Fate Of Persistent Organic Pollutants Research Articles

Unveiling the Mechanism and Kinetics of Pollutant Attenuation by Free Radicals Triggered from Goethite in Water Distribution Systems.

Investigating the fate of persistent organic pollutants in water distribution systems (WDSs) is of great significance for preventing human health risks. The role of iron corrosion scales in the migration and transformation of organics in such systems remains unclear. Herein, we determined that hydroxyl (•OH), chlorine, and chlorine oxide radicals are generated by Fenton-like reactions due to the coexistence of oxygen vacancy-related Fe(II) on goethite (a major constituent of iron corrosion scales) and hypochlorous acid (HClO, the main reactive chlorine species of residual chlorine at pH ∼ 7.0). •OH contributed mostly to the decomposition of atrazine (ATZ, model compound) more than other radicals, producing a series of relatively low-toxicity small molecular intermediates. A simplified kinetic model consisting of mass transfer of ATZ and HClO, •OH generation, and ATZ oxidation by •OH on the goethite surface was developed to simulate iron corrosion scale-triggered residual chlorine oxidation of organic compounds in a WDS. The model was validated by comparing the fitting results to the experimental data. Moreover, the model was comprehensively applicable to cases in which various inorganic ions (Ca2+, Na+, HCO3-, and SO42-) and natural organic matter were present. With further optimization, the model may be employed to predict the migration and accumulation of persistent organic pollutants under real environmental conditions in the WDSs.

Dataset of Contamination (2009–2022) Legacy Contaminants (PCB and DDT) in Zooplankton of Lake Maggiore (CIPAIS, International Commission for the Protection of Italian-Swiss Waters)

In this paper, we describe a 13-year (2009–2022) dataset of legacy POP concentrations (DDTtot and sumPCB14 from 2016 isomers and congeners concentrations are also reported) in the planktonic crustaceans of Lake Maggiore (≥450 µm size fraction). The data were collected in the framework of a monitoring program finalized to assess the presence of pollutants in the lake biota, including zooplankton organisms directly preyed by fish. The data report both concentration of DDTtot and sumPCB14 in the zooplankton and the standing stock density and biomass of the population in each season. The dataset allows for detecting changes in the concentration over the long term and within a year, thus providing evidence for the seasonal and the plurennial variations in the presence of these pollutants in the lake. They also provide a basis for further studies aimed at modeling paths and the fate of persistent organic pollutants, for which the amount of toxicants stocked in the zooplankton compartment linked to fish is a crucial estimate.

A data-driven analysis of global research trends on dirty-dozen persistent organic pollutants.

The occurrence, distribution, and fate of persistent organic pollutants (POPs) have been extensively studied worldwide; however, the patterns and dynamics of scientific publications on POPs are still unclear. In this study, the research trends on dirty dozen POPs, which are identified under the Stockholm Convention (SC) for immediate action were investigated and evaluated in a broad context to obtain up-to-date information. For this purpose, bibliometric analysis was carried out between 1945 and 2021 using the Web of Science (WoS) database. A total of 197,029 publications were analyzed. "Environmental Sciences" was the most popular research category and the USA was the leading country in dirty dozen POPs studies. The research hotspots are related to the most used keywords such as "Polychlorinated Biphenyls", "Dioxin" and "Persistent Organic Pollutants". In the evaluation of keyword clusters with highlighted research points, 7 clusters were obtained from the publications, which are related to the chemical properties, synthesis, structures, health effects, and analysis methods of dirty dozen POPs. The number of publications and, accordingly, the scientific interest in dirty dozen POPs listed under the SC has not reached equilibrium and continues regardless of the level of development of countries in the world.

Terrestrial inputs govern spatial distribution of polychlorinated biphenyls (PCBs) and hexachlorobenzene (HCB) in an Arctic fjord system (Isfjorden, Svalbard).

Considerable amounts of previously deposited persistent organic pollutants (POPs) are stored in the Arctic cryosphere. Transport of freshwater and terrestrial material to the Arctic Ocean is increasing due to ongoing climate change and the impact this has on POPs in marine receiving systems is unknown This study has investigated how secondary sources of POPs from land influence the occurrence and fate of POPs in an Arctic coastal marine system. Passive sampling of water and sampling of riverine suspended particulate matter (SPM) and marine sediments for analysis of polychlorinated biphenyls (PCBs) and hexachlorobenzene (HCB) was carried out in rivers and their receiving fjords in Isfjorden system in Svalbard. Riverine SPM had low contaminant concentrations (<level of detection-28pg/g dw ΣPCB14, 16-100pg/g dw HCB) compared to outer marine sediments 630-880pg/g dw ΣPCB14, 530-770pg/g dw HCB). There was a strong spatial gradient in sediment PCB and HCB concentrations with lowest concentrations in river estuaries and in front of marine-terminating glaciers and increasing concentrations toward the outer fjord. This suggests that rather than leading to increased concentrations, inputs of SPM from land lead to a dilution of contaminant concentrations in nearshore sediments. Preliminary estimates of SPM:water activity ratios suggest that terrestrial particles (with low contaminant concentrations) may have the potential to act as sorbents of dissolved contaminants in the coastal water column, with implications for bioavailability of POPs to the marine food web. There is concern that ongoing increases in fluxes of freshwater, sediments and associated terrestrial material (including contaminants) from land to the Arctic Ocean will lead to increased mobilization and transport of POPs to coastal ecosystems. However, the results of this study indicate that on Svalbard, inputs from land may in fact have the opposite effect, leading to reduced concentrations in coastal sediments and waters.

Source emissions and climate change impacts on the multimedia transport and fate of persistent organic pollutants, Chaohu watershed, eastern China

Emission intensity and climate change control the transport flux and fate of persistent organic pollutants (POPs) in multiple environmental compartments. This study applied a multimedia model (BETR model) to explore alternations in the spatio-temporal trends of concentrations and transport flux of benzopyrene (BaP), phenanthrene (Phe), perfluorooctane sulfonates (PFOS) and polychlorinated biphenyls (PCBs) in the Chaohu watershed, located in the lower reaches of the Yangtze River, China in response to changes in source emissions and climate. The potential historic and future risks of these pollutants also were assessed. The results suggest that current trends in concentrations and transport were similar to that of their emissions between 2005 and 2018. During the next 100 years, temporal trends and spatial patterns were not predicted to change significantly, which is consistent with climate change. Based on sensitivity and correlation analyses, climate change had significant effects on multi-media concentrations and transport fluxes of BaP, Phe, PFOS and PCBs, and rainfall intensity was the predominant controlling factor. Risk quotients (RQs) of BaP and Phe-in soil increased from 0.42 to 0.95 and 0.06 to 0.35, respectively, from 2005 to 2090, indicating potential risks. The RQs of the other examined contaminants exhibited little potential risk in soil, water, or sediment. Based on spatial patterns, it was inferred that the ecosystem around Lake Chaohu is the most at risk. The study provides insights needed for local pollution control of POPs in the Chaohu watershed. In addition, the developed approach can be applied to other watersheds world-wide.

Role of low-latitude forests in modulating forest filter effect on a continental scale: Long-term simulation on PCB-153 in Chinese forests.

Forests are important compartments influencing the environmental fate of persistent organic pollutants (POPs). To illustrate the effect of forests on the regional cycle of POPs, a level IV fugacity fate and transport model coupled with a detailed dynamic-forest module was applied to simulate the long-term variations of PCB-153 in China, where forest coverage accounts for approximately one fifth of land area. In the scenarios with forests, atmospheric outflow from China was 69% of that in the scenario without forests due to the enhanced storage in soil, degradation, and leaching. Previous studies regarded high-latitude areas, such as the polar region and boreal forests, as environments capable of reducing mobility of PCB-153, and they act as sinks of POPs. This modeling result suggests that tropical and subtropical forests may also play a similar role despite high temperatures favoring volatilization. Unlike boreal forest, the low-latitude forests may reduce the overall lifetime of PCB-153 in China due to enhanced degradation in warmer and moist soils of the tropical and subtropical area. Given that approximately half of the global forests are located in tropical and subtropical regions, they can be important environments influencing the global geochemical cycle and distribution of POPs, hence deserving more scientific attention by modeling and empirical studies.

Do dissipation and transformation of γ-HCH and p,p'-DDT in soil respond to a proxy for climate change? Insights from a field study on the eastern Tibetan Plateau.

While the influence of climate change on the fate of persistent organic pollutants (POPs) is becoming a topic of global concern, it has yet to be demonstrated how POPs and their transformation products in soil respond to a changing climate at the local scale. We conducted a year-long field experiment with spiked soils to investigate the impact of climate on the dissipation of γ-hexachlorocyclohexane (γ-HCH) and p,p'-dichlorodiphenyltrichloroethane (p,p'-DDT) as well as the formation of their products. Four sites along an elevational gradient on the eastern Tibetan Plateau were selected to represent four scenarios ranging from a dry and cold to a warm and humid climate. Based on the measured concentrations of the two pesticides and their transformation products, we calculated the dissipation rates of γ-HCH and p,p'-DDT in soil using two biphasic kinetic models, and the formation rates of transformation products using a mid-point rectangular approximation method. The spiked γ-HCH generally showed the expected decrease in dissipation from soils with increasing altitudes, and therefore decreasing temperature and precipitation, whereas dissipation of p,p'-DDT was influenced more by photolysis and sequestration in soil. The formation rates of the primary products of γ-HCH (i.e. γ-HCH→PeCCH and γ-HCH→TeCCH) and p,p'-DDT (i.e. p,p'-DDT→p,p'-DDE and p,p'-DDT→p,p'-DDD) indicate that a warmer and wetter climate favors dechloroelimination (anaerobic biodegradation) over dehydrochlorination (aerobic biodegradation). The significantly longer dissipation half-lives of γ-HCH at the coldest site suggests that the fate of POPs in frozen regions (e.g. polar regions) needs more attention. Overall, the fate of more volatile chemicals (e.g. γ-HCH) might be more responsive to the climate change.

Polycyclic Aromatic Hydrocarbons in the North Atlantic Ocean and the Arctic Ocean: Spatial Distribution and Water Mass Transport

It is still not clear what role the oceanic transport plays in the fate of persistent organic pollutants (POPs) in the Arctic Ocean. The strong-stratified Arctic Ocean undergoes complex inputs and outputs of polycyclic aromatic hydrocarbons (PAHs) from the neighboring oceans and continents. To better understand PAHs’ transport processes and their contribution in high-latitude oceans, surface seawater, and water column samples were collected from the North Atlantic Ocean and the Arctic Ocean in 2012. The spatial distribution of dissolved PAHs (∑9PAH) in surface seawater showed an “Arctic Shelf > Atlantic Ocean > Arctic Basin” pattern, with a range of 0.3-10.2 ng L-1. Positive matrix factorization (PMF) modeling results suggested that vehicle emissions and biomass combustion were the major PAHs sources in the surface seawater. According to principal component analysis (PCA), PAHs in different water masses showed unique profiles indicating their different origins. The net transport mass flux of PAH individuals ranged from -4.4±1.7 to 53±39 tons/year to the Arctic Ocean, with a sum of 63±53 tons/year. The direct contribution of ocean currents was limited for PAHs transporting to the Arctic Ocean, but their role in modulating atmospheric POPs should be further considered.

Persistent organic pollutants in wood fiber\u2013contaminated sediments from the Baltic Sea

PurposeMany coastal areas in the Baltic Sea are contaminated with wood fiber and pollutants from pulp and paper industries. These anthropogenic, organic-rich, sediments (fiberbanks) have not been characterized and knowledge about their role as secondary sources for dispersal of persistent organic pollutants (POPs) is limited. Hence, the aim of this study was to elucidate the fate of POPs and the relationships between sorption (KD and KTOC), sediment type, and compound hydrophobicity (KOW) in fiber-contaminated sediments.Materials and methodsPaired sediment and pore water samples (n = 24 sites) from three fiber-contaminated areas, located in the Ångermanälven river estuary in northern Sweden, were analyzed for POPs (viz. PCBs, DDT, and HCB) in sediment types representing different fiber content (i.e., fiberbanks, fiber-rich sediments, and natural less fiber impacted sediments). The freely dissolved concentration in sediment pore water was determined by sediment-polyoxymethylene (POM) partitioning. Instrumental analysis was performed using gas chromatography coupled to a triple quadrupole mass spectrometer (GC-MS/MS).Results and discussionHigher levels of total organic carbon (TOC) were found in the fiberbank sediment (range 8.6–37%) than in fiber-rich sediment (range 2.0–6.5%) and more natural sediment (range 2.0–2.9%). The sediment concentrations of POPs (dry weight basis) were also found to be significantly (p < 0.05) elevated in fiberbanks compared to the other sediment types. The fraction of DDD (48–66% of Σ6DDX) was larger in fiberbanks than in the other sediment types, likely due to anoxic conditions favoring reductive dechlorination of DDT. When sediment levels were normalized to TOC, HCB displayed similar levels across sediment type, suggesting a more diffuse source pattern than for PCB and DDT. Although significantly higher sorption (KD) of POPs was observed in fiberbanks, pore water levels were still elevated due to high bulk concentrations.ConclusionsThis study shows that fiberbanks are coastal hot spots for POPs in the Baltic Sea and that the levels are of ecotoxicological concern. Although the POPs are more strongly sorbed (KD) to this type of organic rich sediment, the high pore water concentrations in fiberbanks compared to the other sediment types investigated show that the risk of contaminant dispersal via pore water is elevated for fiberbanks.

Chemical fate of persistent organic pollutants in the arctic: Evaluation of simplebox

Persistent organic pollutants (POPs) are of great concern for decades due to their persistence, bioaccumulation and long-range transport potential. Multimedia fate models are useful scientific and decision-support tools for predicting the chemical fate in the environment. The SimpleBox multimedia fate model (v4.0) was used in this study to estimate the impact of POP emissions from the European and North American mainland on POP contamination in the Arctic. The purpose of the study was to evaluate the performance of SimpleBox by comparing estimations to measurements. Model performance for the air compartment was reasonable as estimated concentrations were generally within a factor of five of measured concentrations. SimpleBox suggested higher POP concentrations in Arctic oceans than in temperate oceans, contrary to the few measured data. Discrepancies between estimations and measurements may be attributed to the variability in emission estimates and degradation rates of POPs, representativeness of monitoring data, and a missing snow and ice environmental compartment in SimpleBox. Emission rates and degradation rate constants were the most influential input parameters in SimpleBox based on sensitivity analysis. Suggestions for improvements of SimpleBox refining POP risk assessment are provided.

Prediction of octanol-air partition coefficients for PCBs at different ambient temperatures based on the solvation free energy and the dimer ratio.

Temperature-dependent octanol-air partition coefficients (KOA) are of great importance in assessing the environmental behavior and fate of persistent organic pollutants including polychlorinated biphenyls (PCBs). Due to the tremendous amounts of time, effort and cost needed for the experimental determination of KOA, it is desirable to develop a rapid and precise predictive method to estimate KOA just based on molecular structure. In the present study, a predictive model for log KOA of PCBs at ambient temperatures was developed based on the thermodynamic relationship between KOA and the solvation free energy from air to octanol (ΔGOA). For the calculation of ΔGOA of PCBs, the optimal combination of theoretical method and basis-set was identified to be HF/MIDI!6D for both geometry optimization and energy calculation. Dimer formation could affect the partition behavior and promote the apparent KOA values of PCBs. After taking the effect of dimer formation into account, the goodness-of-fit, predictive ability, and robustness of the predictive model were significantly improved. Apparent log KOA values of PCBs at different ambient temperatures ranging from 283.15 to 303.15 K were predicted. Compared with other reported models, the model developed in the present study had not only comparable goodness-of-fit and predictive ability, but also a universal application domain and the relative independency of experimental data. Therefore, the solvation free energy method could be a promising method for the prediction of KOA.

Mechanistic Insight into the Uptake and Fate of Persistent Organic Pollutants in Sea Ice.

The fate of persistent organic pollutants in sea ice is a poorly researched area and yet ice serves as an important habitat for organisms at the base of the marine foodweb. This study presents laboratory-controlled experiments to investigate the mechanisms governing the fate of organic contaminants in sea ice grown from artificial seawater. Sea ice formation was shown to result in the entrainment of chemicals from seawater, and concentration profiles in bulk ice generally showed the highest levels in both the upper (ice–atmosphere interface) and lower (ice–ocean interface) ice layers, suggesting their incorporation and distribution is influenced by brine advection. Results from a 1-D sea ice brine dynamics model supported this, but also indicated that other processes may be needed to accurately model low-polarity compounds in sea ice. This was reinforced by results from a melt experiment, which not only showed chemicals were more enriched in saltier brine, but also revealed that chemicals are released from sea ice at variable rates. We use our results to demonstrate the importance of processes related to the occurrence and movement of brine for controlling chemical fate in sea ice which provides a pathway for exposure to ice-associated biota at the base of the pelagic food web.

Fe(III)-citrate enhanced sunlight-driven photocatalysis of aqueous Carbamazepine

We investigated the effect of Fe(III)-citrate complexes on the photodegradation of Carbamazepine (CBZ) upon 365 nm irradiation in aqueous solution. A preliminary study of a {CBZ/Fe(III)-citrate} mixture in the dark and at room temperature showed no evidence of reaction. CBZ degradation efficiency depends on the pH of the medium, an effect attributed mainly to the speciation of Fe(III)-citrate. The influence of [CBZ] or [Fe(III)-citrate] on the kinetics of the reaction was studied. The reaction is biphasic, the first stage ends after ca. fifteen minutes and accounts for the major percentage of degradation. The presence of Fe(III)-citrate complex largely enhances the formation of Fe2+ and HO radicals; they form at the same rate at the beginning of the reaction. Increasing [O2] improved the degradation rate, and the use of i-PrOH as a scavenger confirmed the participation of HO in CBZ photodegradation. CBZ photodegradation was also studied under natural sunlight showing a degradation only slightly lower than under artificial light. HPLC/MS analysis confirmed 11% yield epoxycarbamazepine as the only reaction product observable with this technique after 180 min irradiation. An appropriate mechanism is proposed for CBZ transformation. CBZ phototransformation reached 65% at pH = 6.24, 87% at pH = 4.30 and ca. 100% at pH = 2.86 after 180 min upon 365 nm irradiation and the mineralization efficiency reaches 70% of TOC removal after 6 h of treatment. Our evidences show the epoxide photoproduct is just an intermediate that further reacts towards mineralization. This work highlights the important role of Fe(III)-carboxylate complexes may have on the fate of persistent organic pollutants in aquatic environments when irradiated with UV-A light.

Construction of the hydrological condition-persistent organic pollutants relationship in the Yangtze River Estuary

With anthropogenic activities, the persistent organic pollutants (POPs) accumulated in estuary has been notably concern but the influences of complex hydrodynamic conditions on the fate of POPs in estuary have not fully understood. In this study, the bottom velocity and the concentration of suspended sediment in the Yangtze River Estuary (YRE) were determined using the Acoustic Doppler Current Profiler (ADCP), while the concentration of three typical POPs with distinguishing properties, including polychlorinated biphenyls (PCBs), polycyclic aromatic hydrocarbons (PAHs), and organichlorine pesticides (OCPs), were determined simultaneously. Then three nonlinear equations were determined for identifying the hotspots of PCBs, OCPs and PAHs in the YRE. The results indicated the goodness-of-fitting of these three equations were satisfactory, indicating the bottom velocity and the suspended sediment level could be used as the reference factor of POPs. For the YRE, the north branch, the upstream of the north branch, and the mouth of the YRE are identified as the hotspots of PCBs, PAHs and OCPs, especially in the normal, flood and dry season, respectively. Simple structure and easy data availability make the results and methods presented in this paper to be easily used as a reference for POPs studies in other regions.

Potential effects of changes in climate and emissions on distribution and fate of perfluorooctane sulfonate in the Bohai Rim, China

Climate change and emissions rates of contaminants are expected to affect distribution and fate of Persistent Organic Pollutants (POPs) in the environment, however, studies on these combined factors are rare. In this study, Perfluorooctane Sulfonate (PFOS) is used as an example to assess how those two factors synthetically affect fate and disposition of POPs in the Bohai Rim of China by using the Berkeley-Trent-Urban-Rural (BETR-Urban-Rural) model. We set up three climate change scenarios and four emission scenarios to conduct the simulations. The results show that climate change could have significant effects on the transport and fate of PFOS mainly including advection, inter-compartmental transfer under the “worst case” emission scenario. For most grids, a remarkable decrease in concentrations of PFOS are predicted for fresh water and urban soil in the future, with precipitation and temperature being predominant factors, whilst for coastal water and rural soil, an increasing trend is predicted. Additionally, predicted sum of sources to the Bohai Sea increases greater than removals from the Bohai Sea in the future, adding evidence that concentrations of PFOS in coastal water will increase more in the future. Under scenarios of reduced emissions and climate change, concentrations of PFOS in each compartment decreased more rapidly over time. We suggest that assessment of future climate change impacts on fate of PFOS could take emission reductions into consideration.

Effect of extracellular polymeric substance components on the sorption behavior of 2,2′,4,4′-tetrabromodiphenyl ether to soils: Kinetics and isotherms

Microbial extracellular polymeric substances (EPS) and persistent organic pollutants (POPs) commonly exist in the soil environment. Currently, there is a knowledge gap regarding the effect of EPS on the fate of POPs in soil. In the present study, 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) was used as a model compound to investigate the effects of bovine serum albumin (BSA) and sodium alginate (SA) - mimicking the main components of EPS - on sorption of POPs to soils, through batch experiments. Irrespective of the concentration of BSA: the addition of BSA did enhance the sorption capacity of BDE-47 to soils, due to generation of more sorption sites. For SA, it increased the sorption capacity of BDE-47 at low BDE-47 concentrations, while the presence of SA negatively affected sorption of BDE-47 at high BDE-47 concentrations. The partition effect dominates the sorption of BDE-47 to soils, but after adding either BSA or SA, the sorption of BDE-47 to soils is dominated by surface sorption. Film diffusion and intra-particle diffusion were also involved in the sorption process with and without BSA or SA, with the latter being the rate-limiting step. The heterogeneous surface and nonlinear sorption behavior of BDE-47 to soils increased in the presence of either BSA or SA. The FTIR spectra indicated that the aromatic CC, H-bonds and OH groups may be involved in the sorption process. Therefore, BSA enhanced the retention of BDE-47 to soil, while SA's influence on BDE-47 sorption to soil depended on the concentration of BDE-47.

Distribution of persistent organic pollutants in aggregate fractions of a temperate forest and semi-rural soil

The fate of persistent organic pollutants (POPs) and their interactions with aggregates of forest soils are not completely understood. Our objectives here were to quantify the distribution of different POPs in water-stable aggregate fractions and to study their influence on soil organic carbon (Corg) content. Soil samples were taken from a forest-site, Gogerddan (G) and a semi-rural site, Hazelrigg (H) in Great Britain, from 0–2 and 2–5 cm and 0–4 and 8–12 cm soil depth, respectively. POPs analyzed were PAHs, PCBs, total DDT, PBDEs and HCB. The bulk soil analysis showed that the concentration of POPs was significantly higher (p ≤ 0.05) in forest site G than in semi-rural site H, particularly at the surface soil levels compared to the subsurface soil depths in both sites. Total concentrations of PCBs and PAHs of both sites were positively correlated with Corg contents. POPs concentrations and Corg, Nt contents of forest site G were significantly higher (p ≤ 0.05) in water-stable macro aggregates (>0.25, >1, >2 mm) than the micro aggregates (>0.053 mm). The POP concentrations of all aggregate fractions after normalizing to their respective Corg content were increased due higher contamination and strong sorption by Corg. These results showed a strong effect of Corg on the partitioning of organic pollutants to soil aggregate size fractions. The present study affirms the ecological significance of forest soils act as a potential sink of POPs. In summary, our results suggest that aggregate fractions may promote soil C storage and act as a potential POP sink in surface soil without increasing their concentration in the aggregate fraction of subsoil.

Using a passive air sampler to monitor air-soil exchange of organochlorine pesticides in the pasture of the central Tibetan Plateau.

Air-soil exchange is a key process controlling the fate of persistent organic pollutants (POPs). However, the "sink effect" of soil for POPs in Tibetan pasture has not been clear. In NamCo, in the central Tibetan Plateau (TP) where the land is covered by grass, a modified passive air sampler (PAS) (thickness: 2cm) was tested. Using the PAS, the atmospheric gaseous phase organochlorine pesticides (OCPs) at 11 heights from close-to-surface (2cm) to 200cm above ground, in summer and in winter, were measured. Concentrations of OCPs in summer were higher than those in winter. Both in summer and winter, atmospheric concentrations of OCPs decreased with decreasing height from 200 to 2cm, indicating that OCPs were being deposited from air to soil. Air deposition of OCPs was possibly driven by wind speed. Furthermore, based on air OCPs at 0-3cm near the surface, the interface exchange of OCPs between air and soil was studied by the fugacity method. The results showed that pastural soil in the TP was a "sink" of OCPs even in summer. The mean deposition fluxes of α-HCH, γ-HCH and o,p'-DDT were 0.72, 0.24 and 0.54pg/h/m2, respectively, and it was estimated that the level of these pollutants in the soil will double every 24, 66 and 206years, respectively. This study will contribute to the further understanding of global cycling of POPs in different land covers.

Levels, sources and chemical fate of persistent organic pollutants in the atmosphere and snow along the western Antarctic Peninsula

The Antarctic continent is among the most pristine regions; yet various organic contaminants have been measured there routinely. Air and snow samples were collected during the austral spring (October–November, 2010) along the western Antarctic Peninsula and analyzed for organochlorine pesticides (OCPs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) to assess the relative importance of long-range transport versus local primary or secondary emissions. Highest concentrations of PCBs, PBDEs and DDTs were observed in the glacier’s snow sample, highlighting the importance of melting glaciers as a possible secondary source of legacy pollutants to the Antarctic. In the atmosphere, contaminants were mainly found in the vapor phase (>65%). Hexachlorobenzene (33.6 pg/m3), PCBs (11.6 pg/m3), heptachlor (5.64 pg/m3), PBDEs (4.22 pg/m3) and cis-chlordane (2.43 pg/m3) were the most abundant contaminants. In contrast to other compounds, PBDEs seem to have originated from local sources, possibly the research station itself. Gas-particle partitioning for analytes were better predicted using the adsorption partitioning model than an octanol-based absorption approach. Diffusive flux calculations indicated that net deposition is the dominant pathway for PBDEs and chlordanes, whereas re-volatilization from snow (during melting or metamorphosis) was observed for PCBs and some OCPs.

Fate and transport of polychlorinated biphenyls (PCBs) in the River Thames catchment – Insights from a coupled multimedia fate and hydrobiogeochemical transport model

The fate of persistent organic pollutants (POPs) in riverine environments is strongly influenced by hydrology (including flooding) and fluxes of sediments and organic carbon. Coupling multimedia fate models (MMFMs) and hydrobiogeochemical transport models offers unique opportunities for understanding the environmental behaviour of POPs. While MMFMs are widely used for simulating the fate and transport of legacy and emerging pollutants, they use greatly simplified representations of climate, hydrology and biogeochemical processes. Using additional information about weather, river flows and water chemistry in hydrobiogeochemical transport models can lead to new insights about POP behaviour in rivers. As most riverine POPs are associated with suspended sediments (SS) or dissolved organic carbon (DOC), coupled models simulating SS and DOC can provide additional insights about POPs behaviour. Coupled simulations of river flow, DOC, SS and POP dynamics offer the possibility of improved predictions of contaminant fate and fluxes by leveraging the additional information in routine water quality time series. Here, we present an application of a daily time step dynamic coupled multimedia fate and hydrobiogeochemical transport model (The Integrated Catchment (INCA) Contaminants model) to simulate the behaviour of selected PCB congeners in the River Thames (UK). This is a follow-up to an earlier study where a Level III fugacity model was used to simulate PCB behaviour in the Thames. While coupled models are more complex to apply, we show that they can lead to much better representation of POPs dynamics. The present study shows the importance of accurate sediment and organic carbon simulations to successfully predict riverine PCB transport. Furthermore, it demonstrates the important impact of short-term weather variation on PCB movement through the environment. Specifically, it shows the consequences of the severe flooding, which occurred in early 2014 on sediment PCB concentrations in the River Thames.