Atlantic (1-32 degrees S), where sigma7PCB concentrations were approximately 10 pg m(-3). Here, a diurnal cycle was noted for some PCB congeners, with the daytime concentrations higher than the nighttime concentrations, typically by a factor of 1.5-2.5. The data are consistent with a close coupling of air-open ocean concentrations, which has important implications for future rates of POP removal from the global "recyclable pool". The observations are discussed in the context of the potential controlling variables. Interactions between the phytoplankton and the dissolved phase are implicated in controlling the observations made here and a hypothesis to explain the cycling trends is presented. However, the precise mechanisms remain unclear; further studies are urgently required to elucidate them.
Air Pollutants↗
Observations on historical, contemporary, and natural PCDD/Fs.
PCDD/Fs were determined in samples of archived surface soils collected from different locations around the world in the early 1880s, in contemporary surface soils from around the world, in archived subsurface soils collected at Rothamsted Experimental Station in the 1870/1880s, and in sections of peat core deposited between 5000 BP and the present. PCDD/Fs were detected in most of the samples. The potential sources and implications of the levels and mixtures of PCDD/Fs present in the samples are discussed. The homologue and isomer patterns observed in most of the contemporary European surface soils are commonly observed for European air samples and soil samples. The homologue pattern in the Rothamsted surface soils collected in the 1800s was similar, suggesting that similar sources of atmospheric emissions of PCDD/ Fs were operating in the UK in the 1800s as currently. Very different patterns, dominated by OCDD and with contributions of HpCDD and HxCDD, were found in some other samples. It is proposed that the PCDD/Fs present in the subsurface Rothamsted soils, archived (1880s) surface soils from Illinois and the Congo, clay beneath the peat bog (deposited approximately 5000 BP), and possibly surface soil samples from Thailand and Australia are of a natural origin. The most abundant TeCDD/F congeners measured in the peat samples here were also those observed by previous workers who studied a Canadian peat bog and are consistent with the microbially mediated oxidative coupling of chlorophenols. The study provides evidence for the widespread occurrence of PCDD/Fs in the environment prior to 1900 and for a complex array of sources (including natural) and environmental transformation processes.
Benzofurans↗
PBDEs in European background soils: levels and factors controlling their distribution.
Surface soils (0-5 cm) from remote/rural woodland (coniferous and deciduous) and grassland locations on a latitudinal transectthrough the United Kingdom and Norway were analyzed for polybrominated diphenyl ethers (PBDEs). Concentrations ranged between 65 and 12 000 sigma(ALL)PBDE ng kg(-1) dry weight. PBDE-47, -99, -100, -153, and -154-the major constituents of the penta-BDE technical product-dominated the average congener pattern of the soils. Indeed, the average congener composition and distribution measured in these European background soils closely matched that reported in the technical penta-BDE product. This is interpreted as evidence that transfer of the congeners present in penta-BDE-treated products from source-air-soil occurs with broadly similar efficiency, perhaps because there has been little weathering/degradation/alteration of the congener source pattern by processes operating during atmospheric transport or within the soil itself. BDE-183, a marker for the octa-BDE mix, was detected at concentrations ranging from <9 to 7000 (median approximately 50 ng kg(-1)). In most soils, it made a minor contribution to the sigma(ALL)PBDE concentration, but it was a major component in some samples from northern England. Forest soils tended to have higher concentrations than grasslands. Underlying the average soil composition, some differences in the congener pattern were observed. Notably, there was evidence of latitudinal fractionation, with the relative contribution of PBDE-47 and lighter congeners to the sigmaPBDE increasing northwards (with increasing distance from source areas), while the proportion of PBDE-99 and heavier congeners decreased. Plots of concentration against percentage soil organic matter had different slopes for different congeners. Higher slopes were generally seen for the lighter PBDEs (e.g., PBDE-47), indicating that they have undergone some air-surface exchange (hopping), while the slopes of heavier congeners (e.g., PBDE-153) were close to zero, indicating that they are retained more effectively by soils after deposition.
Air Pollutants↗
PBDEs in the atmosphere of three locations in western Europe.
Atmospheric concentrations of PBDEs (108 samples in total) were measured at 2 rural/semirural sites in England and 1 remote site on the west coast of Ireland in the years 2001 and 2000, respectively. Detailed analysis of the factors affecting concentrations is performed. The United Kingdom (UK) has been a major producer and user of PBDEs. Concentrations of sigmaPBDEs at Mace Head (MH), Ireland ranged between 0.22 and 5.0 pg m(-3) with a mean of 2.6 pg m(-3) and were controlled primarily by advection. sigmaPBDEs concentrations at Hazelrigg (HR), northwest England, ranged between 2.8 and 37 pg m(-3) with a mean of 12 pg m(-3) and at Chilton (CH), southwest England between 3.4 and 33 pg m(-3) with a mean of 11 pg m(-3). The average mixture of PBDEs in air was similar to that of commercial penta-BDE products. Movement of air over local/regional sources influenced concentrations of PBDEs at all sites, particularly at MH. At the two English sites during the summer, concentrations of PBDEs were strongly influenced bytemperature, indicating that air-surface exchange processes play an important role. Advection became more influential during winter, particularly at CH, where a different congener profile was observed in some samples as ambient air temperatures decreased and PBDE concentrations increased. It is hypothesized that this was due to increased emissions from diffuse combustion sources.
Air Movements↗