Evidence for incorporation of H2S in groundwater fulvic acids from stable isotope ratios and sulfur K-edge X-ray absorption near edge structure spectroscopy

Groundwater samples collected in a shallow oxic and reduced deep groundwater system revealed the influence of dissolved sulfide on the chemical and isotopic composition of fulvic acid associated sulfur. Stable isotope compositions of groundwater sulfate and fulvic acid sulfur and sulfur K-edge X-ray absorption near edge structure (XANES) spectroscopy data were used to determine the sources and processes affecting fulvic acid sulfur in the aquifer. A delta34S value of 2.2 per thousand for the shallow groundwater sulfate and a delta34S value of fulvic acids of 4.9 per thousand accompanied by a contribution of up to 49% of the most oxidized sulfur species (S+6) documented that fulvic acid sulfur is mainly derived from soil S compounds such as ester sulfates, with delta34S values similar to those of atmospheric sulfate deposition. In contrast, in the deep groundwater system with elevated delta34S values in groundwater sulfate of up to 20per thousand due to bacterial sulfate reduction, delta34S values in fulvic acid sulfur were negative and were up to 22per thousand lower compared to those of groundwater sulfate. Furthermore, reduced sulfur compounds constituted a significantly higher proportion of total fulvic acid sulfur in the deep groundwater compared to fulvic acids in shallow groundwater, supporting the hypothesis that fulvic acids act as a sink for dissolved hydrogen sulfide in the deep aquifer. Our results suggest that the combination of sulfur K edge XANES spectroscopy and stable isotope analysis on fulvic acids represents a powerful tool to elucidate the role of fulvic acids in the sulfur cycle in groundwater.     

Use of tritium accelerator mass spectrometry for tree ring analysis

Public concerns over the health effects associated with low-level and long-term exposure to tritium released from industrial point sources have generated the demand for better methods to evaluate historical tritium exposure levels for these communities. The cellulose of trees accurately reflects the tritium concentration in the source water and may contain the only historical record of tritium exposure. The tritium activity in the annual rings of a tree was measured using accelerator mass spectrometry to reconstruct historical annual averages of tritium exposure. Milligram-sized samples of the annual tree rings from a Tamarix located at the Nevada Test Site are used for validation of this methodology. The salt cedar was chosen since it had a single source of tritiated water that was well-characterized as it varied over time. The decay-corrected tritium activity of the water in which the salt cedar grew closely agrees with the organically bound tritium activity in its annual rings. This demonstrates that the milligram-sized samples used in tritium accelerator mass spectrometry are suited for reconstructing anthropogenic tritium levels in the environment.     

Sources and processes affecting sulfate in a karstic groundwater system of the Franconian Alb, southern Germany

Chemical and isotope analyses on groundwater sulfate and 3H measurements on groundwaterwere used to determine the sulfate sources and sulfur transformation processes in a heterogeneous karst aquifer of the Franconian Alb, southern Germany. Sulfate was found to be derived from atmospheric deposition. Young groundwater was characterized by high sulfate concentrations and delta34S values similar to those of recent atmospheric sulfate deposition. However, the delta18O values of groundwater SO4(2-) were depleted by several per mil with respect to those of atmospheric deposition. This isotopic shift is indicative of mineralization of carbon-bonded S in the vadose zone of the karst system. In groundwater with mean residence times of more than 60 years, a trend of increasing delta34S values and delta18O values with decreasing sulfate concentrations was observed. This trend could not be solely explained by preindustrial atmospheric sulfate deposition with higher delta34S values, and hence, we conclude that bacterial (dissimilatory) sulfate reduction in the porous matrix of the karst aquifer must have occurred. This process has the potential to contribute to long-term biodegradation of contaminants in the porous rock matrix representing the dominantwater reservoir of the fissured porous karst aquifer.     

Reconstructing tritium exposure using tree rings at Lawrence Berkeley National Laboratory, California

Annual tritium exposures were reconstructed using tree cores from Pinus jeffreyi and Eucalyptus globulus near a tritiated water vapor release stack. Both tritium (3H) and carbon-14 (14C) from the wood were measured from milligram samples using accelerator mass spectrometry. Because the annual nature of the eucalyptus tree rings was in doubt, 14C measurements provided growth rates used to estimate the age for 3H determinations. A 30-yr comparison of organically bound tritium (OBT) levels to reported 3H release data is achieved using OBT measurements from three trees nearthe stack. The annual average 3H, determined from atmospheric water vapor monitoring stations, is comparable to the OBT in proximal trees. For situations without adequate historical monitoring data, this measurement-based historical assessment provides the only independent means of assessing exposure as compared to fate and transport models that require prior knowledge of environmental conditions and 3H discharge patterns.     

Assessment of sulfate sources in high-elevation Asian precipitation using stable sulfur isotopes

Stable sulfur isotope measurements (delta34S) made on samples collected from a 2 m snowpit on the Inilchek Glacier, Tien Shan Mountains (42.16 degrees N, 80.25 degrees E, 5100 m) are used to estimate sources of sulfate (SO4(2-)) in high-elevation Central Asian precipitation. Comparison of snowpit oxygen isotope (delta18O) data with previous work constrains the age of the snowpit samples to the summer season during which they were retrieved (1999). Delta34S measurements were made at 10 cm resolution (20 samples total), with delta34S values ranging from 0.4/1000 during background ([SO4(2-)] < 1 microequiv L(-1)) periods to 19.4/1000 during a single high [SO4(2-)] event. On the basis of the significant correlation (r = 0.87) between [SO4(2-)] and delta34S values, coupled with major ion concentration time series and concentration ratios, we suggest a two-component mixing system consisting of evaporite dust and anthropogenic SO4(2-) to explain the observed delta34S values. Using a regression model, we estimate that during the 1999 summer season 60% of the deposited SO4(2-) was from an evaporite dust source, while 40% of the SO4(2-) was from anthropogenic sources. Due to the potentially large and unconstrained range of delta34S values for both evaporite and anthropogenic SO4(2-) sources in Asia, the error in our estimates is difficult to assess. However, the delta34S data from the 1999 Tien Shan snowpit provide the first unambiguous identification of evaporite and anthropogenic SO4(2-) in high-elevation Asian precipitation, and future ice core studies using improved analysis techniques and source delta34S values can provide detailed information on sulfur biogeochemistry and anthropogenic impacts in Asian alpine regions.     

Temporal trends in the isotope signature of air-borne sulfur in Central Europe

In various parts of the Northern hemisphere air-borne S exhibits a seasonality, with isotopically light (i.e., 32S-rich) sulfur predominating in the warm summer months. Such seasonality has been reported from the United States, Canada, Japan, and China. Elevated biological emissions of isotopically light S in summer, a temperature-dependent isotope fractionation accompanying the oxidation of SO2, and heavy rains in winter bringing 34S-rich marine S have been suggested as the controlling mechanisms. In the atmosphere of Central Europe, one of the most severely polluted regions of the world, we have found an opposite seasonal trend: Isotopically light SO2-S predominates in the cold winter months, whereas isotopically heavy SO2-S is typical of the summer. The low delta34S values of air-borne SO2 in winter are influenced by low-delta34S emissions from local coal-burning power plants. The coal contains isotopically light S (mean delta34S of 1.6/1000). Higher demand for electricity during the heating season leads to higher anthropogenic S emission rates in winter. On a yearly basis, atmospheric sulfate S in Central Europe is isotopically heavier than atmospheric SO2-S by 4/1000. Atmospheric oxidation of SO2 is accompanied by an isotope fractionation resulting in 34S-enriched sulfate. In addition to the seasonality in air-borne delta34S(SO2), we report also an interannual trend of 1/1000 yr(-1) toward isotopically light sulfate S in atmospheric deposition. This interannual trend cannot be explained by a change in pollution sources accompanying the present massive environmental cleanup. To investigate the role of biological S emissions from the soil of heavily polluted ecosystems, we conducted a series of laboratory experiments using repacked soil columns and 34S-enriched precipitation under summer and winter temperatures. These experiments indicate that, under summer temperatures, the 34S-labeled precipitation is largely captured by the upper organic-rich soil horizons, a high proportion (53-74%) of S input is revolatilized, and the biologically reemitted S is isotopically light. Under winter temperatures more precipitation S is leached to the bottom of the soil columns. Our experiments have shown that biological emissions in Central Europe can be sizable. Yet, they cannot be singled out in the overall SO2 isotope pattern in the atmosphere. The main reason is continuous, variable (0-4/1000), open-system depletion in 34S in the residual SO2 during the isotopically selective SO2-to-SO4(2-) conversion.     

Dendrochemistry of multiple releases of chlorinated solvents at a former industrial site

Trees can take up and assimilate contaminants from the soil, subsurface, and groundwater. Contaminants in the transpiration stream can become bound or incorporated into the annual rings formed in trees of the temperate zones. The chemical analysis of precisely dated tree rings, called dendrochemistry, can be used to interpret past plant interactions with contaminants. This investigation demonstrates that dendrochemistry can be used to generate historical scenarios of past contamination of groundwater by chlorinated solvents at a site in Verl, Germany. Increment cores from trees at the Verl site were collected and analyzed by energy-dispersive X-ray fluorescence (EDXRF) line scanning. The EDXRF profiles showed four to six time periods where tree rings had anomalously high concentrations of chlorine (Cl) as an indicator of potential contamination by chlorinated solvents.     

Carbon isotopes in tree rings of Norway spruce exposed to atmospheric pollution

The Bohemian Forest was exposed to high levels of sulfur and nitrogen deposition during the last century. The change in acid deposition caused a rapid decline in pH and increase in Al concentrations of soil solutions since the 1950s. A possible negative effect of soil chemistry on growth of Norway spruce tree has been studied using the 13C isotopic signal and chemistry of the tree rings. Tree rings were sectioned by decades, and whole wood was analyzed for isotopic composition (delta 13C) and content of Mg, Ca, and Al. Only those rings that formed after the juvenile effect in early rings were used and trends from the beginning of 20th century were evaluated. The mean delta 13C of the spruce tree rings was 17.6%. The delta 13C did not follow climate changes but had an opposite trend to that of acid depositions and Al concentrations in soil solution, but a similar trend as soil acidification (pH decrease), implying a negative effect of acid deposition and soil acidification on tree physiology. The molar ratio of base cations to Al decreased together with delta 13C.     

Evidence for anthropogenic 210Po in the urban atmosphere of Seoul, Korea

We have measured the concentrations of 210Po, 210Pb, SO4(2-), Na+, and 34S in precipitation samples from two metropolitan cities, Seoul and Busan, Korea. The delta34S values ranged from 0 to 10% in most Seoul and Busan precipitation samples, indicating major contributions from industrial sources to S levels. A high level of excess 210Po, which is not produced by 210Pb decay in the troposphere, was observed in both regions. The excess 210Po activities in some samples from Busan, a harbor city, were influenced strongly by sea salt (i.e., sea-surface microlayer) which could be traced using [Na+] and delta34S values. In Seoul precipitations, we observed a good correlation between non-sea-salt SO4(2-) and excess 210Po, suggesting that both species are controlled mainly by the same factor. This correlation and the delta34S values indicate that the major source for both species in this region is likely to be anthropogenic, rather than from traditionally suggested sources such as soil resuspension, stratospheric air intrusion, sea sprays, volcanic emissions, and biogenic emissions.     

Response of sulfate concentration and isotope composition in Icelandic rivers to the decline in global atmospheric SO2 emissions into the North Atlantic Region

This study presents the changes in dissolved sulfate concentration and isotope composition of Icelandic river waters between the peak of SO2 emissions in the United States and Europe and the present. Chloride concentration in Icelandic rivers has not changed much since 1972. The overall average change from 1972-1973 to 1996-2004 was -3%, indicating insignificant sea-salt contribution changes. More than 99% of the river-dissolved sulfur was in the form of sulfate. There are three main sources for dissolved sulfate in the rivers: rocks, sea-salts, and anthropogenic. Total dissolved sulfate, tdSO4(2-), and non-sea-salt sulfate, nssSO4(2-), decreased in all of the rivers from the early 1970s to 1996-2004. The percentage decrease varies from 13% to 65%. The decrease is smallest in rivers were there is considerable rock-derived dissolved SO4(2-). The overall average decrease was 39% for tdSO4(2-) and 46% for nssSO4(2-). The anthropogenic sulfate fraction has declined making most of the river waters delta34S values of sulfate higherthrough time. The overall decline in river sulfate and increase in delta34S, while SO2 emissions from Iceland has been increasing, demonstrates the response of river chemistry in the remote North Atlantic to the decline in man-made emissions of SO2 in North America and Europe.     

Identification of anthropogenic and natural inputs of sulfate and chloride into the karstic ground water of Guiyang, SW China: combined delta37Cl and delta34S approach

Because of active exchange between surface and groundwater of a karstic hydrological system, the groundwater of Guiyang, the capital city of Guizhou Province, southwest China, has been seriously polluted by anthropogenic inputs of NO3-, SO4(2-), Cl-, and Na+. In this work, delta37Cl of chloride and delta34S variations of sulfate in the karstic surface/groundwater system were studied, with a main focus to identify contaminant sources, including their origins. The surface, ground, rain, and sewage water studied showed variable delta37Cl and delta34S values, in the range of -4.1 to +2.0 per thousand, and -20.4 to +20.9 per thousand for delta37Cl and delta34S (SO4(2-)), respectively. The rainwater samples yielded the lowest delta37Cl values among those observed to date for aerosols and rainwater. Chloride in the Guiyang area rain waters emanated from anthropogenic sources rather than being of marine origin, probably derived from HCl (g) emitted by coal combustion. By plotting 1/SO4(2-) vs delta34S and 1/Cl- vs delta37Cl, respectively, we were able to identify some clusters of data, which were assigned as atmospheric deposition (acid rain component), discharge from municipal sewage, paleo-brine components in clastic sedimentary rocks, dissolution of gypsum mainly in dolomite, oxidation of sulfide minerals in coal-containing clastic rocks, and possibly degradation of chlorine-containing organic matter. We conclude that human activities give a significant input of sulfate and chloride ions, as well as other contaminants, into the studied groundwater system through enhanced atmospheric deposition and municipal sewage, and that multiple isotopic tracers constitute a powerful tool to ascertain geochemical characteristics and origin of complex contaminants in groundwater.     

Selenium speciation in kerogen from two Chinese selenium deposits: environmental implications

Selenium is an essential trace element for humans, animals, and vegetation. Its occurrence in the environment is characterized by specific chemical and biochemical properties that control its elemental solubility, toxicity, and environmental behavior. The Laerma Se-Au deposit and Yutangba Se deposit are two important Se-bearing deposits found recently in China. In one of these areas (Yutangba), a serious environmental impact happened involving Se poisoning. Previous studies have shown that Se in both deposits is closely related to organic matter, especially kerogen fractions, but detailed relationships between Se and kerogen and Se chemical forms were not reported. In this study, the different speciation of Se is identified by transmission electron microscopy (TEM) and other geochemical techniques (infrared spectra (IS) and X-ray diffraction (XRD)) from kerogen samples extracted from ore rocks of both deposits. The occurrence of organically bound Se in the Laerma deposit and elemental Se nanograins in the Yutangba deposit is observed, indicating the diversity of formation mechanisms and possible chemical forms of Se in Se-rich rocks. The formation of elemental Se associated with organic matter is likely related to redox conditions, whereas organic species are related to the higher sulfur content of kerogen and possibly result from S-Se substitutions. This discovery provides new evidence with which to assess potential Se mobility during weathering of ore-bearing rocks. In an altered rock, the elemental Se in kerogen is more steadily mobilized and is potentially accumulated by vegetation, which may explain the sudden prevalence of Se poisoning in the Yutangba area. In contrast, organically bound Se seems more resistant to chemical alteration compared to other Se species so that its bioavailability may be very restricted.     

Variation in the sensitivity of predicted levels of atmospheric organic particulate matter (OPM)

This study examines the sensitivity in predicted levels of atmospheric organic particulate matter (M(o), microg m(-3)) to changes in the governing gas/particle partitioning constants and the tau(I) (levels of condensable organic compounds, microg m(-3)). M(o) is given by the difference between sigma tau(i) and the corresponding sum for the gas-phase levels. It is demonstrated that the sensitivity in predicted M(o) levels increases rapidly as M(o) becomes very small relative to sigma tau(i): as the tau(i), decrease, the gas phase becomes increasingly capable of holding the majority of all tau(i) and small changes in system parameters can cause large relative changes in M(o). These effects are illustrated using predictions for two values of the reacted hydrocarbon concentration (deltaHC) for each of three secondary organic aerosol systems for relative humidity (RH) = 20-80%. Specific structures for the oxidation products allows consideration of the effects of varying activity coefficients and water uptake. At low M(o)/sigma tau(i) (as may be found in the atmosphere away from sources and at warm temperatures), relatively small errors in model input parameters (e.g., vapor pressures, vaporization enthalpies, activity coefficient parameters, and the tau(i) values for low volatility compounds) will be amplified into large errors in the predicted M(o) values.     

Distribution of polycyclic aromatic hydrocarbons in the coastal region off Macao, China: assessment of input sources and transport pathways using compositional analysis

The coastal region off Macao is a known depositional zone for persistent organic pollutants (POPs) in the Pearl River Delta and Estuary of southern China and an important gateway for the regional contributions of contamination to the globe. This paper presents a comprehensive assessment of the input sources and transport pathways of polycyclic aromatic hydrocarbons (PAHs) found in the coastal sediments of Macao, based on measurements of 48 2-7 ring PAHs and 7 sulfur/oxygenated (S/O) PAH derivatives in 45 sediment, 13 street dust, and 68 aerosol samples. Total sediment PAHs concentrations ranged from 294 to 12741 ng/g, categorized as moderate contamination compared to other regions of Asia and the world. In addition, the PAH compounds appeared to be bound more strongly to aromatics-rich soot particles than to natural organic matter, implying a prevailing atmospheric transport route for PAHs to Macao's coast. Compositional analysis and principal component analysis (PCA) suggested that different classes of PAHs in the coastal sediments of Macao may have been derived from different input sources via various transport pathways. For example, alkylated and S/O PAHs were likely derived from fossil fuel leakage and transported to sediments by both aerosols particles and street runoff. High-molecular-weight parent PAHs were predominantly originated from automobile exhausts and distributed by direct and indirect atmospheric deposition. Low-molecular-weight parent PAHs, on the other hand, may have stemmed from lower temperature combustion and fossil fuel (such as diesel) spillage from ships and boats and were transported to sediments by river runoff or direct discharge as well as by air-water exchange.     

European atmospheric pollution imported by cooler air masses to the Eastern Mediterranean during the summer

In this study we combine Pb isotopes, Pb, Ni, Cu, Zn, and several major metal concentrations, identification of the aerosol particles, and synoptic and back trajectory analyses to obtain direct evidence for the extent and nature of mixing between Middle Eastern and European sources emissions of metals and aerosols. During the summer months aerosols collected in Israel are highly polluted by metals (EF(Ni) = 120, EF(Cu) = 320, EF(Zn) = 30, EF(Pb) = 540; average values). The fraction of European Pb of mostly industrial sources is 61 +/- 21% in Jerusalem, and the fraction of European Cu, Zn, Ni, and aerosols should be on the same order. Whenever a steep pressure gradient is built between the barometric trough originating from the Persian Gulf and the subtropical ridge along the African coast, stronger westerly winds and cooler temperatures (deep Persian Trough) prevail overthe Middle East, and higher amounts of European pollution are observed in the atmosphere (74 +/- 13%). On the other hand, when the Persian Trough is in its shallow mode, the proportion of European pollution is lower (45 +/- 18%, based on Pb isotopes). This study demonstrates that atmospheric pollution over the East Mediterranean region during the summer is influenced not only by local atmospheric dispersion conditions but also by the ability of the atmosphere to inherit a significant proportion of pollutants from European sources.     

Estimation of atmospheric emissions of six semivolatile polycyclic aromatic hydrocarbons in southern canada and the United States by use of an emissions processing system

Polycyclic aromatic hydrocarbons (PAHs) are toxic compounds that are ubiquitous in the atmospheric environment. The input for an emissions processing system that was originally configured forthe study of criteria air pollutants was updated to calculate emissions of six semivolatile PAHs. The goal of the work was to produce emissions estimates with the spatial and temporal resolution needed to serve as input to a regional air quality model for southern Canada and the U.S. Such modeling is helpful in determining reductions in PAH emissions that may be necessary to protect human and ecosystem health. The total annual emission of the six PAHs (sigma6PAH) for both countries was estimated at 18 273 Mg/year. A total of 90% of these emissions arise from U.S. sources. The top six source types account for 73% of emissions and are related to metal production, open burning, incineration, and forest fires. The emission factors used in this study were derived from published compilations. Although this approach has the advantage of quality control during the compilation process, some compilations include factors from older studies that may overestimate emissions since they do not account for recent improvements in emission control technology. When compared to estimates published in the National Emissions Inventory (NEI) for 2002, the U.S. emissions in this study are higher by a factor of 4 (16 424 vs 4102 Mg/year). The cause of this difference has been investigated, and much of it is likely due to our use of data unavailable in the 2002 NEI but inferred here on the basis of the PAH emissions literature. Augmenting the 2002 NEI with this additional information would bring its reported annual emissions to 8213 Mg/year, which is within a factor of 2 of the estimates herein. The results presented for southern Canada are the first published values for all known PAH sources in that country.     

Mechanisms of hydrogen sulfide removal with steel making slag

In the present study, we experimentally investigated the removal of hydrogen sulfide using steel-making slag (SMS) and clarified the mechanism of hydrogen sulfide removal with the SMS. The results proved that SMS is able to remove hydrogen sulfide dissolved in water, and the maximum removal amount of hydrogen sulfide per unit weight of the SMS for 8 days was estimated to be 37.5 mg S/g. The removal processes of hydrogen sulfide were not only adsorption onto the SMS, but oxidation and precipitation as sulfur. The chemical forms of sulfide adsorbed onto the SMS were estimated to be sulfur and manganese sulfide in the ratio of 81% and 19%, respectively. It is demonstrated here that the SMS is a promising material to remediate organically enriched coastal sediments in terms of removal of hydrogen sulfide. Furthermore, using SMS is expected to contribute to development of a recycling-oriented society.     

Predicting pore water EPA-34 PAH concentrations and toxicity in pyrogenic-impacted sediments using pyrene content

Sediment and freely dissolved pore water concentrations of the U.S. Environmental Protection Agency's list of 34 alkyl and parent PAHs (EPA-34) were measured in 335 sediment samples from 19 different sites impacted by manufactured gas plants, aluminum smelters and other pyrogenic sources. The total EPA-34 freely dissolved pore water concentration, C(pw,EPA-34), expressed as toxic units (TU) is currently considered one of the most accurate measures to assess risk at such sites; however, it is very seldom measured. With this data set, we address how accurately C(pw,EPA-34) can be estimated using limited 16 parent PAH data (EPA-16) commonly available for such sites. An exhaustive statistical analysis of the obtained data validated earlier observations that PAHs with more than 3 rings are present in similar relative abundances and their partitioning behavior typically follows Raoult's law and models developed for coal tar. As a result, sediment and freely dissolved pore water concentrations of pyrene and other 3- and 4-ring PAHs exhibit good log-log correlations (r2 > 0.8) to most individual EPA-34 PAHs and also to C(pw,EPA-34). Correlations improve further by including the ratio of high to low molecular weight PAHs, as 2-ring PAHs exhibit the most variability in terms of their relative abundance. The most practical result of the current work is that log C(pw,EPA-34) estimated by the recommended pyrene-based estimation techniques was similarly well correlated to % survival of the benthic amphipods Hyalella azteca and Leptocheirus plumulosus as directly measured log C(pw,EPA-34) values (n = 211). Incorporation of the presented C(pw,EPA-34) estimation techniques could substantially improve risk assessments and guidelines for sediments impacted by pyrogenic residues, especially when limited data are available, without requiring any extra data or measurement costs.     

Mass budget of perfluorooctane surfactants in Lake Ontario

Perfluorooctane surfactants have been reported in biota, water, and air samples worldwide. Despite these reports, the main environmental sources of these compounds remain undefined. To address this gap in knowledge, an annual lake-wide mass budget of eight perfluorooctane surfactants was developed for Lake Ontario. To determine the atmospheric contribution to the mass budget, over-the-lake gas-phase air concentrations for N-EtFOSE and N-EtFOSA and particulate-phase air concentrations for PFOS in any air sample are reported for the first time, with mean concentrations when present of 0.5+/-0.32 (N-EtFOSE gas-phase), 1.1+/-0.9 (N-EtFOSA gas-phase), and 6.4+/-3.3 (PFOS particulate-phase) pg/m3. The mass budget finds inflow from Lake Erie (14 361+/-4489 kg sigma perfluorooctane surfactants) and wastewater discharge (1762+/-2697 kg sigma perfluorooctane surfactants) to be the major sources, while outflow through the St. Lawrence River is the dominant loss mechanism (22,727+/-7060 kg/year sigma perfluorooctane surfactants). Using the mass budget data, the steady state and measured mean concentrations in the lake water are the same at the 95% confidence level.     

Influence of Asian and Western United States urban areas and fires on the atmospheric transport of polycyclic aromatic hydrocarbons, polychlorinated biphenyls, and fluorotelomer alcohols in the Western United States

Atmospheric measurements of semivolatile organic compounds (SOCs) were made at Mt Bachelor Observatory (MBO), located in Oregon's Cascade Range, to understand the trans-Pacific and regional transport of SOCs from urban areas. High volume air sampling (approximately 644 m3 for 24 h periods) of both the gas and particulate phases was conducted from April 19, 2004 to May 13, 2006 (n = 69); including NASA's INTEX-B campaign in spring 2006 (n = 34 of 69). Air mass back trajectories were calculated and were used to calculate source region impact factors (SRIFs), the percentage of time the sampled air mass resided in a given source region. Particulate-phase polycyclic aromatic hydrocarbon (PAH) concentrations at MBO increased with the percentage of air mass time in Asia and, in conjunction with other data, provided strong evidence that particulate-phase PAHs are emitted from Asia and undergo trans-Pacific atmospheric transport to North America. Gas-phase PAH and fluorotelomer alcohol (FTOH) concentrations significantly increased with the percentage of air mass time in California's urban areas, whereas retene and polychlorinated biphenyl (PCB) concentrations increased with the percentage of air mass time in Oregon and during regional fire events. In addition, sigma(gas-phase) PAH, retene, and levoglucosan concentrations were significantly correlated (p-value < 0.001) with sigma(PCB) concentrations, suggesting that increased atmospheric PCB concentrations were associated with fires due to the volatilization of stored PCBs from soil and vegetation.