Temporal trends of organochlorine pesticides in the Canadian Arctic atmosphere

Temperature normalization (TN), multiple linear regression (MLR), and digital filtration (DF) were used to analyze the temporal trends of an atmospheric dataset on organochlorine pesticides (OCs) collected at the Canadian high arctic site of Alert, Nunavut. Details of these techniques have been presented before (Environ. Sci. Technol. 2001, 35, 1303-1311). Both the TN and DF methods revealed that the majority of OC pesticides declined over the 5 years of study, except endosulfan I and several of the pesticide metabolites, including dieldrin and p,p'-DDE. In comparison to studies conducted in the Great Lakes, atmospheric levels in the Arctic were less dependent on temperature, although seasonal variations were apparent. Generally, levels in the winter were lower than during the rest of the year. A notable exception was p,p'-DDE. Many compounds also showed a second minimum in concentrations during June/July and possible explanations are presented to account for this. The estimated first order half-lives for the decline in OC concentrations were generally found to be comparable or slightly longer than those obtained at temperate locations, with the exception of alpha-HCH, which displayed a much longer half-life in the Arctic (approximately 17 yrs). Sporadic increases in heptachlor as well as increases in the ratio of trans- to cis-chlordane suggest episodic input of chlordanes between 1995 and 1997, especially during the winter.     

Potential sources of pesticides,PCBs, and PAHs to the atmosphere of the Great Lakes

A probabilistic model called the potential source contribution function (PSCF) has been used to estimate atmospheric source regions of polycyclic aromatic hydrocarbons (PAHs), chlorinated pesticides, and polychlorinated biphenyls (PCBs) to the Great Lakes. This model allows us to map each compound's source region on a 0.5 degrees x 0.5 degrees latitude/longitude grid centered over the Great Lakes basin. PCBs primarily have urban sources, the strengths of which vary. Like PCBs, PAHs show a strong urban signature, but these compounds also seem to come from rural sites. The source regions of PAH become less distinct as the molecular weight of the compound increases. Since reactivity increases with PAH size, this diminishing trend may be an indication that atmospheric degradation plays a large role in PAH transport. The pesticides have the strongest source regions and are typically transported the farthest, often from areas distant from the Great Lakes basin.     

Aging of organochlorine pesticides and polychlorinated biphenyls in muck soil: volatilization, bioaccessibility, and degradation

An organic rich muck soil which is highly contaminated with native organochlorine pesticide (OCs) was spiked with known amounts of (13)C-labeled OCs and nonlabeled polychlorinated biphenyls (PCBs). Spiked soils were aged under indoor, outdoor, and sterile conditions and the change in volatility, surrogate bioaccessibility, and degradation of chemicals was monitored periodically over 730 d. Volatility was measured using a fugacity meter to characterize the soil-air partition coefficient (K(SA) = C(SOIL)/C(AIR)). The fraction of bioaccessible residues was estimated by comparing recoveries of chemical with a mild extractant, hydroxylpropyl-β-cyclodextrin (HPCD) vs a harsh extractant, DCM. K(SA) of the spiked OCs in the nonsterile (Indoor, Outdoor) soils were initially lower and approached the K(SA) of native OCs over time, showing reduction of volatility upon aging. HPCD extractability of spiked OCs and PCBs were negatively correlated with K(SA), which suggests that volatility can be used as a surrogate for bioaccessibility. Degradation of endosulfans, PCB 8 and 28 was observed in the nonsterile soils, and (13)C(6)-α-HCH showed selective degradation of the (+) enantiomer. Enantiomer fractions (EF) in air and HPCD extracts were lower than in nonsterile soils, suggesting greater sequestering of the (+) enantiomer in the soil during microbial degradation.     

Air-water gas exchange of organochlorine pesticides in Taihu Lake, China

Previous research in the Taihu Lake Region (TLR) of China found high levels of atmospheric organochlorine pesticides (OCPs). To understand the sources and the environmental behaviors of these OCPs in the TLR, research on air-water gas exchange was performed in 2004. Hexachlorocyclohexanes (HCHs), DDT related compounds (DDTs), cis-chlordane (CC), trans-chlordane (TC), heptachlor (HEPT), and alpha-endosulfan in both air and water samples were analyzed, and air-water gas exchange fluxes of these compounds were calculated. The net volatilization flux of alpha-HCH was 58 ng m(-2) day(-1), suggesting that the residue of technical HCH in the lake sediment might have been an important source of alpha-HCH to the air of this region after the ban of technical HCH two decades ago. The main components of technical chlordane, TC, CC, and HEPT, each had net volatilization fluxes >230 ng m(-2) day(-1), suggesting that waste discharge from manufacturing plants in the upper region was the main source of chlordane to the lake. Unlike alpha-HCH and chlordane, o,p'-DDT and alpha-endosulfan had net deposition fluxes, suggesting that these compounds were transported through the atmosphere from land sources and then deposited into the lake. The correlation between air concentrations and ambient air temperature indicated that the current sources of o,p'-DDT and alpha-endosulfan were from land; alpha-HCH and chlordane were mainly from the lake.     

Passive air sampling of PCBs, PBDEs, and organochlorine pesticides across Europe

This study presents concurrently sampled ambient air data for a range of persistent organic pollutants at the continental scale. This was achieved using a passive air sampling system, deploying polyurethane foam disks, which was prepared in one laboratory, sealed to prevent contamination, sent out by courier to volunteers participating in different countries, exposed for 6 weeks, collected, resealed, and returned to the laboratory for analysis. Europe was the study area--a region with a history of extensive POPs usage and emission and with marked national differences in population density, the degree of urbanization and industrial/agricultural development. Samplers were deployed at remote/rural/urban locations in 22 countries and analyzed for PCBs, a range of organochlorine pesticides (HCB, alpha-HCH, gamma-HCH, ppDDT, ppDDE), and PBDEs. Calculated air concentrations were in line with those obtained by conventional active air sampling techniques. The geographical pattern of all compounds reflected suspected regional emission patterns and highlighted localized hotspots. PCB and PBDE levels varied by over 2 orders of magnitude; the highest values were detected in areas of high usage and were linked to urbanized areas. HCB was relatively uniformly distributed, reflecting its persistence and high degree of mixing in air. Higher gamma-HCH, ppDDT, and ppDDE levels generally occurred in South and East Europe.     

The global distribution of PCBs and organochlorine pesticides in butter

In this study we explored the use of butter as a sampling matrix to reflect the regional and global scale distribution of PCBs and selected organochlorine pesticides/metabolites in air. This was because persistent organic pollutants (POPs) concentrate in dairy fats, where concentrations are controlled by feed intake (primarily from pasture/silage), which is in turn primarily controlled by atmospheric deposition. Butter sigmaPCB concentrations varied by a factor of approximately 60 in 63 samples from 23 countries. They were highest in European and North American butter and lowest in southern hemisphere (Australian, New Zealand) samples, consistent with known patterns of historical global usage and estimated emissions. Concentrations in butter reflected differences in the propensity of PCB congeners to undergo long range atmospheric transport from global source regions to remote areas and the relatively even distribution of HCB in the global atmosphere. Concentrations of p,p'-DDT, p,p'-DDE, and HCH isomers all varied over many orders of magnitude in the butter samples, with highest levels in areas of current use (e.g. India and south/central America for DDT; India, China, and Spain for HCH). We conclude that butter is sensitive to local, regional, and global scale spatial and temporal atmospheric trends of many POPs and may therefore provide a useful sampling medium for monitoring purposes. However, to improve the quantitative information derived on air concentrations requires an awareness of climatic and livestock management factors which influence air-milk fat transfer processes.     

Organochlorine pesticides in the soils and atmosphere of Costa Rica

A survey of the contamination of the physical environment of Costa Rica with banned organochlorine pesticides (OCPs) relied on sampling air and soil at 23 stations acrossthe country in 2004. Average annual air concentrations, determined with XAD-based passive samplers, and surface soil concentrations were generally low when compared to values reported for North and Central America, which is consistent with relatively low historical domestic use and little atmospheric inflow from neighboring countries. Statistical analysis and concentration maps reveal three types of spatial distribution: alpha-hexachlorocyclohexane and p,p'-DDD had a relatively uniform distribution across the country; other DDT-related species were greatly elevated over the national average at Manuel Antonio, a National Park on the Pacific coast; and dieldrin, lindane, and chlordane-related species had higher concentrations in Costa Rica's populated Central Valley. An altitudinal transect of stations in the Central Valley shows declining air-soil concentration ratios with elevation for lindane, likely driven by atmospheric inversions and soil organic carbon content. Enantiomeric composition of chiral OCPs in air and soil was close to racemic, with slight depletion of (-)-alpha-HCH, (-)-cis-chlordane, and (+)-trans-chlordane. Estimated air-soil fugacity fractions are highly uncertain but indicate equilibrium conditions for most OCPs, net volatilization of lindane at some sites, and net deposition for p,p'-DDE. The study demonstrates an approach for quickly evaluating the spatial distribution of OCPs in an understudied area, identifying regionally important contaminants and areas of elevated concentrations.     

Temporal and spatial trends of organochlorine pesticides in Great Lakes precipitation

Organochlorine pesticide concentrations in precipitation samples collected from 1997 to 2003 at seven Integrated Atmospheric Deposition Network sites around the Great Lakes are reported. The 28-day volume weighted mean concentrations of several pesticides, including gamma-hexachlorocyclohexane (HCH), endosulfan, hexachlorobenzene, chlordane, and DDE, showed significant seasonal trends. For current-use pesticides (endosulfan and gamma-HCH), their concentrations peaked in late spring to summer just after their agricultural application. For the banned pesticides, higher concentrations were observed in the winter due to their enhanced partitioning to particles and scavenging by snow. Long-term decreasing trends were observed for several pesticides such as gamma-HCH and DDE. On the other hand, beta-HCH showed significant increasing concentrations as a function of time at Brule River, Eagle Harbor, and Sleeping Bear Dunes. Generally, Chicago had the highest concentration of chlordanes, dieldrin, and DDT, indicating that urban areas could be a source for these compounds to precipitation. For gamma-HCH and endosulfans, Point Petre had the highest concentrations due to the application of these pesticides in the surrounding areas.     

Fate of chiral and achiral organochlorine pesticides in the north atlantic bloom experiment

Organochlorine pesticides (OCPs) were measured in the surface seawater and lower atmosphere during the North Atlantic Bloom Experiment in the spring 2008 from samples collected on the R/V Knorr. The gaseous concentration profiles resulted from both long-range transport (LRT) from the Arctic by polar easterlies and local biogeochemical processes. Relatively constant α/γ-hexachlorocyclohexane (HCH) ratios and enantiomer fractions of α-HCH indicated that a single water mass was sampled throughout the cruise. Changes in dissolved phase concentrations were dominated by bloom processes (air-water exchange, partitioning to organic particles, and subsequent sinking) rather than LRT. α-HCH and dissolved phase trans-chlordanes showed depletion of (+) enantiomer, whereas depletion of the (-) enantiomer was observed for heptachlor exo-epoxide (HEPX) and cis-chlordanes. Fugacity ratio calculations suggest that hexachlorobenzene (HCB) and γ-HCH were depositing from air to water whereas heavier OCPs (chlordanes, HEPX) were evaporating. Dissolved phase concentrations did not decrease with time during the three-week bloom period; neither were lipophilic OCPs drawn down from air to water as previous studies hypothesized. Comparison with Arctic measurements suggested that the Arctic returned higher concentrations of α-HCH and HCB through both the atmospheric (polar easterlies) as well as oceanic transport (East Greenland Current) to the lower latitudes.     

Passive air sampling of polychlorinated biphenyls and organochlorine pesticides at the Korean Arctic and Antarctic research stations: implications for long-range transport and local pollution

To assess levels and patterns of polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in polar regions, XAD-resin based passive air samplers were deployed for one year at the Korean polar research stations at Ny-Alesund, Norway (2005-2006) and King George Island, Antarctica (2004-2005). Backward trajectories suggest that these stations are affected by long-range transport from source regions in Northern Europe and Russia and the southern tip of South America, respectively. Relatively high levels of PCB-11, averaging 60 pg x m(-3), were observed in Antarctica, suggesting an unusual source of PCB-11 to the Southern Hemisphere. Reflecting the hemispheric distribution of global PCB emissions, the average level of sigma205PCB (excluding three mono-CBs and PCB-11) was five times higher in the Arctic (95 pg x m(-3)) than in the Antarctic (19 pg x m(-3)). Levels of sigma9PCB at Ny-Alesund were similarto those reported for other Arctic sites, while levels at King George Island were lower than at other sites on the Antarctic Peninsula but 1 order of magnitude higher than background levels measured at a more remote Antarctic site. Light homologues were predominant in all samples (except for one Arctic sample), consistent with the hypothesis of global fractionation and predictions of long-range transport potential. Dominance of heavy PCBs on the roof of the main building at Ny-Alesund and a concentration gradient with distance from the main building at King George Island strongly indicated the influence of local sources. OCP levels were also influenced by long-range transport but not by local sources. This study highlights the feasibility of using passive air sampling to assess both long-range transport and local pollution in remote regions.     

Comparison of PCDD/F and dl-PCB levels in Turkish foodstuffs: industrial versus rural,local versus supermarket products,and assessment of dietary intake

Polychlorinated dibenzo-p-dioxin and dibenzofurans (PCDD/Fs) and dioxin-like and non-dioxin-like (indicator) polychlorinated biphenyls (PCBs) were monitored in various foodstuffs of animal origin and edible oil samples obtained from two different cities in Turkey both rural and industrial. Total dioxin+dioxin-like PCBs and indicator PCB concentrations of pooled samples ranged 0.20–4.19 pg World Health Organization-Toxic Equivalency (WHO-TEQ)₍₁₉₉₈₎/g fat and 57.2–1710 pg/g fat, respectively. The dominant congeners were 2,3,4,7,8-PeCDF, 1,2,3,7,8-PeCDD, 2,3,7,8-TCDD and PCB126. Dietary intake of dioxin+dioxin-like PCBs and indicator PCBs from fish, dairy products, edible oil, egg and meat was 0.509 pg WHO-TEQ₁₉₉₈/kg bw (body weight)/day and 839 pg/kg bw/day in Afyon and 0.588 pg WHO-TEQ₁₉₉₈/ kg bw/day and 1070 pg/kg bw/day in Kocaeli, respectively. The major contributors to total exposure were dairy products and fish. Despite the unexplained high contamination level in an individual egg sample from Kocaeli, average concentration levels in Turkey, even in industrialized regions, were low compared to reported concentrations in Western Europe. Exposure levels were well below the tolerable daily intake (TDI) of 2 pg WHO-TEQ₁₉₉₈/kg body weight.     

Multiresidue analysis of PCB, organochlorine pesticides and chlordanes in marine products by GC-micro ECD

A multiresidue method using dual-injection, dual-column, and dual-micro electron capture detection gas chromatography (dual-column GC-μECD) was developed for the determination of PCB, organochlorine pesticides and chlordanes in marine products. The sample was extracted with hexane-acetone (2 : 1), and the extract was cleaned up by gel permeation chromatography(GPC)/solid-phase extraction (SPE). The GPC fraction was selectively collected, and loaded directly onto a graphitized carbon/PSA 2-layered column. After fractionation by 4% hydrated silica-gel column chromatography, each fraction was determined by dual-column GC-μECD. Recoveries of PCB, organochlorine pesticides and chlordanes were in the ranges of 84-109% (RSD ≤ 21.6%), 74-117% (RSD ≤ 14.6%) and 69-114% (RSD ≤ 12.9%), respectively. This method is superior to single chromatography for the determination of total PCB, and should be useful for monitoring of these pollutants in marine products.     

Enantioselective degradation of organochlorine pesticides in background soils: variability in field and laboratory studies

Variability in the enantioselective degradation of chiral organochlorine pesticides (alpha-HCH, cis- and trans-chlordane (CC and TC), and o,p'-DDT) in the field and laboratory was investigated. Background soils presumably receive the same EF signature of a compound via atmospheric deposition and then degrade that compound in a way that can vary over small spatial areas. Background soils from woodland and grassland areas were sampled to compare chiral signatures and determine the spatial variability within a few square meters. The enantiomer fractions, EF = areas of the (+)/[(+)+(-)]-enantiomers, showed variability between and within ecosystems. For example, the EF of CC varied between 0.272 -and 0.558 in nine samples taken over a few square meters, and a range of 0.431-0.506 was found within depths of a few centimeters. Woodland and grassland soils were spiked with alpha-HCH, TC, CC, and o,p'-DDT, and one portion was placed in the field to monitor changes in EF under in situ conditions and the other taken to the laboratory. In general, the enantiomer degradation preferences in the laboratory paralleled those in the field, with some differences. Soil organic matter content and pH exerted a minor influence on this variability. The results of this study have implications for the use of chiral compounds to make inferences about air-soil exchange and for the mechanisms of biodegradation/ biotransformation of anthropogenic compounds in soils.     

Fate of brominated flame retardants and organochlorine pesticides in urban soil: volatility and degradation

As the uses of polybrominated diphenyl ethers (BDEs) are being phased out in many countries, soils could become a secondary emission source to the atmosphere. It is also anticipated that the demand for alternative brominated flame retardants (BFRs) will grow, but little is known about their environmental fate in soils. In this study, the volatility and degradation of BFRs and organochlorine pesticides (OCPs) in soil was investigated. A low organic carbon (5.6%) urban soil was spiked with a suite of BFRs and OCPs, followed by incubation under laboratory condition for 360 days. These included BDE- 17, -28, -47, -99; α- and β-1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane (TBECH), β-1,2,5,6-tetrabromocyclooctane (TBCO), and 2,3-dibromopropyl-2,4,6-tribromophenyl ether (DPTE), OCPs: α-hexachlorocyclohexane (α-HCH) and (13)C(6)-α-HCH, trans-chlordane (TC), and (13)C(10)-TC. The volatility of spiked chemicals was investigated using a fugacity meter to measure the soil-air partition coefficient (K(SA)). K(SA) of some spiked BFRs and OCPs increased from Day 10 to 60 or 90 and leveled off afterward. This suggests that the volatility of BFRs and OCPs decreases over time as the chemicals become more strongly bound to the soil. Degradation of alternative BFRs (α- and β-TBECH, β-TBCO, DPTE), BDE-17, and α-HCH ((13)C-labeled and nonlabeled) was evident in soils over 360 days, but no degradation was observed for the BDE-28, -47, -99, and TC ((13)C-labeled and nonlabeled). A method to separate the enantiomers of α-TBECH and β-TBCO was developed and their degradation, along with α-HCH ((13)C-labeled and nonlabeled) was enantioselective. This is the first study which reports the enantioselective degradation of chiral BFRs in soils. Discrepancies between the enantiomer fraction (EF) of chemicals extracted from the soil by dichloromethane (DCM) and air were found. It is suggested that DCM removes both the sequestered and loosely bound fractions of chemicals in soil, whereas air accesses only the loosely bound fraction, and these two pools are subject to different degrees of enantioselective degradation. This calls for caution when interpreting EFs obtained from DCM extraction of soil with EFs in ambient air.     

Atmospheric distribution and long-range transport behavior of organochlorine pesticides in North America

Annually averaged concentrations and enantiomeric compositions of organochlorine pesticides (OCPs) in air were determined in 2000/2001 at 40 stations across North America using XAD-based passive samplers. Absolute concentration differences acrossthe continent, the skewness and kurtosis of the concentration distribution, the relative abundance of parent compound and metabolites, and the chiral signatures can identify regional sources of OCP to the atmosphere. Specifically, air samples collected in the southeastern United States had elevated concentrations of chlordane-related compounds, higher ratios of trans- to cis-chlordane and heptachlor to heptachlor epoxide, as well as higher enantiomeric fractions of trans-chlordane as compared to other regions, suggesting continued release of microbially unprocessed chlordane to the regional atmosphere. Similarly, greatly elevated concentrations of p,p'-DDT, low relative abundance of the metabolite DDE, and a racemic composition of o,p'-DDT in samples from southern Mexico and Belize indicate recent use of DDT in these regions. Belize is also a potential source region for dieldrin. Reflecting its continued use in North America, endosulfan is now one of the most abundant and ubiquitous OCPs in the continental atmosphere. In contrast to these OCPs, air concentrations of penta- and hexachlorobenzene vary only by factors of 2-4 across the continent, reflecting a long atmospheric residence time and few primary sources. Atmospheric levels of the chlorobenzenes, alpha-endosulfan, and p,p'-DDE increase with elevation in the Canadian Rocky Mountains. Empirical travel distances for the OCPs derived from latitudinal concentration profiles are in good agreementwith model-derived indicators of long-range transport potential and, in particular, lead to a similar categorization of the OCPs. Large-scale passive air sampling networks are suitable for monitoring compliance with, and effectiveness of, regulatory control measures and for establishing experimentally the atmospheric long-range transport behavior of organic air pollutants.     

Chlorinated polycyclic aromatic hydrocarbons in the atmosphere: seasonal levels, gas-particle partitioning, and origin

Ambient concentrations of 26 chlorinated polycyclic aromatic hydrocarbons (CIPAHs) with 2- to 5-rings were investigated in a Japanese urban city from December 2004 to December 2005. All the targeted CIPAHs were detected in either the gaseous or particulate phase. During the study, the ambient (gaseous + particulate) concentration of total CIPAH ranged from 18 to 330 pg m(-3). The concentrations of gaseous CIPAHs tended to be 2 approximately 100 times higher than those of particulate CIPAHs. A seasonal variability of both gaseous and particulate CIPAH concentrations was observed, with higher concentrations in winter than in summer. A compositional analysis also showed a characteristic trend: relatively low molecular weight CIPAHs dominated in warmer seasons, and high molecular weight CIPAHs dominated in colder seasons. For some CIPAHs, temperature dependence of gas-phase concentrations was statistically significant (p < 0.05), and temperature accounted for 27-63% of the variability in their concentrations. The natural logarithm of total concentrations of particulate CIPAHs were significantly correlated (p < 0.05) with the reciprocal mean temperatures, but not for gaseous CIPAHs, suggesting that there are differences of the sources and ambient fates between gaseous and particulate CIPAHs. Back trajectory analyses suggested that air masses, originating from China, were associated with the highest CIPAH concentrations.     

Selection of bioindicators of polybrominated diphenyl ethers, polychlorinated biphenyls, and organochlorine pesticides in mollusks in the Chinese Bohai Sea

Mollusks, including bivalve and gastropod samples, were collected in the summer of 2006 and 2007 to evaluate the spatial patterns of organochlorine pesticides (OCPs), polychlorinated biphenyl (PCBs), and polybrominated biphenyl ethers (PBDEs) in the coastal water of the Chinese Bohai Sea. Seven species of mollusks, including Rapana venosa (Rap), Neverita didyma (Nev), Scapharca subcrenata (Sca), Mytilus edulis (Blue mussel, Myt), Amusium (Amu), Meretix meretrix (Mer), and Crassostrea talienwhanensis (Oyster, Ost) were investigated to select appropriate bioindicators. Compared with other species, Ost and Myt possess higher lipid contents and have higher concentrations of OCPs and PBDEs. Multivariate linear regression analysis revealed that the most influential factor on the contaminant concentrations in mollusks is the trophic level (TL), followed by the lipid contents. Concentrations of OCPs, PCBs, and PBDEs correlated negatively with the TL of the selected mollusks. Results of principal component and correlation analyses suggest that Ost and Myt can be used as potential bioindicators of pollution by OCPs, PCBs, and PBDEs of the Chinese Bohai Sea.     

2001 survey of organochlorine pesticides in retail milk from Beijing, P R China.

A monitoring study was conducted in 2001 to determine the organochlorine pesticides and their metabolite residues in milk taken from supermarkets in Beijing, P. R. China. The average concentrations of total HCH and DDT were 0.038 and 0.046 mg x kg(-1), respectively, expressed on a fat basis. The aldrin residue was detected in nine milk samples, with a mean concentration of 0.035 mg x kg(-1). Heptachlor and its epoxides were not found in any milk samples. Of 72 milk samples analysed, three from South China contained the higher levels of DDT and HCH residues that exceeded the FAO/WHO accepted tolerance level. Although organochlorine pesticides such as DDT and HCH have been banned in China since 1983, the residues of such compounds still exist in the environment and cause food contamination, a fact likely attributed to the short prohibition period and illegal use for agricultural purposes at present.     

Atmospheric concentrations and air-water flux of organochlorine pesticides along the Western Antarctic Peninsula

Air, seawater, sea ice, and snow were collected during the austral winter (September-October 2001) and summer (January-February 2002) along the Western Antarctic Peninsula. Hexachlorobenzene (HCB) > heptachlor > alpha- and gamma-hexachlorocyclohexane (HCH) and heptachlor epoxide, were the most frequently detected organochlorine pesticides in air. HCB and HCH levels declined over the past 20 years, with a half-life of 3 years for sigmaHCH in Antarctic air. However, heptachlor epoxide levels have not declined in Antarctic air over the past decade, possibly due to continued use of heptachlor in the southern hemisphere. Peak heptachlor concentrations in air were measured coincident with air masses moving into the region from lower latitudes. Levels of lindane were 1.2-200 times higher in annual sea ice and snow compared to alpha-HCH, likely due to greater atmospheric input of gamma-HCH. The ratio of alpha/gamma-HCH in Antarctic air, sea ice and snow was <1, illustrative of a predominance of influx of lindane versus technical HCH to the regional environment. However, alpha/gamma-HCH in seawater was >1, likely due to more rapid microbial degradation of gamma- versus alpha-HCH. Water/air fugacity ratios for HCHs demonstrate continued atmospheric influx of HCHs to coastal Antarctic seas, particularly during late summer.     

Distribution of organochlorine pesticides in the northern South China Sea: implications for land outflow and air-sea exchange

The South China Sea (SCS) is surrounded by developing countries in Southeast Asia, where persistent organic pollutants (POPs), such as organochlorine pesticides (OCPs), are still used legally or illegally, and are of concern. Yet little is known about the distribution of OCPs in the water and atmosphere over SCS, as well as their air-sea equilibrium status and time trends. In this study, ship-board air samples and surface seawater collected in the northern SCS between September 6 and 22, 2005 were analyzed for selected OCPs. The measured OCP concentrations in the atmosphere over the northern SCS were influenced by proximity to source regions and air mass origins. The highest atmospheric OCP concentrations were found at sampling sites adjacent to continental South China. OCPs in surface seawater showed significant spatial variations, with the highest concentration observed in a water sample from off Vietnam. The coastal currents were suggested to play a key role in the delivery of waterborne OCPs in the northern SCS. Time trend, land outflow, and air-sea exchange of selected OCPs in the SCS were investigated, by comparison of this dataset with historical data.