Polycyclic Aromatic Hydrocarbons Fluxes Research Articles

Transport of polycyclic aromatic hydrocarbons in a highly vulnerable karst underground river system of southwest China.

The concentration and fluxes of polycyclic aromatic hydrocarbons (PAHs) were investigated in a karst underground river system in southwest China. Groundwater, particles, and sediments from underground river, topsoil, and surface water were monitored, allowing establishment of a conceptual model of PAH transport at the watershed scale. The results showed that PAHs could be transported from the surface to the subsurface through two migration pathways, which were slow-flowing water in the karst fissure and fast-flowing water in conduits. During rainfall events, increasing PAH levels (concentrations and fluxes) at the underground river exit indicated that hydrodynamic force could facilitate PAH transport. The PAHs in water were dominated by dissolved PAHs, accounting for 58.7% of total, especially in the freely dissolved phase, in which SPM-associated PAHs accounted for 41.3% of the total PAHs. Low molecular weight PAHs dominated transport and were mainly transported in dissolved form, whereas high molecular weight PAHs were dominated by SPM-associated transport during the rainfall events. A significantly positive correlation was observed between two-ring and three-ring freely dissolved PAHs and dissolved organic carbon (p < 0.01), respectively. Moreover, PAHs with four to five rings were relatively more abundant in the dissolved organic matter (DOM) associated phase than in the freely dissolved phase, suggesting a major role of DOM in their transport during rainfall events. The trend of PAH fluxes suggested that particle-facilitated transport was another dominant cause of PAH mobilization.

Pivotal Role of Snow Deposition and Melting Driving Fluxes of Polycyclic Aromatic Hydrocarbons at Coastal Livingston Island (Antarctica).

The atmosphere-land-ocean dynamics of semivolatile organic compounds in polar regions is poorly understood,also for the abundant and ubiquitous polycyclic aromatic hydrocarbons (PAHs). We report the concentrations and fluxes of PAHs in a polar coastal ecosystem (Livingston Island, Antarctica). From late spring (December 2014) to late summer (February 2015), we sampled air, snow, coastal seawater, plankton, and the fugacity in soils and snow. The concentrations of PAHs in seawater were low but increased during the austral summer. The PAH concentrations in snow were significantly higher than in coastal seawater. Soil-air fugacity ratios showed a net volatilization of PAH when soils were covered with lichens, and close to air-soil equilibrium for bare soils. Concentrations in surface snow were also close to equilibrium with atmospheric PAHs. Conversely, there was a net diffusive deposition of PAHs to coastal seawater during late spring, but a net volatilization from seawater during late summer. Volatilization fluxes were correlated with seawater temperature and salinity, consistent with a key role of snowmelt to the fluxes and dissolved phase concentrations during the austral summer. The comprehensive assessment provided here shows that the fugacity amplification in snow is transferred to soils and coastal seawater supporting PAH concentrations and fluxes.

The AKARI 2.5–5 micron spectra of luminous infrared galaxies in the local Universe

We present AKARI 2.5–5 μm spectra of 145 local luminous infrared galaxies (LIRG; LIR ≥ 1011 L⊙) in the Great Observatories All-sky LIRG Survey (GOALS). In all of the spectra, we measure the line fluxes and equivalent widths (EQWs) of the polycyclic aromatic hydrocarbon (PAH) at 3.3 μm and the hydrogen recombination line Brα at 4.05 μm, with apertures matched to the slit sizes of the Spitzer low-resolution spectrograph and with an aperture covering ∼95% of the total flux in the AKARI two-dimensional (2D) spectra. The star formation rates (SFRs) derived from the Brα emission measured in the latter aperture agree well with SFRs estimated from LIR, when the dust extinction correction is adopted based on the 9.7 μm silicate absorption feature. Together with the Spitzer Infrared Spectrograph (IRS) 5.2–38 μm spectra, we are able to compare the emission of the PAH features detected at 3.3 μm and 6.2 μm. These are the two most commonly used near/mid-infrared indicators of starburst or active galactic nucleus (AGN) dominated galaxies. We find that the 3.3 μm and 6.2 μm PAH EQWs do not follow a linear correlation and at least a third of the galaxies classified as AGN-dominated sources using the 3.3 μm feature are classified as starbursts based on the 6.2 μm feature. These galaxies have a bluer continuum slope than galaxies that are indicated to be starburst-dominated by both PAH features. The bluer continuum emission suggests that their continuum is dominated by stellar emission rather than hot dust. We also find that the median Spitzer/IRS spectra of these sources are remarkably similar to the pure starburst-dominated sources indicated by high PAH EQWs in both 3.3 μm and 6.2 μm. Based on these results, we propose a revised starburst/AGN diagnostic diagram using 2–5 μm data: the 3.3 μm PAH EQW and the continuum color, Fν(4.3 μm)/Fν(2.8 μm). We use the AKARI and Spitzer spectra to examine the performance of our new starburst/AGN diagnostics and to estimate 3.3 μm PAH fluxes using the James Webb Space Telescope (JWST) photometric bands in the redshift range 0 &lt; z &lt; 5. Of the known PAH features and mid-infrared high ionization emission lines used as starburst/AGN indicators, only the 3.3 μm PAH feature is observable with JWST at z &gt; 3.5, because the rest of the features at longer wavelengths fall outside the JWST wavelength coverage.

Multimedia modeling of the PAH concentration and distribution in the Yangtze River Delta and human health risk assessment

Emissions of polycyclic aromatic hydrocarbons (PAHs) in China remain at a high level compared to those in developed countries. The Yangtze River Delta (YRD) is an economic and industrial center in China with an extremely large population. The potentially high emissions and excess cancer risk from human exposure in this region cannot be neglected. This study applied a multimedia model to estimate the concentrations of 16 US EPA priority PAHs in the environment in the YRD with a well-developed PAH-emission inventory for 2014. The model predicted that the average concentrations of ΣPAHs were 274 ng/m3 in the air, 255 ng/g in the soil, 15 ng/g in vegetation, 147 ng/L in freshwater and 144 ng/g in sediment, as well as 99 ng/L and 80 ng/g in seawater and sediment, respectively. Soil is the PAH sink in this region, and the net flux of the total PAHs is always from air to soil for each isomer. A deterministic assessment observed that the ELCR (excess lifetime cancer risk) ranged from 2.5 × 10−6 to 3.0 × 10−5 for exposure by air inhalation and from 3.5 × 10−7 to 7.9 × 10−6 for exposure by soil ingestion. The probabilistic results did not find any probability of ELCR >10−4 by exposure via soil ingestion in the YRD. The probabilistic ELCR induced by inhalation exposure varied from 8.1 × 10−7 to 3.1 × 10−4 in the YRD. This study provided a comprehensive overview of PAHs occurrence in natural environments and of the relevant human health risks. The information presented in this study could help authorities to enact a strategy regarding emission reduction and pollution control relevant to PAHs. CapsuleMultimedia modeling predicted distributions and compositions of PAHs in different environmental compartments, and deterministic and probabilistic ELCRs induced by air inhalation and soil ingestion were also provided.

PAHs in the Northern South China Sea: Horizontal transport and downward export on the continental shelf

Abstract To investigate horizontal transport and particulate export of semivolatile pollutants on the continental shelf or marginal sea, surface and depth water samples were collected across the northern South China Sea (SCS) and analyzed for polycyclic aromatic hydrocarbons (PAHs). The total concentrations of Σ 15 PAH in seawater were in the range of 1.6–14 ng L −1 (mean 5.5 ng L −1 ), and the offshore decreasing trend of PAHs revealed intense terrigenous transport on the continental shelf, which was originated from combustion activity. Vertically, PAHs in the particulate phase followed surface-enrichment and depth-depletion pattern with a concentration maximum (2.9 ng L −1 ) at the biomass maximum, while the dissolved PAH concentrations showed a minimum (1.5 ng L −1 ) at the same depth. Particulate export fluxes of PAHs were between 24 and 195 ng m −2 d −1 in the northern SCS based on 238 U/ 234 Th equilibria, which is suggested appropriate to quantify their downward flux in the upper water column. Efficient oceanic biological pump drives PAHs downward export to the deep ocean in the northern SCS.

Sediment evidence of industrial leakage-induced asynchronous changes in polycyclic aromatic hydrocarbons and trace metals from a sub-trophic lake, southwest China.

It has been well established that regional patterns of atmosphere-borne polycyclic aromatic hydrocarbons (PAHs) and trace metals were predominantly associated with the trajectory of socio-economic development; however, they could be potentially modulated by anthropogenic fingerprint of local sources such as industrial spill. Here, we established historical pollution data of both PAHs and trace metals from a well-dated sediment core from Yangzong Lake of Southwest China, which experienced a severe tailing leakage accident derived from a zinc concentrate smelting plant in 2007, aiming to evaluate the heterogeneity in their temporal trajectories and their sources of contamination in the context of regional deposition patterns. Sedimentary records show that the concentrations and fluxes of both PAHs and trace metals remained a consistently low level before the 1950s. An increasing trend and the synchronous changes of both PAHs and trace metals during ~ 1950-2002 were well consistent with the temporal pattern of socio-economic development in western China, with coal combustion and smelting industries as the main sources of contamination in this region. However, arsenic (As) and PAHs exhibited a concurrent spike for the period of ~ 2007-2013, contrasting strongly to the regional pattern of these contaminants. The modern concentrations of As revealed a 5- to 14-fold increase over the pre-1950 level, with the contemporary concentrations of PAHs rising by ~ 10-14 times. The sediment records reveal that local fingerprints of smelting activities in the catchment of Yangzong Lake have overridden the temporary pattern of regional atmosphere-borne As and PAHs over the last decade. This highlights the important role of local pollution sources in modulating or even overriding the regional pattern of anthropogenic contamination in highly impacted systems.

Influence of anthropogenic activities on polycyclic aromatic hydrocarbons in sediments from mangrove wetland at Dongzhai Harbor, China: distribution, sources, probability risk, and temporal trend

Sixteen polycyclic aromatic hydrocarbons (PAHs) in 37 surface sediments and a sediment core from the Dongzhai National Nature Reserve in Hainan island of China were analysed. The total concentration of the 16 PAHs ranged from 15.7 to 464.0 ng g−1 (mean value of 76.7 ng g−1) in the surface sediments, and 8.6–115.9 ng g−1 (average 39.3 ng g−1) in the sediment core. Combustions of petroleum, biomass, coal, and grass were the major pyrogenic sources in surface sediments, and some areas had petrogenic sources (mainly petroleum spills). Results of the ecological risk assessment show little negative effect of most of the PAHs in the study area. The depositional flux of PAHs generally increased from the deeper layers toward the upper layers of the sediments. The flux rate rapidly increased after the 1980s, in contrast to that of some developed countries.

Seasonal atmospheric deposition and air–sea gas exchange of polycyclic aromatic hydrocarbons over the Yangtze River Estuary, East China Sea: Implications for source–sink processes

In this work, air samples and surface seawater samples covering four seasons from March 2014 to January 2015 were collected from a background receptor site in the YRE to explore the seasonal fluxes of air–sea gas exchange and dry and wet deposition of 15 polycyclic aromatic hydrocarbons (PAHs) and their source–sink processes at the air–sea interface. The average dry and wet deposition fluxes of 15 PAHs were estimated as 879 ± 1393 ng m−2 d−1 and 755 ± 545 ng m−2 d−1, respectively. Gaseous PAH release from seawater to the atmosphere averaged 3114 ± 1999 ng m−2 d−1 in a year round. The air–sea gas exchange of PAHs was the dominant process at the air–sea interface in the YRE as the magnitude of volatilization flux of PAHs exceeded that of total dry and wet deposition. The gas PAH exchange flux was dominated by three-ring PAHs, with the highest value in summer and lowest in winter, indicating a marked seasonal variation owing to differences in Henry's law constants associated with temperature, as well as wind speed and gaseous-dissolved gradient among seasons. Based on the simplified mass balance estimation, a net 11 tons y−1 of PAHs (mainly three-ring PAHs) were volatilized from seawater to the atmosphere in a ∼20,000 km2 area in the YRE. Other than the year-round Yangtze River input and ocean ship emissions, the selective release of low-molecular-weight PAHs from bottom sediments in winter due to resuspension triggered by the East Asian winter monsoon is another potential source of PAHs. This work suggests that the source–sink processes of PAHs at the air–sea interface in the YRE play a crucial role in regional cycling of PAHs.

CONCENTRATIONS and WET DEPOSITION FLUXES of POLYCYCLIC AROMATIC HYDROCARBONS (PAHs) in a SUBURBAN LOCATION of ESKİŞEHiR

Wet-only precipitation samples were collected using a collection plate between June 2007 and April 2008, in Eskisehir, Turkey. Polycyclic aromatic hydrocarbons (PAHs) were analyzed in precipitation samples by gas chromatography-mass spectrometry (GC-MS). PAH concentrations in the sampling location in atmospheric gas and particle phase samples were also determined. Significant difference in atmospheric concentrations and precipitation samples were observed. Annual PAH flux was found comparable with other cities in Turkey and calculated around 177.2±120.4 μg m -2 day -1 . Wet deposition was noticed an important mechanism on removal of semi-volatile organic compounds from atmosphere.

Comparison of direct benthic flux to ebullition-facilitated flux of polycyclic aromatic hydrocarbons and heavy metals measured in the field

No studies to date have compared directly the ebullition-facilitated organic and metal contaminant fluxes to direct benthic contaminant fluxes measured in the field. To address this knowledge gap, we measured benthic organic and metal contaminant fluxes at the sediment-water interface and compared them to simultaneously measured ebullition-facilitated contaminant fluxes at nine sites in a contaminated waterway in the Chicago River, IL, USA, to determine the relative importance of each transport mechanism to total sediment release. Two benthic flux chambers with integrated gas ebullition samplers were built to measure both gas ebullition and in situ fluxes of polycyclic aromatic hydrocarbons (PAHs), metals, sulfide, ammonia, nitrate, dissolved organic carbon (DOC), total filtered phosphorus (TFP), and dissolved oxygen (DO) across the sediment-water interface over time. Aqueous pH and oxidation-reduction potential (ORP) within the chamber were also monitored. The gas ebullition collection system trapped heavy metals and the 16 United States Environmental Protection Agency (USEPA) priority-pollutant PAHs (Σ16PAH) transported with gas bubbles through sorption and particle entrainment on a pre-combusted glass wool trap as in our previous studies. The results demonstrate that gas ebullition contaminant transport is a significant source of pollution release to the water column, as great as or greater than direct benthic transport. In several sites, release rates of Σ16PAHs and some metals from the sediment by gas ebullition were more than an order of magnitude higher than from direct benthic release. The average total PAH ebullition-facilitated release of all sites is predicted to be nearly 0.5 g m−2 on an annual basis. Gas ebullition is an important pathway for release of PAHs and heavy metal pollutants to the water column and monitoring of this important release pathway should be performed to adequately address the true environmental impacts of polluted sediments.

A 150-year record of polycyclic aromatic compound (PAC) deposition from high Andean Cajas National Park, southern Ecuador

The temporal profiles of polycyclic aromatic compounds (PACs) in lake sediments reflect past changes in emissions, transport and deposition of these pollutants and, thus, record natural and anthropogenic processes. We document fluxes of PACs [(polycyclic aromatic hydrocarbons (PAHs), oxygenated PAHs (OPAHs) and azaarenes (AZAs)] deposited in two tropical high-altitude lakes in the Cajas National Park (Ecuadorian Andes, 2°50′S, 79°10′W). In remote and high elevation Laguna Fondococha (4130m a.s.l.), the temporal fluxes of OPAHs and AZAs were similar to those of PAHs suggesting similar sources. A significant increase of PAC deposition after the 1950s reflects Ecuador's economic development. PAH fluxes were relatively low (∑27PAHs (without retene and perylene): 0.86–11.21ngcm−2yr−1) with a composition pattern typical for long-range atmospheric transport (high 9-fluorenone/fluorene ratios) and biomass burning (30% low molecular weight PAHs). PAHs diagnostic of high temperature combustion (industry, traffic) make up 20–25% of total PAHs. Perylene concentrations increase linearly with increasing sediment depth suggesting diagenetic in-situ production. At lower elevations (Laguna Llaviucu, 3140m a.s.l.) and closer to urban areas, PAC fluxes in the past decades were 4–5 times higher than in the remote high-elevation lake. Laguna Llaviucu also showed higher concentrations of high molecular weight pyrogenic PAHs and a greater diversity of AZAs. Individual OPAHs and AZAs reflect mainly combustion activities. In Laguna Llaviucu, which is at a lower elevation (3140m a.s.l.) and closer to the city, molecular ratios suggest short-range atmospheric transport and deposition of PACs. A very foggy climate (170 rainy days per year) with the precipitation maximum at 3500m removes PACs very efficiently (by wet deposition) from the atmosphere at very short distances from emission sources. This partly explains why L. Llaviucu shows higher fluxes of PACs than the higher elevation L. Fondococha. This study presents the first historical record of organic pollutants from environmental archives in Ecuador.

Transfer of lipid molecules and polycyclic aromatic hydrocarbons to open marine waters by dense water cascading events

Settling particles were collected by a set of moored sediment traps deployed during one year in the western Gulf of Lion along Cap de Creus and Lacaze-Duthiers submarine canyons and on the adjacent southern open slope. These traps collected particles during periods of pelagic settling and also during events of deep water flushing by dense shelf water cascading (DSWC). Analyses of lipid biomarkers (n-alkanes, n-alkan-1-ols, sterols and C37-C38 alkenones) and polycyclic aromatic hydrocarbons (PAHs) showed much higher transfer of terrestrial lipids and PAHs to open deep waters during DSWC than in the absence of cascading. The area of highest lateral fluxes was mostly located at 1000m depth but also at 1500m depth and extended along the canyons and to the adjacent slope. Higher fluxes were observed near the bottom (30m above bottom; mab) than at intermediate waters (500 mab) which is consistent with the formation and sinking of dense water over the continental shelf, and its transport through the canyons towards the continental slope and deep basin. DSWC involved the highest settling fluxes of terrestrial lipids and PAHs ever described in marine continental slopes and the pelagic domain, as illustrated by peak values of C23-C33 odd carbon numbered alkanes (405ngm−2d−1), C22-C32 even carbon numbered alkan-1-ols (850ngm−2d−1), β-sitosterol+sitostanol (4800ngm−2d−1) and PAHs (55µgm−2d−1). The algal lipids also showed higher transfer to deep waters during DSWC but to a lower extent than the terrigenous compounds. However, the C37-C38 alkenones constituted an exception and their settling fluxes were not influenced by DSWC. The lack of influence of the DSWC on the C37-C38 alkenone settling is consistent with absence of haptophyte algal inputs from the continental shelf and reinforces the reliability of these molecules for palaeothermometry and palaeoproductivity measurements in pelagic systems.

Fate of polycyclic aromatic hydrocarbons from the North Pacific to the Arctic: Field measurements and fugacity model simulation

Polycyclic aromatic hydrocarbons (PAHs) have accumulated ubiquitously inArctic environments, where re-volatilization of certain organic pollutants as a result of climate change has been observed. To investigate the fate of semivolatile organic compounds in the Arctic, dissolved PAHs in the surface seawaters from the temperate Pacific Ocean to the Arctic Ocean, as well as a water column in the Arctic Ocean, were collected during the 4th Chinese National Arctic Research Expedition in summer 2010. The total concentrations of seven dissolved PAHs in surface water ranged from 1.0 to 5.1 ng L−1, decreasing with increasing latitude. The vertical profile of PAHs in the Arctic Ocean was generally characteristic of surface enrichment and depth depletion, which emphasized the role of vertical water stratification and particle settling processes. A level III fugacity model was developed in the Bering Sea under steady state assumption. Model results quantitatively simulated the transfer processes and fate of PAHs in the air and water compartments, and highlighted a summer air-to-sea flux of PAHs in the Bering Sea, which meant that the ocean served as a sink for PAHs, at least in summer. Acenaphthylene and acenaphthene reached equilibrium in air-water diffusive exchange, and any perturbation, such as a rise in temperature, might lead to disequilibrium and remobilize these compounds from their Arctic reservoirs.

Indirect influence of eutrophication on air – water exchange fluxes, sinking fluxes, and occurrence of polycyclic aromatic hydrocarbons

How eutrophication affects biogeochemical processes of hydrophobic organic contaminants (HOCs) in aquatic environments is a pending challenge. Although the direct influence of eutrophication on biogeochemical processes of HOCs in waters has been well addressed, the indirect influence of eutrophication on biogeochemical processes of HOCs remains largely unknown. Here we take the large shallow eutrophic Lake Taihu in China and polycyclic aromatic hydrocarbons (PAHs) as examples to provide novel knowledge on the indirect influence of eutrophication on air – water exchange fluxes, sinking fluxes, and occurrence of HOCs. The air – water exchange fluxes of individual PAHs varied dramatically at different sites in all studied seasons. The sinking flux of ΣPAH16 was 14 855.3 ± 1579.9, 3548.9 ± 650.6, and 5588.4 ± 530.7 ng m−2 d−1 in spring, summer, and winter. The corresponding concentration of ΣPAH16 in surface sediments was 713.1 ± 78.6, 339.7 ± 36.6, and 293.0 ± 35.2 ng g−1 d.w. Our study for the first time suggested that recruitment of cyanobacteria from surface sediments to water column in spring reduced the concentrations of PAHs in surface sediments, but enhanced their concentrations in the bulk water column, and overwintering of cyanobacteria in winter enhanced the concentrations of PAHs in surface sediments. High pH induced indirectly by eutrophication decreased seasonal air – water exchange fluxes (enhanced net volatilization) of PAHs, reduced the aromaticity of surface sediments and the hydrophobicity of phytoplankton cell surface, and reduced the accumulation of PAHs in surface sediments and phytoplankton consequently. Sinking fluxes and daily loss of PAHs from the water column decreased with phytoplankton biomass because the fraction of organic matter sinking from the water column decreased with phytoplankton biomass. Our study provides novel complementary knowledge for the biological pump for HOCs, and has important implications for understanding the coupling between eutrophication and biogeochemical processes of HOCs in subtropical shallow eutrophic waters.

Use of a numerical simulation approach to improve the estimation of air-water exchange fluxes of polycyclic aromatic hydrocarbons in a coastal zone

The air-water exchange is important for determining the transport, fate, and chemical loading of polycyclic aromatic hydrocarbons (PAHs) in the atmosphere and in aquatic systems. Investigations of PAH air-water exchange are mostly based on observational data obtained using complicated field sampling processes. This study proposes a new approach to improve the estimation of long-term PAH air-water exchange fluxes by using a multivariate regression model to simulate hourly gaseous PAH concentrations. Model performance analysis and the benefits from this approach indicate its effectiveness at improving the flux estimations and at decreasing the field sampling difficulty.The proposed GIS mapping approach is useful for box model establishment and is tested for visualization of the spatiotemporal variations of air-water exchange fluxes in a coastal zone. The air-water exchange fluxes illustrated by contour maps suggest that the atmospheric PAHs might have greater impacts on offshore sites than on the coastal area in this study.

Assessing soil-air partitioning of PAHs and PCBs with a new fugacity passive sampler

Soil-air fluxes of polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) were determined using a novel application of passive samplers to measure air and soil air, which is air in close proximity and in equilibrium with soil. Existing methods to measure flux of semi-volatile compounds between soil and air require collecting samples from the top soil layer. Yet, the top soil layer is hard to define and oversampling may misrepresent the exchangeable fraction. Alternatively, modified active samplers can measure soil air in situ, but require electricity while deployed. We present a new method to measure time-weighted averages of soil air concentrations in situ using passive sampling and requiring no electricity: a box is placed over low-density polyethylene passive samplers deployed 1cm above the soil. Passive air samplers were also co-deployed 1.5m above the soil to measure ambient air concentrations in three U.S. locations: near a former PCB manufacturing facility in Anniston, Alabama; on a former creosoting and the current Wyckoff/Eagle Superfund site near Seattle, Washington; and near the site of a recent oil-train derailment and fire in Mosier, Oregon. Following n-hexane extraction, sampler extracts were analyzed for PAHs with gas chromatography-tandem mass spectrometry and PCBs with dual gas chromatography-electron capture detectors. PAHs were generally depositing at Anniston and Mosier sites, but volatilizing from soil in Wyckoff, the site with historically-contaminated soil. PCBs were detected most frequently at the Anniston site, although levels were lower than previous reports. Variability in concentration measurements was greater among soil air samplers than air samplers, likely due to soil heterogeneity. Environmental conditions under the novel soil air box did not substantially change soil-air partitioning behavior. This method of measuring soil air in situ will allow for understanding of source-sink dynamics at sites with recent and historical contamination, and where conventional sampling is challenging.

Historical record of anthropogenic polycyclic aromatic hydrocarbons in a lake sediment from the southern Tibetan Plateau.

High-altitude lake sediments can be used as natural archives to reconstruct the history of pollutants. In this work, the temporal distribution of polycyclic aromatic hydrocarbons (PAHs) was determined in a sediment core collected from the southern Tibetan Plateau (TP), which was dated by using the 210Pb dating method and validated with the 137Cs fallout peak. The concentrations of the anthropogenic PAHs (Σ8PAH) in the sediment core ranged from 0.83 to 12ng/g dw, and the fluxes of the Σ8PAH were in the range of 2.1-27g/cm2/year. The temporal variations in the concentration and input flux of anthropogenic PAHs were low with little variability before the 1950s, and then gradually increased from the 1950s to the 1980s, and an accelerated increase was observed after the early 1980s. The content of total organic carbon played an insignificant role in affecting the time trends of PAHs in the sediment core. Diagnostic concentration fractions of PAH components indicate PAHs in the lake sediment of the southern TP which are mainly from biomass burning and/or from long-range atmospheric transport.

Diffusive flux of PAHs across sediment–water and water–air interfaces at urban superfund sites

Superfund sites may be a source of polycyclic aromatic hydrocarbons (PAHs) to the surrounding environment. These sites can also act as PAH sinks from present-day anthropogenic activities, especially in urban locations. Understanding PAH transport across environmental compartments helps to define the relative contributions of these sources and is therefore important for informing remedial and management decisions. In the present study, paired passive samplers were co-deployed at sediment-water and water-air interfaces within the Portland Harbor Superfund Site and the McCormick and Baxter Superfund Site. These sites, located along the Willamette River (Portland, OR, USA), have PAH contamination from both legacy and modern sources. Diffusive flux calculations indicate that the Willamette River acts predominantly as a sink for low molecular weight PAHs from both the sediment and the air. The sediment was also predominantly a source of 4- and 5-ring PAHs to the river, and the river was a source of these same PAHs to the air, indicating that legacy pollution may be contributing to PAH exposure for residents of the Portland urban center. At the remediated McCormick and Baxter Superfund Site, flux measurements highlight locations within the sand and rock sediment cap where contaminant breakthrough is occurring. Environ Toxicol Chem 2017;36:2281-2289. © 2017 SETAC.

Air-water exchange of PAHs and OPAHs at a superfund mega-site

Chemical fate is a concern at environmentally contaminated sites, but characterizing that fate can be difficult. Identifying and quantifying the movement of chemicals at the air-water interface are important steps in characterizing chemical fate. Superfund sites are often suspected sources of air pollution due to legacy sediment and water contamination. A quantitative assessment of polycyclic aromatic hydrocarbons (PAHs) and oxygenated PAH (OPAHs) diffusive flux in a river system that contains a Superfund Mega-site, and passes through residential, urban and agricultural land, has not been reported before. Here, passive sampling devices (PSDs) were used to measure 60 polycyclic aromatic hydrocarbons (PAHs) and 22 oxygenated PAH (OPAHs) in air and water. From these concentrations the magnitude and direction of contaminant flux between these two compartments was calculated. The magnitude of PAH flux was greater at sites near or within the Superfund Mega-site than outside of the Superfund Mega-site. The largest net individual PAH deposition at a single site was naphthalene at a rate of −14,200 (±5780) (ng/m2)/day. The estimated one-year total flux of phenanthrene was −7.9×105 (ng/m2)/year. Human health risk associated with inhalation of vapor phase PAHs and dermal exposure to PAHs in water were assessed by calculating benzo[a]pyrene equivalent concentrations. Excess lifetime cancer risk estimates show potential increased risk associated with exposure to PAHs at sites within and in close proximity to the Superfund Mega-site. Specifically, estimated excess lifetime cancer risk associated with dermal exposure and inhalation of PAHs was above 1 in 1 million within the Superfund Mega-site. The predominant depositional flux profile observed in this study suggests that the river water in this Superfund site is largely a sink for airborne PAHs, rather than a source.

Atmospheric deposition of polycyclic aromatic hydrocarbons (PAHs) in Shanghai: the spatio-temporal variation and source identification

This study investigated the dry and wet deposition fluxes of atmospheric polycyclic aromatic hydrocarbons (PAHs) in Shanghai, China. The flux sources were traced based on composition and spatio-temporal variation. The results show that wet deposition concentrations of PAHs ranged from 0.07 to 0.67 mg·L–1 and were correlated with temperature (P<0.05). Dry deposition of PAHs concentrations ranged from 3.60–92.15 mg·L–1 and were higher in winter and spring than in summer and autumn. The annual PAH average fluxes were 0.631 mg·m–2·d–1 and 4.06 mg·m–2·d–1 for wet and dry deposition, respectively. The highest wet deposition of PAH fluxes was observed in summer, while dry deposition fluxes were higher in winter and spring. Atmospheric PAHs were deposited as dry deposition in spring and winter, yet wet deposition was the dominant pathway during summer. Total atmospheric PAH fluxes were higher in the northern areas than in the southern areas of Shanghai, and were also observed to be higher in winter and spring. Annual deposition of atmospheric PAHs was about 10.8 t in across all of Shanghai. Wet deposition of PAHs was primarily composed of two, three, or four rings, while dry deposition of PAHs was composed of four, five, or six rings. The atmospheric PAHs, composed of four, five, or six rings, primarily existed in the form of particulates. Coal combustion and vehicle emissions were the dominant sources of PAH in the observed area of downtown Shanghai. In suburban areas, industrial pollution, from sources such as coke oven, incinerator, and oil fired power plant, was as significant as vehicle emissions in contributing to the deposition of PAHs.