Unraveling the Marine Microplastic Cycle: The First Simultaneous Data Set for Air, Sea Surface Microlayer, and Underlying Water.

Microplastics (MP) including tire wear particles (TWP) are ubiquitous. However, their mass loads, transport, and vertical behavior in water bodies and overlying air are never studied simultaneously before. Particularly, the sea surface microlayer (SML), a ubiquitous, predominantly organic, and gelatinous film (<1 mm), is interesting since it may favor MP enrichment. In this study, a remote-controlled research catamaran simultaneously sampled air, SML, and underlying water (ULW) in Swedish fjords of variable anthropogenic impacts (urban, industrial, and rural) to fill these knowledge gaps in the marine-atmospheric MP cycle. Polymer clusters and TWP were identified and quantified with pyrolysis-gas chromatography-mass spectrometry. Air samples contained clusters of polyethylene terephthalate, polycarbonate, and polystyrene (max 50 ng MP m-3). In water samples (max. 10.8 µg MP L-1), mainly TWP and clusters of poly(methyl methacrylate) and polyethylene terephthalate occurred. Here, TWP prevailed in the SML, while the poly(methyl methacrylate) cluster dominated the ULW. However, no general MP enrichment was observed in the SML. Elevated anthropogenic influences in urban and industrial compared to the rural fjord areas were reflected by enhanced MP levels in these areas. Vertical MP movement behavior and distribution were not only linked to polymer characteristics but also to polymer sources and environmental conditions.

A marine biogenic source of atmospheric ice-nucleating particles.

The amount of ice present in clouds can affect cloud lifetime, precipitation and radiative properties. The formation of ice in clouds is facilitated by the presence of airborne ice-nucleating particles. Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice. Sea-spray aerosol contains large amounts of organic material that is ejected into the atmosphere during bubble bursting at the organically enriched sea-air interface or sea surface microlayer. Here we show that organic material in the sea surface microlayer nucleates ice under conditions relevant for mixed-phase cloud and high-altitude ice cloud formation. The ice-nucleating material is probably biogenic and less than approximately 0.2 micrometres in size. We find that exudates separated from cells of the marine diatom Thalassiosira pseudonana nucleate ice, and propose that organic material associated with phytoplankton cell exudates is a likely candidate for the observed ice-nucleating ability of the microlayer samples. Global model simulations of marine organic aerosol, in combination with our measurements, suggest that marine organic material may be an important source of ice-nucleating particles in remote marine environments such as the Southern Ocean, North Pacific Ocean and North Atlantic Ocean.

The Role of Extracellular Carbonic Anhydrase in Biogeochemical Cycling: Recent Advances and Climate Change Responses.

Climate change has been predicted to influence the marine phytoplankton community and its carbon acquisition strategy. Extracellular carbonic anhydrase (eCA) is a zinc metalloenzyme that catalyses the relatively slow interconversion between HCO3- and CO2. Early results indicated that sub-nanomolar levels of eCA at the sea surface were sufficient to enhance the oceanic uptake rate of CO2 on a global scale by 15%, an addition of 0.37 Pg C year-1. Despite its central role in the marine carbon cycle, only in recent years have new analytical techniques allowed the first quantifications of eCA and its activity in the oceans. This opens up new research areas in the field of marine biogeochemistry and climate change. Light and suitable pH conditions, as well as growth stage, are crucial factors in eCA expression. Previous studies showed that phytoplankton eCA activity and concentrations are affected by environmental stressors such as ocean acidification and UV radiation as well as changing light conditions. For this reason, eCA is suggested as a biochemical indicator in biomonitoring programmes and could be used for future response prediction studies in changing oceans. This review aims to identify the current knowledge and gaps where new research efforts should be focused to better determine the potential feedback of phytoplankton via eCA in the marine carbon cycle in changing oceans.

Extracellular carbonic anhydrase: Method development and its application to natural seawater.

We developed an effective fluorometric technique to quantify extracellular carbonic anhydrase (eCA) present in natural seawater samples. The technique includes the separation of eCA from cells to achieve low detection limits through high signal : noise ratios. eCA was efficiently extracted from cell membranes by treatment with 0.1 M phosphate buffer containing 2.5 M NaCl. The free eCA specifically forms a fluorescent complex with dansylamide, and the detection limit of the complex is below 0.1 nM. We applied the technique to samples from different culture solutions and natural seawater collected from the Baltic Sea. We observed eCA concentrations to be in the range of 0.10-0.67 nM in natural seawater. The data indicated that this technique is very sensitive, accurate, and feasible for routine and shipboard measurement of eCA from natural seawater. It is therefore an effective and rapid tool to investigate the carbon acquisition of phytoplankton both in mono culture as well natural communities.

The impact of rainfall on the sea surface salinity: a mesocosm study.

Sea surface salinity may serve as a tracer for freshwater fluxes because it is linked to evaporation and precipitation that force the freshwater balance of the ocean's surface. The relationship between freshwater fluxes and salinity anomalies in the upper few centimeters remains widely unknown. In a mechanistic approach, we investigated how these anomalies develop by conducting experiments with artificial rain over a large basin. We measured conductivity and temperature at different depths and rain characteristics (intensity, rain temperature, droplet sizes, and velocities). In the absence of turbulence, the rain causes a strong salinity change of up to 6.02 g kg - 1 in 0-4 cm depth. At the highest rain intensity of 56 mm h - 1 , salinity changed thrice as fast as at an intensity of 18 mm h - 1 . At the sea surface microlayer (first millimeter of the surface) the anomalies are always highest and reached a maximum of 14.18 g kg - 1 . With mechanical mixing, salinity changes were less pronounced (maximum SML salinity anomaly: 6.17 g kg - 1 ), and freshwater was mixed fast with the existing seawater body. In general, our study shows that freshwater remains in the upper few centimeters, and even with induced turbulence, are not mixed below 16 cm.

Vertical distribution and risk assessment of pharmaceuticals and other micropollutants in southern North Sea coastal waters.

Pharmaceutical compounds are micropollutants of emerging concern, as well as other classes of chemicals such as UV filters and artificial sweeteners. They enter marine environments via wastewater treatment plants, aquaculture runoff, hospital effluents, and shipping activities. While many studies have investigated the presence and distribution of these pollutants in numerous coastal areas, our study is the first to focus on their occurrence, spatial distribution, and vertical distribution in the sea surface microlayer (SML) and the near-surface layer of marine environments. We analyzed 62 pharmaceutical compounds, one UV filter, and six artificial sweeteners from the SML to the corresponding underlying water (0 cm, 20 cm, 50 cm, 100 cm, and 150 cm) at four stations in the southern North Sea. One station is the enclosed Jade Bay, one is the Weser estuary at Bremerhaven, and the other two stations (NS_7 and NS_8) are in the open German Bight. Jade Bay receives pollutants from surrounding wastewater treatment plants, while the Weser estuary receives pollutants from cities like Bremerhaven, which has dense populations and industrial activities. Concentrations of pharmaceutical compounds were higher in the upper water layers (from the SML to 20 cm). Eleven pharmaceutical compounds (caffeine, carbamazepine, gemfibrozil, ibuprofen, metoprolol, salicylic acid, clarithromycin, novobiocin, clindamycin, trimethoprim, and tylosin) were detected in >95 % of our samples. One UV filter (benzophenone-4) was found in 83 % and three artificial sweeteners (acesulfame, saccharin, and sucralose) in 100 % of all our samples. All artificial sweeteners posed high risks to the freshwater invertebrate Daphnia magna. Understanding the spatial and vertical distribution of pharmaceuticals and other micropollutants in marine environments may be essential in assessing their dispersal and detection in other aquatic environments.

Usage of antibiotics in aquaculture and the impact on coastal waters.

For decades, coastal marine ecosystems have been threatened by a wide range of anthropogenic pollutants. Recently, there has been increasing concern about the accumulation and impacts of antibiotic compounds on marine ecosystems. However, information regarding the accumulation of antibiotics and the impacts they may have on microbial communities in coastal water bodies and on human health is sparse in literature. Antibiotics from aquacultures are constantly discharged into marine environments via rivers. Large rivers transport tons of antibiotics every year into coastal waters, e.g., 12 tons of sulfonamide by the river Mekong. Here, we discuss a potential influence of such imported antibiotics on bacterial communities in coastal waters. Potential accumulation of antibiotics in the uppermost surface layer of aquatic ecosystems, the so-called sea surface microlayer (SML), is of interest. Because of the ability of the SML to accumulate anthropogenic pollutants, it may serve as a pool for antibiotics and correspondingly also for resistant organisms. Also, due to its biofilm-like structure, the SML could serve as a hotspot for horizontal gene transfer, speeding up the spread of antibiotic resistant strains to encompassing marine environments. The emergence of antibiotic resistant bacteria is a global threat and scientists projected that it could pave the way for the next pandemic that could ravage the world in the next decades. For this reason, it is time to focus research on understanding and minimizing the impact of antibiotics on the sustainability of coastal waters and on the health of humans who depend on coastal resources for food and recreational purposes. Also, knowledge about antibiotics in the SML is necessary to understand the effects they are likely to have on bacterial abundance, diversity, and metabolic activities in coastal water bodies.

Occurrence and backtracking of microplastic mass loads including tire wear particles in northern Atlantic air.

Few studies report the occurrence of microplastics (MP), including tire wear particles (TWP) in the marine atmosphere, and little data is available regarding their size or sources. Here we present active air sampling devices (low- and high-volume samplers) for the evaluation of composition and MP mass loads in the marine atmosphere. Air was sampled during a research cruise along the Norwegian coast up to Bear Island. Samples were analyzed with pyrolysis-gas chromatography-mass spectrometry, generating a mass-based data set for MP in the marine atmosphere. Here we show the ubiquity of MP, even in remote Arctic areas with concentrations up to 37.5 ng m-3. Cluster of polyethylene terephthalate (max. 1.5 ng m-3) were universally present. TWP (max. 35 ng m-3) and cluster of polystyrene, polypropylene, and polyurethane (max. 1.1 ng m-3) were also detected. Atmospheric transport and dispersion models, suggested the introduction of MP into the marine atmosphere equally from sea- and land-based emissions, transforming the ocean from a sink into a source for MP.

Ecogenomics and cultivation reveal distinctive viral-bacterial communities in the surface microlayer of a Baltic Sea slick.

Visible surface films, termed slicks, can extensively cover freshwater and marine ecosystems, with coastal regions being particularly susceptible to their presence. The sea-surface microlayer (SML), the upper 1-mm at the air-water interface in slicks (herein slick SML) harbors a distinctive bacterial community, but generally little is known about SML viruses. Using flow cytometry, metagenomics, and cultivation, we characterized viruses and bacteria in a brackish slick SML in comparison to non-slick SML as well as seawater below slick and non-slick areas (subsurface water = SSW). Size-fractionated filtration of all samples distinguished viral attachment to hosts and particles. The slick SML contained higher abundances of virus-like particles, prokaryotic cells, and dissolved organic carbon compared to non-slick SML and SSW. The community of 428 viral operational taxonomic units (vOTUs), 426 predicted as lytic, distinctly differed across all size fractions in the slick SML compared to non-slick SML and SSW. Specific metabolic profiles of bacterial metagenome-assembled genomes and isolates in the slick SML included a prevalence of genes encoding motility and carbohydrate-active enzymes (CAZymes). Several vOTUs were enriched in slick SML, and many virus variants were associated with particles. Nine vOTUs were only found in slick SML, six of them being targeted by slick SML-specific clustered-regularly interspaced short palindromic repeats (CRISPR) spacers likely originating from Gammaproteobacteria. Moreover, isolation of three previously unknown lytic phages for Alishewanella sp. and Pseudoalteromonas tunicata, abundant and actively replicating slick SML bacteria, suggests that viral activity in slicks contributes to biogeochemical cycling in coastal ecosystems.

Sea foams are ephemeral hotspots for distinctive bacterial communities contrasting sea-surface microlayer and underlying surface water.

The occurrence of foams at oceans' surfaces is patchy and generally short-lived, but a detailed understanding of bacterial communities inhabiting sea foams is lacking. Here, we investigated how marine foams differ from the sea-surface microlayer (SML), a <1-mm-thick layer at the air-sea interface, and underlying water from 1 m depth. Samples of sea foams, SML and underlying water collected from the North Sea and Timor Sea indicated that foams were often characterized by a high abundance of small eukaryotic phototrophic and prokaryotic cells as well as a high concentration of surface-active substances (SAS). Amplicon sequencing of 16S rRNA (gene) revealed distinctive foam bacterial communities compared with SML and underlying water, with high abundance of Gammaproteobacteria. Typical SML dwellers such as Pseudoalteromonas and Vibrio were highly abundant, active foam inhabitants and thus might enhance foam formation and stability by producing SAS. Despite a clear difference in the overall bacterial community composition between foam and SML, the presence of SML bacteria in foams supports the previous assumption that foam is strongly influenced by the SML. We conclude that active and abundant bacteria from interfacial habitats potentially contribute to foam formation and stability, carbon cycling and air-sea exchange processes in the ocean.

Global reduction of in situ CO2 transfer velocity by natural surfactants in the sea-surface microlayer.

For decades, the effect of surfactants in the sea-surface microlayer (SML) on gas transfer velocity (k) has been recognized; however, it has not been quantified under natural conditions due to missing coherent data on in situ k of carbon dioxide (CO2) and characterization of the SML. Moreover, a sea-surface phenomenon of wave-dampening, known as slicks, has been observed frequently in the ocean and potentially reduces the transfer of climate-relevant gases between the ocean and atmosphere. Therefore, this study aims to quantify the effect of natural surfactant and slicks on the in situ k of CO2. A catamaran, Sea Surface Scanner (S3), was deployed to sample the SML and corresponding underlying water, and a drifting buoy with a floating chamber was deployed to measure the in situ k of CO2. We found a significant 23% reduction of k above surfactant concentrations of 200 µg Teq l-1, which were common in the SML except for the Western Pacific. We conclude that an error of approximately 20% in CO2 fluxes for the Western Pacific is induced by applying wind-based parametrization not developed in low surfactant regimes. Furthermore, we observed an additional 62% reduction in natural slicks, reducing global CO2 fluxes by 19% considering known frequency of slick coverage. From our observation, we identified surfactant concentrations with two different end-members which lead to an error in global CO2 flux estimation if ignored.

The Ocean's Skin Layer in the Tropics.

We provide a large data set on salinity anomalies in the ocean's skin layer together with temperature anomalies and meteorological forcing. We observed an average salinity anomaly of 0.40 ± 0.41 practical salinity unity (n = 23,743), and in 83% of the observations the salinity anomaly was positive; that is, the skin layer was more saline. Temperature anomalies determined by an infrared camera were -0.23 ± 0.28 °C (upper 20-µm layer in reference to nominal 1-mm depth) and slightly warmer with -0.19 ± 0.25 °C in an upper 80-µm layer in reference to 1-m depth. In 75% of the observations, our data confirmed the presence of a cooler skin layer. Light rain rates (<4 mm/hr) induced an immediate freshening by 0.25 practical salinity unit in the skin layer without any effect in the mixed layer at 1-m depth. Vertical mixing by strong winds (12 m/s) masked freshening during a heavy rain fall (47 mm/hr) by the intrusion of saltier deeper waters, but a freshening was observed after the wind and rain calmed down. We computed density anomalies, which suggest that denser skin layers can remain afloat up to a density anomaly of 1.3 g/L, likely due to the interfacial tension between the skin layer and underlying bulk water. It implies that salinization by evaporation regulates buoyancy fluxes, a key process for the exchange of climate-relevant gases and heat between the ocean and atmosphere.

High-resolution observations on enrichment processes in the sea-surface microlayer.

For decades, researchers assumed that enrichment of dissolved organic matter (DOM) in the sea surface microlayer (SML) is solely controlled by changes in the DOM concentration at this uppermost thin boundary layer between the ocean and the atmosphere. We conducted high-resolution observations of fluorescent-DOM (FDOM) at 13 stations in the coastal and open Atlantic Ocean to understand the enrichment processes. Results show that FDOM enrichment in the SML varied between 0.8 and 2.0 (in comparison to the concentrations in the underlying water; ULW), and FDOM enrichment is a common feature of the SML despite the varied distances to the terrestrial sources. At six stations, the FDOM concentration in the SML was less variable over the sampling period (>5 h) compared to FDOM concentrations in the ULW characterized with sudden changes. Even so we observed slightly lower enrichments with increasing wind speeds and solar radiation, changes in ULW concentrations forced the enrichment to change. In addition, we found evidences for the occurrence of photochemical degradation of FDOM in near-shore SML with implications on coastal carbon cycling. Overall, the results show that the processes leading to the enrichment of DOM in the SML are more complex than previously assumed. Given the importance of the organic-rich SML as a diffusion layer in the air-sea exchange of climate-relevant gases and heat, understanding the layer's enrichment processes is crucial.

A modified technique for field measurements of dry deposition fluxes of polychlorinated biphenyls in tropical regions.

This report focused on the development of a technique to measure dry deposition fluxes of PCBs in tropical environments. Temperature resistant double-adhesive tape has been used as a new surrogate surface for collection of deposited PCBs. The new technique includes the measurement of field blanks for the entire sampling period. A sonication-assisted extraction procedure has been validated for the extraction of PCBs from the tape. The new technique has been used in the field for a period of 4 months in the tropical region of Singapore. The average dry deposition flux measured for total PCBs was 15.3 ng m(-2) day(-1) and, on a global scale, this can be considered to be low.

Atmospheric wet deposition of PAHs to the sea-surface microlayer.

Sea-surface microlayer (SML) and subsurface seawater samples (SSW) collected from Singapore's coastal environment were analyzed for 14 polycyclic aromatic hydrocarbons (PAHs) in the dissolved (DP) and suspended particulate phase (SPM). Samples were collected prior to and after rainfall events to ascertain the contribution of wet atmospheric deposition of PAH enrichment to the SML. The concentration ranges of summation operatorPAHs in the SML before rain and after wet deposition were 2.6-46.2 ngL(-1) and 4.3-278.0 ngL(-1), respectively, for the DP and 3.8-31.4 ngL(-1) and 12.8-1280 ngL(-1), respectively, for the SPM. Load factors (i.e. concentration after wet deposition relative to before wet deposition) of the atmospheric wet deposition for DP and SPM ranged from 1.4 to 42.9 and 1.2 to 337, respectively. This study provides the first data on PAH concentration, enrichment (i.e. concentration of PAHs in SML relative to subsurface water) and load factors in the SML before and after wet deposition to the ocean surface.

High wind speeds prevent formation of a distinct bacterioneuston community in the sea-surface microlayer.

The sea-surface microlayer (SML) at the boundary between atmosphere and hydrosphere represents a demanding habitat for bacteria. Wind speed is a crucial but poorly studied factor for its physical integrity. Increasing atmospheric burden of CO2, as suggested for future climate scenarios, may particularly act on this habitat at the air-sea interface. We investigated the effect of increasing wind speeds and different pCO2 levels on SML microbial communities in a wind-wave tunnel, which offered the advantage of low spatial and temporal variability. We found that enrichment of bacteria in the SML occurred solely at a U10 wind speed of ≤5.6 m s-1 in the tunnel and ≤4.1 m s-1 in the Baltic Sea. High pCO2 levels further intensified the bacterial enrichment in the SML during low wind speed. In addition, low wind speed and pCO2 induced the formation of a distinctive bacterial community as revealed by 16S rRNA gene fingerprints and influenced the presence or absence of individual taxonomic units within the SML. We conclude that physical stability of the SML below a system-specific wind speed threshold induces specific bacterial communities in the SML entailing strong implications for ecosystem functioning by wind-driven impacts on habitat properties, gas exchange and matter cycling processes.

The role of the sea-surface microlayer in the air-sea gas exchange of organochlorine compounds.

Simultaneous measurements of organochlorine compounds (OCs) in seawater, the sea-surface microlayer and the atmosphere were conducted in June-July 2004 in the coastal marine environment of Singapore. Together, these measurements represent the first data on the flux of OCs between the ocean and atmosphere reported in the scientific literature that take into account the implication of the sea surface microlayer (SML) as a controlling boundary layer for the exchange of OCs. The average fluxes of SigmaPCBs and SigmaHCHs were 127.5 and -32.8 ng m(-2) day(-1) respectively using a modified two-layer model (negative flux indicates adsorption by the ocean). The average fluxes using a conventional approach, ignoring the SML as boundary layer (classical two-layer model), were 67.2 and -43.1 ng m(-2) day(-1) for SigmaPCBs and SigmaHCHs, respectively. However, the maximum difference in the flux calculation between the two approaches was up to 15-fold for individual compounds at high enrichment in the SML. It is shown that the SML plays an important role in the control of air-sea gas exchange of OCs, particular under a low prevailing wind regime and with an enrichment of OCs in the SML. The physical and chemical properties of OCs are critical factors in the control of the air-sea gas exchange process, and the effect of the SML on this process is more significant for more hydrophobic OCs.

Distribution of organochlorine compounds in the sea-surface microlayer, water column and sediment of Singapore's coastal environment.

Hexachlorocyclohexanes (HCHs), dichlorodiphenylethanes (DDTs) and 38 PCB congeners were determined in the water column (sea-surface microlayer, subsurface, mid-depth and bottom water) and sediments from Singapore's coastal environment. The concentration ranges for summationHCHs, summationDDTs and summationPCBs in the seawater dissolved phase (DP) were 101-6110 (mean 1833), <5-405 (mean 76) and 60-6979 (mean 1611)pg/l, respectively. The concentration ranges for summationHCHs, summationDDTs and summationPCBs in the suspended particulate matter (SPM) were 26-2395 (mean 243), <5-124 (mean 19) and 38-3793 (mean 715) pg/l, respectively. Concentration levels in sediments ranged between 521 and 1758 (mean 1094), 50 and 290 (mean 88) and 339 and 1356 (mean 858) pg/g for summationHCHs, summationDDTs and summationPCBs, respectively. It was shown that the interfaces of the sea-surface microlayer (SML) and near bottom water are important compartments for the distribution of organochlorine compounds (OCs) in the water column. In comparison with data from China, the concentration levels in the water column and sediments of Singapore can be considered as low, but the reported levels were higher compared to available data from Europe.

Occurrence and distribution of polybrominated diphenyl ethers (PBDEs) in the dissolved and suspended phases of the sea-surface microlayer and seawater in Hong Kong, China.

This study reports the first data on the concentration and distribution of polybrominated diphenyl ethers (PBDEs) in the sea-surface microlayer (SML), and their enrichment relative to bulk seawater, for coastal waters in the marine environment of Hong Kong, China. Samples were collected in March 2005 at five sample locations and analysed for eight congeners of primary interest, i.e. BDE 28, 47, 99, 100, 153, 156, 183 and 209. Concentration ranges of summation operatorPBDE in the dissolved phase (DP, defined as sum of truly dissolved and colloidal phase) and suspended particulate matter (SPM) of seawater were 31.1-118.7 pg/l (mean 70.7 pg/l), and 25.7-32.5 pg/l (mean 28.1 pg/l), respectively. Concentrations in the SML were generally higher by factor of 1.3-3.6 in the DP (concentration range from 40.2 to 228.2 pg/l, mean 149.2 pg/l) and by 0.3-2.1 in the SPM (concentration range 8.1-69.1 pg/l, mean 38.2 pg/l). Concentrations of PBDEs were general low and below detection limits in samples of an oceanic character and highest in the sheltered waters of Victoria Harbour. The congeners BDE 28, 47, 100 and 183 were most abundant, where BDE 209 was detected only in trace amounts. It is suggested that Hong Kong's marine waters show relatively low levels of PBDE contamination, and these compounds may originate from the disposal of electronic waste in southern China, as well as untreated discharge of wastewater locally.

Distribution of organochlorines in the dissolved and suspended phase of the sea-surface microlayer and seawater in Hong Kong, China.

Polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) were measured in the dissolved and suspended particulate phase in the sea-surface microlayer (SML) and subsurface water (SSW) collected from Hong Kong's coastal environment. The concentration ranges (pg/L) for summation sigmaHCHs, summation sigmaDDTs and summation sigmaPCBs in the SSW dissolved phase (DP i.e. sum of truly dissolved and colloidal phase) were 409-940 (mean 602), 774-5583 (mean 1908) and 266-433 (mean 278), respectively. The concentration ranges (pg/L) for summation sigmaHCHs, summation sigmaDDTs and summation sigmaPCBs in SSW suspended particulate matter (SPM) were <5-85 (mean 59), 358-1369 (mean 787) and 85.6-273 (mean 172), respectively. The enrichment factor of PCBs and OCPs in the SML varied between 1.1 and 4.5 for the DP, and 0.4-8.2 for the SPM. The distribution of contaminants between DP and SPM in both the SML and SSW indicates that particulate matter plays an important role in the distribution and fate of DDTs and PCBs, but not for HCH isomers. The Pearl River Estuary is likely to be a major source of contaminants transported to Hong Kong.