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Plastic pellets and microbes are important constitutes in sediment, but the significance of microbes colonizing on plastic pellets to the environmental fate and transport of organic contaminants has not been adequately recognized and assessed. To address this issue, low-density polyethylene (LDPE), polyoxymethylene (POM) and polypropylene (PP) slices were preloaded with dichlorodiphenyltrichloroethanes (DDTs), polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) and incubated in abiotic and biotic sediment microcosms. Images from scanning electron microscope, Lysogeny Broth agar plates and confocal laser scanning microscope indicated that all polymer slices incubated in biotic sediments were colonized by microorganisms, particularly the LDPE slices. The occurrence of biofilms induced higher dissipation rates of DDTs and PAHs from the LDPE slice surfaces incubated in the biotic sediments than in the abiotic sediments. Plastic colonization on LDPE slice surfaces enhanced the biotransformation of DDT and some PAHs in both marine and river sediments, but had little impact on PCBs. By comparison, PP and POM with unique properties were shown to exert different impacts on the physical and microbial activities as compared to LDPE. These results clearly demonstrated that the significance of polymer surface affiliated microbes to the environmental fate and behavior of organic contaminants should be recognized. [ABSTRACT FROM AUTHOR]

A letter to the editor is presented that comments on the article “Global Aquatic Passive Sampling (AQUA-GAPS): Using Passive Samplers to Monitor POPs in the Waters of the World,” by R. Lohmann and D. Muir in a 2010 issue.

Marine antibiofouling using low-amplitude electric pulses (EP) is an energy-efficient and eco-friendly approach, but potential mechanisms for preventing biofouling remain unclear. In the present study, the 3D adhesion dynamics of a model microorganism─ Pseudomonas aeruginosa (PAO1)─under low-amplitude cathodic EP were examined as a function of applying voltage and its duration ( t d ). The results demonstrated that adhered bacteria escaped from the electrode surface even when EP was removed. The escaped bacteria ratio, induction period of escape, and duration of the detachment were influenced profoundly by EP amplitude but slightly by t d when t d ≥ 5 min. The acceleration of escaped PAO1 from the surface indicated that their flagellar motor was powered by EP. Particularly, EP enabled swimming bacteria to have adaptive motions that were sustainable and regulated by the gene rsmA . As a result, they had less accumulation near the surface. The propulsion of adhered bacteria and adaptive escape of swimming bacteria were enhanced in response to low-amplitude EP. Hence, low-amplitude and short-duration EP is promising for sustainable antibiofouling applications.

Dermal absorption of gaseous chemicals is an important contributor to increased health risk and has yet to be adequately addressed due to the lack of available sampling techniques. In the present study, a novel personal passive sampler consisting of a housing (embracing a polydimethylsiloxane (PDMS) disk as the sorbent phase, a membrane filter, and a stainless-steel mesh) and a watchband (traditional wristband) was constructed and used to characterize gaseous phthalates (PAEs) near the air-skin interface. In a real-life setting, the utility of the passive sampler was validated by comparing the composition profiles of PAEs in the PDMS disks and in active samples and watchbands. The compositions of PAEs were consistent in disks and gaseous constituents from ambient air, with low-molecular-weight (<306 g mol -1 ) PAEs accounting for 87-100% and approximately 100%, respectively. Appreciable amounts of diisononyl phthalate, diisodecyl phthalate, dinonyl phthalate, and skin lipid (e.g., squalene) were detected in watchbands but not in disks. Apparently, the passive sampler can prevent particles and skin-related chemicals from adhering to the disk and collect gaseous PAEs only. The vast majority of PAEs in watchbands was associated with nongaseous constituents. The present study demonstrated that the sampling strategy is a key factor in exposure assessment.

Environmental tobacco smoke (ETS) is known to pose potential risk to human health, but the effects of tar level remain to be clarified. In the present study, ETS samples from two cigarette types with different tar levels in a 72.5 m 3 room were collected for measurement of 16 polycyclic aromatic hydrocarbons (PAHs). Urine samples of volunteers participating in smoking events were collected and analyzed for eight hydroxyl-PAHs. The concentrations, compositions, and particle size distribution patterns of PAHs from higher-tar and lower-tar cigarettes were similar, while the emission factors of PAHs from higher-tar cigarettes were lower than those from lower-tar cigarettes. Furthermore, the change in the concentrations of PAH metabolites in urine samples before and after smoking was not attributed to tar level. Assuming that a single cigarette was smoked in a 100 m 3 room, the estimated average inhalation cancer risks for different age groups from exposure to PAHs in ETS were below 1.0 × 10 -6 , but potential risks should not be overlooked, especially considering that only inhaled particle-bound PAHs in ETS were included in this assessment. Apparently, reduced tar levels would not necessarily lead to lowered risk of exposure to PAHs. Kicking the habit is perhaps the best choice to minimize any potential health risk.

Assessment of surface water pollution by organic pollutants is a top priority in many parts of the world, as it provides critical information for implementing effective measures to ensure drinking water safety. This is particularly important in China, where insufficient data of national scale have been acquired on the occurrence of any organic pollutants in the country's water bodies. To fill the knowledge gap, we employed passive samplers to survey polycyclic aromatic hydrocarbons (PAHs) in 42 freshwaters throughout the country. The dissolved Σ 24 PAH concentrations ranged from 0.28 to 538 ng L -1 , with the highest and lowest values obtained in Southern Lake in Wuhan and in the Nam Co Lake in Tibet, respectively. Average Σ 24 PAH concentrations in West, Central, and East China correlated well with the population densities in these regions. The composition profiles of PAHs showed a mixed PAH source of coal combustion, fossil fuel combustion, and oil spills. In addition, all dissolved PAH concentrations were below the water guidelines developed by the U.S. Environmental Protection Agency, the European Union, and the Canadian government, except for anthracene in Southern Lake. Our results also demonstrated the feasibility of establishing a global network of monitoring organic pollutants in the aquatic environment with passive sampling techniques.

The present study examined the bioacessibility of DDTs and PBDEs in cooked fish (yellow grouper; Epinephelus awoara) with and without heating using the colon extended physiologically based extraction test. The bioaccessibility of DDTs and PBDEs increased from 60 and 26% in raw fish to 83 and 63%, respectively, after the addition of oil to raw fish. However, they decreased from 83 to 66% and from 63 to 40%, respectively, when oil-added fish were cooked. Human health risk assessment based on bioaccessible concentrations of DDTs and PBDEs in fish showed that the maximum allowable daily fish consumption rates decreased from 25, 59, and 86 g day -1 to 22, 53, and 77 g day -1 for children, youths, and adults, respectively, after fish were cooked with oil. These findings indicated that the significance of cooking oil to the bioaccessibility of DDTs and PBDEs in food should be considered in assessments of human health risk.

Organic contaminants, in particular persistent organic pollutants (POPs), adversely affect water quality and aquatic food webs across the globe. As of now, there is no globally consistent information available on concentrations of dissolved POPs in water bodies. The advance of passive sampling techniques has made it possible to establish a global monitoring program for these compounds in the waters of the world, which we call the Aquatic Global Passive Sampling (AQUA-GAPS) network. A recent expert meeting discussed the background, motivations, and strategic approaches of AQUA-GAPS, and its implementation as a network of networks for monitoring organic contaminants (e.g., POPs and others contaminants of concern). Initially, AQUA-GAPS will demonstrate its operating principle via two proof-of-concept studies focused on the detection of legacy and emerging POPs in freshwater and coastal marine sites using both polyethylene and silicone passive samplers. AQUA-GAPS is set up as a decentralized network, which is open to other participants from around the world to participate in deployments and to initiate new studies. In particular, participants are sought to initiate deployments and studies investigating the presence of legacy and emerging POPs in Africa, Central, and South America.

Skin absorption of gaseous organic contaminants is an important and relevant mechanism in human exposure to such contaminants, but has not been adequately examined. This article demonstrates that dermal uptake from airborne contaminants could be recognized as a significant exposure route for local residents subjecting to combustion fume from e-waste recycling activities. It is particularly true for organic pollutants which have high dermal penetration rates and large skin-air partition coefficients, such as low molecular weight plasticizers and flame retardants.

Barbecuing or charcoal-grilling has become part of popular outdoor recreational activities nowadays; however, potential human health hazards through outdoor exposure to barbecue fumes have yet to be adequately quantified. To fill this knowledge gap, atmospheric size-fractioned particle and gaseous samples were collected near an outdoor barbecuing vendor stall (along with charcoal-grilled food items) in Xinjiang of Northwest China with a 10-stage micro-orifice uniform deposit impactor and a polyurethane foam (PUF) sampler and were analyzed for particulate matter and polycyclic aromatic hydrocarbons (PAHs). Exposure to PAHs through inhalation and dermal contact by adult consumers who spent 1 h per day near a charcoal-grilling vendor for a normal meal (lunch or dinner) amounted to a BaP equivalent (BaPeq) dosage of 3.0-77 ng day(-1) (inhalation: 2.8-27 ng day(-1) of BaPeq; dermal contact: 0.2-50 ng day(-1) of BaPeq), comparable to those (22-220 ng day(-1) of BaPeq) from consumer exposure through the consumption of charcoal-grilled meat, assumed to be at the upper limit of 50-150 g. In addition, the potential health risk was in the range of 3.1 × 10(-10) to 1.4 × 10(-4) for people of different age groups with inhalation and dermal contact exposure to PAHs once a day, with a 95% confidence interval (7.2 × 10(-9) to 1.2 × 10(-5)) comparable to the lower limit of the potential cancer risk range (1 × 10(-6) to 1 × 10(-4)). Sensitivity analyses indicated that the area of dermal contact with gaseous contaminants is a critical parameter for risk assessment. These results indicated that outdoor exposure to barbecue fumes (particularly dermal contact) may have become a significant but largely neglected source of health hazards to the general population and should be well-recognized.

Size distribution of particles in part dictates the environmental behavior of particle-bound organic pollutants in the atmosphere. The present study was conducted to examine the potential mechanisms responsible for the distribution of organic pollutants in size fractionated particles and their environmental implications, using an e-waste recycling zone in South China as a case study. Size-fractionated atmospheric particles were collected at the heights of 1.5, 5, and 20 m near two residential apartments and analyzed for polybrominated diphenyl ethers (PBDEs). The concentrations of particle-bound ΣPBDE (sum of 18 PBDE congeners) were significantly greater at 5 and 20 m than those at 1.5 m. The size-fractionated distributions of airborne ΣPBDE displayed trimodal peaks in 0.10–0.18, 1.8–3.2, and 10–18 μm at 1.5 m but only an unimodal peak in 1.0–1.8 μm at 20 m height. Emission sources, resuspension of dust and soil, and volatility of PBDEs were important factors influencing the size distribution of particle-bound PBDEs. The dry deposition fluxes of particle-bound PBDE estimated from the measured data in the present study were approximately twice the estimated wet deposition fluxes, with a total deposition flux of 3000 ng m(–2) d(–1). The relative contributions of particles to dry and wet deposition fluxes were also size-dependent, e.g., coarse (aerodynamic diameters (Dp) > 1.8 μm) and fine (Dp < 1.8 μm) particles dominated the dry and wet deposition fluxes of PBDEs, respectively.

Wet deposition is an effective and important mechanism for removal of atmospheric pollutants, particularly in urban regions. To examine the effectiveness of natural and anthropogenic factors in such removal mechanisms, we conducted a study in Guangzhou, a mega metropolitan center in South China. Rainwater and dry particle deposition samples were simultaneously collected from Guangzhou during the entire year of 2010, and analyzed for polybrominated diphenyl ethers (PBDEs), a group of pollutants mainly derived from industrial and household consumer products. Concentrations of ΣPBDE (sum of the 21 congeners of PBDEs) and BDE-209 in wet deposition samples ranged from 0.11 to 640 (average: 23 ± 36 ng L(-1)) and 0.071 to 420 (average: 20 ± 31 ng L(-1)), respectively. Assessed by conditional inference tree, particulate matter was recognized as the most important factor controlling concentration levels of PBDEs. The combined wet and dry deposition flux of ΣPBDE (1.4 (± 1.2) × 10(4) ng m(-2) quarter(-1)) in the first quarter of 2010 was not significantly different from that (1.3 (± 0.46) × 10(4) ng m(-2) quarter(-1)) in the fourth quarter, indicating that source control measures implemented by local governments for the 16th Asian Games and 10th Asian Para Games (held in November and December 2010, respectively) were ineffective in reducing the loadings of atmospheric PBDEs. In addition, the lower removal efficiency of ΣPBDE was found in the fourth quarter compared to other quarters. This result suggested that rain interventions conducted to maintain clear weather conditions for the Asian Games turned out to lower the efficacy for removal of PBDEs by wet deposition.

Many cases of severe environmental contamination arise from historical episodes, where recalcitrant contaminants have resided in the environment for a prolonged time, leading to potentially decreased bioavailability. Use of bioavailable concentrations over bulk chemical levels improves risk assessment and may play a critical role in determining the need for remediation or assessing the effectiveness of risk mitigation operations. In this study, we applied the principle of isotope dilution to quantify bioaccessibility of legacy contaminants DDT and PCBs in marine sediments from a Superfund site. After addition of 13C or deuterated analogues to a sediment sample, the isotope dilution reached a steady state within 24 h of mixing. At the steady state, the accessible fraction (E) derived by the isotope dilution method (IDM) ranged from 0.28 to 0.89 and was substantially smaller than 1 for most compounds, indicating reduced availability of the extensively aged residues. A strong linear relationship (R2=0.86) was found between E and the sum of rapid (Fr) and slow (Fs) desorption fractions determined by sequential Tenax desorption. The IDM-derived accessible concentration (Ce) was further shown to correlate closely with tissue residue in the marine benthic polychaete Neanthes arenaceodentata exposed in the same sediments. As shown in this study, the IDM approach involves only a few simple steps and may be readily adopted in laboratories equipped with mass spectrometers. This novel method is expected to be especially useful for historically contaminated sediments or soils, for which contaminant bioavailability may have changed significantly due to aging and other sequestration processes.

To examine the impacts of urbanization and industrialization on the coastal environment, sediment samples were collected from an urbanized coastal zone (i.e., Daya Bay and Hong Kong waters of South China) and analyzed for 20 polybrominated diphenyl ethers (PBDEs) and 10 alternative halogenated flame retardants (AHFRs). The sum concentration of PBDEs was in the range of 1.7-55 (mean: 17) ng g(-1), suggesting a moderate pollution level compared to the global range. The higher fractions of AHFRs (i.e., TBB+TBPH, BTBPE and DBDPE) than those of legacy PBDEs (i.e., penta-BDE, octa-BDE and deca-BDE) corresponded with the phasing out of PBDEs and increasing demand for AHFRs. Heavy contamination occurred at the estuary of Dan'ao River flowing through the Daya Bay Economic Zone, home to a variety of petrochemicals and electronics manufacturing facilities. The concentrations of HFRs in surface sediments of Hong Kong were the highest in Victoria Harbor, which receives around 1.4 million tons of primarily treated sewage daily, and a good relationship (r(2) = 0.80; p < 0.0001) between the HFR concentration and population density in each council district was observed, highlighting the effect of urbanization. Moreover, the AHFR concentrations were significantly correlated (r(2) > 0.73; p < 0.05) with the production volume of electronic devices, production value of electronic industries and population size, demonstrating the importance of industrializing and urbanizing processes in dictating the historical input patterns of AHFRs.

Inhalation of pollutants is an important exposure route for causing human health hazards, and inhalation exposure assessment must take into account particle size distribution because particle-bound pollutants are size-dependent. Such information is scarce, particularly for residents dwelling within e-waste recycling zones where abundant atmospheric halogenated flame retardants (HFRs) commonly used in electronic/electrical devices have been widely reported. Atmospheric size-fractioned particle samples were collected using a 10-stage Micro-Orifice Uniform Deposit Impactor from an e-waste recycling zone in South China. The deposition efficiencies and fluxes of size-fractioned HFRs including polybrominated diphenyl ethers (PBDEs), alternative brominated flame retardants, and Dechlorane Plus in the human respiratory tract were estimated using the International Commission on Radiological Protection deposition model. The majority of HFRs was found to deposit in the head airways, with coarse particles (aerodynamic diameter (Dp) > 1.8 μm) contributing the most (69-91%). Conversely, fine particles (Dp < 1.8 μm) were dominant in the alveolar region (62-80%). The inhalation intake of PBDEs within the e-waste recycling zone was 44 ng/d (95% confidence interval (CI): 30-65 ng/d), close to those through food consumption in non-e-waste recycling regions. The estimated total hazard quotient of particle-bound HFRs was 5.6 × 10(-4) (95% CI: 3.8 × 10(-4)-8.8 × 10(-4)). In addition, incremental lifetime cancer risk induced by BDE-209 was 1.36 × 10(-10) (95% CI: 7.3 × 10(-11)-2.3 × 10(-10)), much lower than the Safe Acceptable Range (1.0 × 10(-6)-1.0 × 10(-4)) established by the United States Environmental Protection Agency. These results indicate that the potential health risk from inhalation exposure to particle-bound HFRs for residents dwelling in the e-waste recycling zone was low.

Molecular diffusion across the sediment-water interface, as one of the key geochemical processes, dictates whether a sediment is a source or sink of chemicals, providing useful data in designing remedial actions. Despite ample previous efforts in quantifying sediment-water diffusion fluxes, the resulting methods are largely unsatisfactory. Herein, we introduce a novel passive sampling device capable of measuring vertical profiles of chemical concentrations near the sediment-water interface, from which diffusion fluxes can be calculated based on a model that we developed. In laboratory testing, diffusion fluxes (0.032-310 ng m(-2) d(-1)) of dichlorodiphenyltrichloroethane and its metabolites obtained from the present sampling device were consistent with those (0.38-610 ng m(-2) d(-1)) determined by using a conventional active sampling method, solid-phase extraction/liquid-liquid extraction. Field deployment of the sampling device yielded individual diffusion fluxes of p,p'-DDD, p,p'-DDE, p,p'-DDMU, o,p'-DDMU, p,p'-DDNU, and p,p'-DBP in the range of 5.9-150 ng m(-2) d(-1), which were comparable to those (5.5-85 ng m(-2) d(-1)) obtained with a benthic chamber. Moreover, diffusion fluxes of p,p'-DDT and o,p'-DDT obtained with the sampling device were negative; i.e., the sediment is acting as a sink for these chemicals, while that could not be found using the benthic chamber. Thus, the passive sampling device can provide better information about the movement of chemicals through the sediment and overlying water for the choice of remedial strategies.

In situ measurements of hydrophobic organic chemicals in sediment porewater, a central component in assessing the bioavailability and mobility of chemicals in sediment, have been scarce. Here, we introduce a multisection passive sampler with low-density polyethylene (LDPE) as the sorbent phase, which is appropriate for measuring vertical concentration profiles of chemicals in sediment porewater. This sampler is composed of a series of identical sampling cells insulated with seclusion rings. In each section, sorption of chemicals into LDPE is diffusion-controlled through the water layer separated from the sediment by a glass fiber filtration membrane and a porous stainless steel shield. Pilot laboratory testing indicated that the sampler can roughly determine the porewater concentrations of 1,1-dichloro-2,2-bis-(chlorophenyl)ethane (p,p'-DDD) and 1,1-dichloro-2,2-bis-(chlorophenyl)ethylene (p,p'-DDE), comparable to those yielded through centrifugation/liquid-liquid extraction, a conventional technique for sampling sediment porewater. Field deployment of the sampler was performed in an urbanized coastal region to measure the depth profiles of dichlorodiphenyltrichloroethane and its metabolites in sediment porewater. Sampling rate-calibrated and performance reference compound-calibrated concentrations were calculated, which were consistent with those obtained by the centrifugation/liquid-liquid extraction method. These results verified the utility of the sampler for measuring depth profiles of sediment porewater chemicals.

Although the production and use of dichlorodiphenyltrichloroethane (DDT), a legacy component of persistent organic pollutants, have been highly restricted worldwide, the environmental fate of DDT has remained a great concern as it is not only ubiquitous and bioaccumulative but can also be degraded to a series of metabolites that may be more hazardous ecologically. The present study, taking advantage of the abundant levels of DDT and its metabolites in a subtropical coastal region of China, investigated into the degradation pathways of DDT in natural coastal sediment. Sediment profiles indicated that degradation of 1,1,1-trichloro-2,2-bis-(p-chlorophenyl)ethane (p,p'-DDT) to 1,1-dichloro-2,2-bis-(p-chlorophenyl)ethane (p,p'-DDD) mainly occurred in sediment of the top 20 cm layer. 1,1-dichloro-2,2-bis-(p-chlorophenyl)ethylene (p,p'-DDE), aerobically transformed from p,p'-DDT prior to sedimentation, was likely to degrade to 1-chloro-2,2-bis-(p-chlorophenyl)ethylene (p,p'-DDMU) which was further converted to 2,2-bis(p-chlorophenyl)ethylene (p,p'-DDNU). In addition, p,p'-DDNU could be transformed to 2,2-bis(p-chlorophenyl)ethane (p,p'-DDNS) and other high-order metabolites. On the other hand, the conversions of p,p'-DDD to p,p'-DDMU and 1-chloro-2,2-bis-(p-chlorophenyl)ethane (p,p'-DDMS) to p,p'-DDNU were deemed slow in anaerobic sediment. Therefore, the present study confirmed all the degradation pathways involving reductive dechlorination and p,p'-DDE being a more important precursor for p,p'-DDMU than p,p'-DDD in anaerobic sediment, as proposed previously. On the other hand, the present study suggested that p,p'-DDMU instead of p,p'-DDMS was more likely the precursor for formation of high-order metabolites. Based on the current assessments, use of (DDD+DDE)/DDTs to indicate whether there is fresh DDT input may lead to large uncertainties if the concentrations of high-order metabolites are not negligible. Similarly, ecological risk assessment associated with DDT should be conducted with consideration of high-order DDT metabolites.