Your browser doesn't support javascript.
loading
Show: 20 | 50 | 100
Results 1 - 20 de 147
Filter
Add more filters

Publication year range
1.
Environ Sci Technol ; 58(15): 6772-6780, 2024 Apr 16.
Article in English | MEDLINE | ID: mdl-38577774

ABSTRACT

The quality of chemical analysis is an important aspect of passive sampling-based environmental assessments. The present study reports on a proficiency testing program for the chemical analysis of hydrophobic organic compounds in silicone and low-density polyethylene (LDPE) passive samplers and hydrophilic compounds in polar organic chemical integrative samplers. The median between-laboratory coefficients of variation (CVs) of hydrophobic compound concentrations in the polymer phase were 33% (silicone) and 38% (LDPE), similar to the CVs obtained in four earlier rounds of this program. The median CV over all rounds was 32%. Much higher variabilities were observed for hydrophilic compound concentrations in the sorbent: 50% for the untransformed data and a factor of 1.6 after log transformation. Limiting the data to the best performing laboratories did not result in less variability. Data quality for hydrophilic compounds was only weakly related to the use of structurally identical internal standards and was unrelated to the choice of extraction solvent and extraction time. Standard deviations of the aqueous concentration estimates for hydrophobic compound sampling by the best performing laboratories were 0.21 log units for silicone and 0.27 log units for LDPE (factors of 1.6 to 1.9). The implications are that proficiency testing programs may give more realistic estimates of uncertainties in chemical analysis than within-laboratory quality control programs and that these high uncertainties should be taken into account in environmental assessments.


Subject(s)
Polyethylene , Water Pollutants, Chemical , Polyethylene/analysis , Water Pollutants, Chemical/analysis , Environmental Monitoring/methods , Organic Chemicals , Silicones
2.
Environ Sci Technol ; 2024 Jul 20.
Article in English | MEDLINE | ID: mdl-39031616

ABSTRACT

Polycyclic aromatic hydrocarbons (PAHs), released from petrogenic, pyrogenic or diagenetic sources (degradation of wood materials), are of global concern due to their adverse effects, and potential for long-range transport. While dissolved PAHs have been frequently reported in the literature, there has been no consistent approach of sampling across water bodies. Passive samplers from the AQUA/GAPS-MONET initiative were deployed at 46 sites (28 marine and 18 freshwater), and analyzed for 28 PAHs and six polycyclic musks (PCMs) centrally. Freely dissolved PAH concentrations were dominated by phenanthrene (mean concentration 1500 pg L-1; median 530 pg L-1) and other low molecular weight compounds. Greatest concentrations of phenanthrene, fluoranthene, and pyrene were typically from the same sites, mostly in Europe and North America. Of the PCMs, only galaxolide (72% of samples) and tonalide (61%) were regularly detected, and were significantly cross-correlated. Benchmarking of PAHs relative to penta- and hexachlorobenzene confirmed that the most remote sites (Arctic, Antarctic, and mountain lakes) displayed below average PAH concentrations. Concentrations of 11 of 28 PAHs, galaxolide and tonalide were positively correlated (P < 0.05) with population density within a radius of 5 km of the sampling site. Characteristic PAH ratios gave conflicting results, likely reflecting multiple PAH sources and postemission changes.

3.
Environ Sci Technol ; 57(14): 5544-5557, 2023 04 11.
Article in English | MEDLINE | ID: mdl-36972291

ABSTRACT

Aqueous film-forming foams historically were used during fire training activities on Joint Base Cape Cod, Massachusetts, and created an extensive per- and polyfluoroalkyl substances (PFAS) groundwater contamination plume. The potential for PFAS bioconcentration from exposure to the contaminated groundwater, which discharges to surface water bodies, was assessed with mobile-laboratory experiments using groundwater from the contamination plume and a nearby reference location. The on-site continuous-flow 21-day exposures used male and female fathead minnows, freshwater mussels, polar organic chemical integrative samplers (POCIS), and polyethylene tube samplers (PETS) to evaluate biotic and abiotic uptake. The composition of the PFAS-contaminated groundwater was complex and 9 PFAS were detected in the reference groundwater and 17 PFAS were detected in the contaminated groundwater. The summed PFAS concentrations ranged from 120 to 140 ng L-1 in reference groundwater and 6100 to 15,000 ng L-1 in contaminated groundwater. Biotic concentration factors (CFb) for individual PFAS were species, sex, source, and compound-specific and ranged from 2.9 to 1000 L kg-1 in whole-body male fish exposed to contaminated groundwater for 21 days. The fish and mussel CFb generally increased with increasing fluorocarbon chain length and were greater for sulfonates than for carboxylates. The exception was perfluorohexane sulfonate, which deviated from the linear trend and had a 10-fold difference in CFb between sites, possibly because of biotransformation of precursors such as perfluorohexane sulfonamide. Uptake for most PFAS in male fish was linear over time, whereas female fish had bilinear uptake indicated by an initial increase in tissue concentrations followed by a decrease. Uptake of PFAS was less for mussels (maximum CFb = 200) than for fish, and mussel uptake of most PFAS also was bilinear. Although abiotic concentration factors were greater than CFb, and values for POCIS were greater than for PETS, passive samplers were useful for assessing PFAS that potentially bioconcentrate in fish but are present at concentrations below method quantitation limits in water. Passive samplers also accumulate short-chain PFAS that are not bioconcentrated.


Subject(s)
Fluorocarbons , Groundwater , Water Pollutants, Chemical , Animals , Male , Female , Water Pollutants, Chemical/analysis , Fishes , Water , Fluorocarbons/analysis , Alkanesulfonates , Massachusetts , Polyethylene
4.
Environ Sci Technol ; 57(14): 5592-5602, 2023 04 11.
Article in English | MEDLINE | ID: mdl-36972708

ABSTRACT

Drinking water supplies across the United States have been contaminated by firefighting and fire-training activities that use aqueous film-forming foams (AFFF) containing per- and polyfluoroalkyl substances (PFAS). Much of the AFFF is manufactured using electrochemical fluorination by 3M. Precursors with six perfluorinated carbons (C6) and non-fluorinated amine substituents make up approximately one-third of the PFAS in 3M AFFF. C6 precursors can be transformed through nitrification (microbial oxidation) of amine moieties into perfluorohexane sulfonate (PFHxS), a compound of regulatory concern. Here, we report biotransformation of the most abundant C6 sulfonamido precursors in 3M AFFF with available commercial standards (FHxSA, PFHxSAm, and PFHxSAmS) in microcosms representative of the groundwater/surface water boundary. Results show rapid (<1 day) biosorption to living cells by precursors but slow biotransformation into PFHxS (1-100 pM day-1). The transformation pathway includes one or two nitrification steps and is supported by the detection of key intermediates using high-resolution mass spectrometry. Increasing nitrate concentrations and total abundance of nitrifying taxa occur in parallel with precursor biotransformation. Together, these data provide multiple lines of evidence supporting microbially limited biotransformation of C6 sulfonamido precursors involving ammonia-oxidizing archaea (Nitrososphaeria) and nitrite-oxidizing bacteria (Nitrospina). Further elucidation of interrelationships between precursor biotransformation and nitrogen cycling in ecosystems would help inform site remediation efforts.


Subject(s)
Fluorocarbons , Groundwater , Water Pollutants, Chemical , Ecosystem , Water Pollutants, Chemical/analysis , Groundwater/chemistry , Biotransformation , Fluorocarbons/analysis , Alkanesulfonates
5.
Environ Sci Technol ; 57(25): 9342-9352, 2023 06 27.
Article in English | MEDLINE | ID: mdl-37294896

ABSTRACT

Persistent organic pollutants (POPs) are recognized as pollutants of global concern, but so far, information on the trends of legacy POPs in the waters of the world has been missing due to logistical, analytical, and financial reasons. Passive samplers have emerged as an attractive alternative to active water sampling methods as they accumulate POPs, represent time-weighted average concentrations, and can easily be shipped and deployed. As part of the AQUA-GAPS/MONET, passive samplers were deployed at 40 globally distributed sites between 2016 and 2020, for a total of 21 freshwater and 40 marine deployments. Results from silicone passive samplers showed α-hexachlorocyclohexane (HCH) and γ-HCH displaying the greatest concentrations in the northern latitudes/Arctic Ocean, in stark contrast to the more persistent penta (PeCB)- and hexachlorobenzene (HCB), which approached equilibrium across sampling sites. Geospatial patterns of polychlorinated biphenyl (PCB) aqueous concentrations closely matched original estimates of production and use, implying limited global transport. Positive correlations between log-transformed concentrations of Σ7PCB, ΣDDTs, Σendosulfan, and Σchlordane, but not ΣHCH, and the log of population density (p < 0.05) within 5 and 10 km of the sampling sites also supported limited transport from used sites. These results help to understand the extent of global distribution, and eventually time-trends, of organic pollutants in aquatic systems, such as across freshwaters and oceans. Future deployments will aim to establish time-trends at selected sites while adding to the geographical coverage.


Subject(s)
Air Pollutants , Environmental Pollutants , Hydrocarbons, Chlorinated , Pesticides , Polychlorinated Biphenyls , Polychlorinated Biphenyls/analysis , Environmental Monitoring/methods , Hexachlorobenzene/analysis , Fresh Water , Air Pollutants/analysis , Pesticides/analysis , Hydrocarbons, Chlorinated/analysis
6.
Environ Sci Technol ; 57(48): 19066-19077, 2023 Dec 05.
Article in English | MEDLINE | ID: mdl-37943968

ABSTRACT

Pollution by chemicals and waste impacts human and ecosystem health on regional, national, and global scales, resulting, together with climate change and biodiversity loss, in a triple planetary crisis. Consequently, in 2022, countries agreed to establish an intergovernmental science-policy panel (SPP) on chemicals, waste, and pollution prevention, complementary to the existing intergovernmental science-policy bodies on climate change and biodiversity. To ensure the SPP's success, it is imperative to protect it from conflicts of interest (COI). Here, we (i) define and review the implications of COI, and its relevance for the management of chemicals, waste, and pollution; (ii) summarize established tactics to manufacture doubt in favor of vested interests, i.e., to counter scientific evidence and/or to promote misleading narratives favorable to financial interests; and (iii) illustrate these with selected examples. This analysis leads to a review of arguments for and against chemical industry representation in the SPP's work. We further (iv) rebut an assertion voiced by some that the chemical industry should be directly involved in the panel's work because it possesses data on chemicals essential for the panel's activities. Finally, (v) we present steps that should be taken to prevent the detrimental impacts of COI in the work of the SPP. In particular, we propose to include an independent auditor's role in the SPP to ensure that participation and processes follow clear COI rules. Among others, the auditor should evaluate the content of the assessments produced to ensure unbiased representation of information that underpins the SPP's activities.


Subject(s)
Conflict of Interest , Ecosystem , Humans , Environmental Pollution , Biodiversity
7.
Mar Chem ; 257: 1-11, 2023 Nov 20.
Article in English | MEDLINE | ID: mdl-38274497

ABSTRACT

Black carbon (BC) is ubiquitous in pelagic sediments and presumed to have an older radiocarbon age due to long ocean residence times and pre-aging in terrestrial soils. Here, we analyzed sediments from five regions in the subtropical Atlantic Ocean to quantify the black carbon fraction of the total organic carbon pool. Black carbon, derived from the chemothermal oxidation method, comprised between 17±6% of the sedimentary organic carbon in the Northwest Argentina Basin and 65±18% in the Amazon Delta. Black carbon sediment accumulation rates were six times greater in the Sierra Leone Rise (8.4±4.1 mg cm-2 kyr-1) compared to the remote Northwest Argentina Basin (1.3±0.4 mg cm-2 kyr-1), possibly due to enhanced regional atmospheric deposition from annual African grassland fires. The radiocarbon age for BC from subtropical Atlantic sediments were more modern compared to the bulk total organic carbon, and BC source was apportioned as biomass burning byproducts from their stable carbon isotopic signatures and characteristic ratios of polycyclic aromatic hydrocarbons. This study demonstrated that subtropical Atlantic Ocean sediments serve as an important sink for young BC.

8.
Environ Sci Technol ; 56(22): 15573-15583, 2022 11 15.
Article in English | MEDLINE | ID: mdl-36280234

ABSTRACT

Per- and polyfluoroalkyl substances (PFAS) are a diverse class of fluorinated anthropogenic chemicals that include perfluoroalkyl acids (PFAA), which are widely used in modern commerce. Many products and environmental samples contain abundant precursors that can degrade into terminal PFAA associated with adverse health effects. Fish consumption is an important dietary exposure source for PFAS that bioaccumulate in food webs. However, little is known about bioaccumulation of PFAA precursors. Here, we identify and quantify PFAS in recreational fish species collected from surface waters across New Hampshire, US, using a toolbox of analytical methods. Targeted analysis of paired water and tissue samples suggests that many precursors below detection in water have a higher bioaccumulation potential than their terminal PFAA. Perfluorobutane sulfonamide (FBSA), a short-chain precursor produced by electrochemical fluorination, was detected in all fish samples analyzed for this compound. The total oxidizable precursor assay interpreted using Bayesian inference revealed fish muscle tissue contained additional, short-chain precursors in high concentration samples. Suspect screening analysis indicated these were perfluoroalkyl sulfonamide precursors with three and five perfluorinated carbons. Fish consumption advisories are primarily being developed for perfluorooctane sulfonate (PFOS), but this work reinforces the need for risk evaluations to consider additional bioaccumulative PFAS, including perfluoroalkyl sulfonamide precursors.


Subject(s)
Alkanesulfonic Acids , Fluorocarbons , Water Pollutants, Chemical , Animals , Fluorocarbons/analysis , Bioaccumulation , Bayes Theorem , Water Pollutants, Chemical/analysis , Fishes/metabolism , Fresh Water , Water/metabolism , Sulfonamides/metabolism
9.
Environ Sci Technol ; 56(10): 6232-6242, 2022 05 17.
Article in English | MEDLINE | ID: mdl-34608797

ABSTRACT

Per- and polyfluoroalkyl substances (PFAS) are a class of substances for which there are widespread concerns about their extreme persistence in combination with toxic effects. It has been argued that PFAS should only be employed in those uses that are necessary for health or safety or are critical for the functioning of society and where no alternatives are available ("essential-use concept"). Implementing the essential-use concept requires a sufficient understanding of the current uses of PFAS and of the availability, suitability, and hazardous properties of alternatives. To illustrate the information requirements under the essential-use concept, we investigate seven different PFAS uses, three in consumer products and four industrial applications. We investigate how much information is available on the types and functions of PFAS in these uses, how much information is available on alternatives, their performance and hazardous properties and, finally, whether this information is sufficient as a basis for deciding on the essentiality of a PFAS use. The results show (i) the uses of PFAS are highly diverse and information on alternatives is often limited or lacking; (ii) PFAS in consumer products often are relatively easy to replace; (iii) PFAS uses in industrial processes can be highly complex and a thorough evaluation of the technical function of each PFAS and of the suitability of alternatives is needed; (iv) more coordination among PFAS manufacturers, manufacturers of alternatives to PFAS, users of these materials, government authorities, and other stakeholders is needed to make the process of phasing out PFAS more transparent and coherent.


Subject(s)
Fluorocarbons
10.
Anal Bioanal Chem ; 414(3): 1235-1243, 2022 Jan.
Article in English | MEDLINE | ID: mdl-34355253

ABSTRACT

There is widespread contamination by per- and polyfluoroalkyl substances (PFAS) across the globe, with adverse effects on human and environmental health. For human exposure, drinking water and dietary exposure have been recognized as important PFAS exposure pathway for the general population. Several documented cases of dairy milk contamination by PFAS have raised concerns over this exposure pathway in general. A sensitive method for determination of 27 PFAS in milk was hence modified and applied on raw and processed milk samples from 13 farms across the United States (U.S.). A combination of acid and basic extraction method and ENVI-Carb clean-up achieved recoveries of targeted PFAS between 70 and 141%. The method detection limits (MDL) ranged from 0.8 to 22 ng/L (for 26 PFAS) and 144 ng/L for perfluorobutanoic acid (PFBA). The uniqueness of this method is considered in the targeted screening of a broad range of legacy PFAS, as well as perfluorinated sulfonamide species and fluorotelomer sulfonates. No legacy PFAS were detected in 13 milk samples from regions of concern given local use of biosolids or proximity to fire training areas. Overall, then, the uptake of perfluoroalkyl acids (PFAA) from dairy milk in the U.S. is considered low.


Subject(s)
Fluorocarbons/analysis , Food Contamination/analysis , Milk/chemistry , Tandem Mass Spectrometry/methods , Animals , Cattle , Chromatography, Liquid/methods , Dairying , Food Analysis/methods , Limit of Detection
11.
Environ Sci Technol ; 55(14): 9518-9526, 2021 07 20.
Article in English | MEDLINE | ID: mdl-33826304

ABSTRACT

The time trend of α- and γ-hexachlorocyclohexane (HCH) isomers in Lake Superior water was followed from 1986 to 2016, the longest record for any persistent organic pollutant (POP) in Great Lakes water. Dissipation of α-HCH and γ-HCHs was first order, with halving times (t1/2) of 5.7 and 8.5 y, respectively. Loss rates were not significantly different starting a decade later (1996-2016). Concentrations of ß-HCH were followed from 1996-2016 and dissipated more slowly (t1/2 = 16 y). In 1986, the lake contained an estimated 98.8 tonnes of α-HCH and 13.2 tonnes of γ-HCH; by 2016, only 2.7% and 7.9% of 1986 quantities remained. Halving times of both isomers in water were longer than those reported in air, and for γ-HCH, they were longer in water than those reported in lake trout. Microbial degradation was evident by enantioselective depletion of (+)α-HCH, which increased from 1996 to 2011. Volatilization was the main removal process for both isomers, followed by degradation (hydrolytic and microbial) and outflow through the St. Mary's River. Sedimentation was minor. Major uncertainties in quantifying removal processes were in the two-film model for predicting volatilization and in microbial degradation rates. The study highlights the value of long-term monitoring of chemicals in water to interpreting removal processes and trends in biota.


Subject(s)
Pesticides , Water Pollutants, Chemical , Hexachlorocyclohexane/analysis , Lakes , Pesticides/analysis , Water , Water Pollutants, Chemical/analysis
12.
Environ Sci Technol ; 55(14): 9498-9507, 2021 07 20.
Article in English | MEDLINE | ID: mdl-33147956

ABSTRACT

Oceans have remained the least well-researched reservoirs of persistent organic pollutants (POPs) globally, due to their vast scale, difficulty of access, and challenging (trace) analysis. Little data on POPs exists along South America and the effect of different currents and river plumes on aqueous concentrations. Research cruise KN210-04 (R/V Knorr) offered a unique opportunity to determine POP gradients in air, water, and their air-water exchange along South America, covering both hemispheres. Compounds of interest included polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs), polybrominated diphenylethers (PBDEs), and polycyclic aromatic hydrocarbons (PAHs). Remote tropical Atlantic Ocean atmospheric concentrations varied little between both hemispheres; for HCB, BDEs 47 and 99, they were ∼5 pg/m3, PCBs were ∼1 pg/m3, α-HCH was ∼0.2 pg/m3, and phenanthrene and other PAHs were in the low 100s pg/m3. Aqueous concentrations were dominated by PCB 52 (mean 4.1 pg/L), HCB (1.6 pg/L), and ß-HCH (1.9 pg/L), with other compounds <1 pg/L. Target PCBs tended to undergo net volatilization from the surface ocean, while gradients indicated net deposition for a-HCH. In contrast to atmospheric concentrations, which were basically unchanged between hemispheres, we detected strong gradients in aqueous POPs, with mostly nondetects in the tropical western South Atlantic. These results highlight the importance of currents and loss processes on ocean scales for the distribution of POPs.


Subject(s)
Air Pollutants , Environmental Pollutants , Hydrocarbons, Chlorinated , Pesticides , Polychlorinated Biphenyls , Air Pollutants/analysis , Atlantic Ocean , Environmental Monitoring , Hydrocarbons, Chlorinated/analysis , Oceans and Seas , Pesticides/analysis , Polychlorinated Biphenyls/analysis , Water
13.
Environ Sci Technol ; 55(19): 12755-12765, 2021 10 05.
Article in English | MEDLINE | ID: mdl-34519210

ABSTRACT

Despite decades of research on per- and polyfluoroalkyl substances (PFAS), fundamental obstacles remain to addressing worldwide contamination by these chemicals and their associated impacts on environmental quality and health. Here, we propose six urgent questions relevant to science, technology, and policy that must be tackled to address the "PFAS problem": (1) What are the global production volumes of PFAS, and where are PFAS used? (2) Where are the unknown PFAS hotspots in the environment? (3) How can we make measuring PFAS globally accessible? (4) How can we safely manage PFAS-containing waste? (5) How do we understand and describe the health effects of PFAS exposure? (6) Who pays the costs of PFAS contamination? The importance of each question and barriers to progress are briefly described, and several potential paths forward are proposed. Given the diversity of PFAS and their uses, the extreme persistence of most PFAS, the striking ongoing lack of fundamental information, and the inequity of the health and environmental impacts from PFAS contamination, there is a need for scientific and regulatory communities to work together, with cooperation from PFAS-related industries, to fill in critical data gaps and protect human health and the environment.


Subject(s)
Fluorocarbons , Humans
14.
Environ Sci Technol ; 54(20): 12820-12828, 2020 10 20.
Article in English | MEDLINE | ID: mdl-33043667

ABSTRACT

Fluoropolymers are a group of polymers within the class of per- and polyfluoroalkyl substances (PFAS). The objective of this analysis is to evaluate the evidence regarding the environmental and human health impacts of fluoropolymers throughout their life cycle(s). Production of some fluoropolymers is intimately linked to the use and emissions of legacy and novel PFAS as polymer processing aids. There are serious concerns regarding the toxicity and adverse effects of fluorinated processing aids on humans and the environment. A variety of other PFAS, including monomers and oligomers, are emitted during the production, processing, use, and end-of-life treatment of fluoropolymers. There are further concerns regarding the safe disposal of fluoropolymers and their associated products and articles at the end of their life cycle. While recycling and reuse of fluoropolymers is performed on some industrial waste, there are only limited options for their recycling from consumer articles. The evidence reviewed in this analysis does not find a scientific rationale for concluding that fluoropolymers are of low concern for environmental and human health. Given fluoropolymers' extreme persistence; emissions associated with their production, use, and disposal; and a high likelihood for human exposure to PFAS, their production and uses should be curtailed except in cases of essential uses.


Subject(s)
Fluorocarbons , Environmental Health , Fluorocarbons/analysis , Humans , Polyethylene
15.
Environ Sci Technol ; 54(20): 12938-12948, 2020 10 20.
Article in English | MEDLINE | ID: mdl-32894676

ABSTRACT

Per- and polyfluoroalkyl substances (PFAS) are anthropogenic, globally distributed chemicals. Legacy PFAS, including perfluorooctane sulfonate (PFOS), have been regularly detected in marine fauna but little is known about their current levels or the presence of novel PFAS in seabirds. We measured 36 emerging and legacy PFAS in livers from 31 juvenile seabirds from Massachusetts Bay, Narragansett Bay, and the Cape Fear River Estuary (CFRE), United States. PFOS was the major legacy perfluoroalkyl acid present, making up 58% of concentrations observed across all habitats (range: 11-280 ng/g). Novel PFAS were confirmed in chicks hatched downstream of a fluoropolymer production site in the CFRE: a perfluorinated ether sulfonic acid (Nafion byproduct 2; range: 1-110 ng/g) and two perfluorinated ether carboxylic acids (PFO4DA and PFO5DoDA; PFO5DoDA range: 5-30 ng/g). PFOS was inversely associated with phospholipid content in livers from CFRE and Massachusetts Bay individuals, while δ 13C, an indicator of marine versus terrestrial foraging, was positively correlated with some long-chain PFAS in CFRE chick livers. There is also an indication that seabird phospholipid dynamics are negatively impacted by PFAS, which should be further explored given the importance of lipids for seabirds.


Subject(s)
Alkanesulfonic Acids , Fluorocarbons , Water Pollutants, Chemical , Alkanesulfonic Acids/analysis , Animals , Birds , Environmental Monitoring , Fluorocarbons/analysis , Humans , Massachusetts , Rivers , Sulfonic Acids/analysis , United States , Water Pollutants, Chemical/analysis
16.
Environ Sci Technol ; 53(21): 12348-12356, 2019 Nov 05.
Article in English | MEDLINE | ID: mdl-31565932

ABSTRACT

The ocean is thought to be the terminal sink for poly- and perfluoroalkyl substances (PFAS) that have been produced and released in large quantities for more than 60 years. Regulatory actions have curbed production of legacy compounds such as perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA), but impacts of regulations on PFAS releases to the marine environment are poorly understood. Here, we report new data for 21 targeted PFAS in seawater and plankton from the coast, shelf, and slope of the Northwestern Atlantic Ocean. We find strong inverse correlations between salinity and concentrations of most PFAS, indicating that ongoing continental discharges are the major source to the marine environment. For legacy PFAS such as PFOS and PFOA, a comparison of inland and offshore measurements from the same year (2014) suggests that there are ongoing releases to the marine environment from sources such as submarine groundwater discharges. Vertical transport of most PFAS associated with settling particles from the surface (10 m) to deeper waters is small compared to advective transport except for perfluorodecanoic acid (PFDA; 35% of vertical flux) and precursor compounds to PFOS (up to 86%). We find higher than expected bioaccumulation factors (BAFs = Cplankton/Cwater) for perfluorinated carboxylic acids (PFCAs) with five and six carbons (log BAF = 2.9-3.4) and linear PFOS (log BAF = 2.6-4.3) in marine plankton compared to PFCAs with 7-11 carbons. We postulate that this reflects additional contributions from precursor compounds. Known precursor compounds detected here have among the highest BAFs (log BAF > 3.0) for all PFAS in this study, suggesting that additional research on the bioaccumulation potential of unknown organofluorine compounds is urgently needed.


Subject(s)
Alkanesulfonic Acids , Fluorocarbons , Water Pollutants, Chemical , Atlantic Ocean , Environmental Monitoring , Plankton , Seawater
17.
Bull Environ Contam Toxicol ; 103(6): 770-775, 2019 Dec.
Article in English | MEDLINE | ID: mdl-31620816

ABSTRACT

Little is known about the presence and effects of polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in Puerto Rico's waters. Four coastal aquatic systems were investigated using low-density polyethylene passive sampling for PCBs and OCPs in water and its overlying air. The highest total freely dissolved and gaseous concentrations of PCBs were found in Guánica Bay, with 4000 pg/L and 270 pg/m3, respectively. Five OCPs were detected, mainly in water, with greatest concentrations (pg/L) in Guánica Bay: α-HCH (7400), p,p'-DDE (390), aldrin (2000), dieldrin (420), and endrin (77). The compound α-HCH was also measured at elevated water concentrations in Condado Lagoon (5700 pg/L) and Laguna Grande (2900 pg/L). Jobos Bay did not show values of concern for these persistence organic pollutants. Levels of PCBs and OCPs in water, particularly in Guánica Bay, exceeded USEPA ambient water quality criteria values representing a human health risk regarding consumption of aquatic organisms.


Subject(s)
Bays/chemistry , Environmental Monitoring/methods , Hydrocarbons, Chlorinated/analysis , Pesticides/analysis , Seawater/chemistry , Water Pollutants, Chemical/analysis , Humans , Pilot Projects , Polychlorinated Biphenyls/analysis , Puerto Rico
18.
Environ Sci Technol ; 52(24): 14061-14069, 2018 12 18.
Article in English | MEDLINE | ID: mdl-30433769

ABSTRACT

The largest fresh water body in North America, Lake Superior, has the potential to both accumulate and serve as a secondary source of persistent bioaccumulative toxins, such as polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs). Polyethylene passive samplers (PEs) were thus simultaneously deployed at 19 sites in surface water and near surface atmosphere across Lake Superior to determine air and water concentrations and air-water gradients of 18 PCBs and 24 OCPs. PCBs in the air and water were characterized by penta- and hexachlorobiphenyls with distribution along the coast correlated with proximity to developed areas. Surface water and atmospheric concentrations were dominated by α-HCH (average 250 pg L-1 and 4.2 pg m-3, respectively), followed by HCB (average 17 pg L-1 and 89 pg m-3, respectively). Decreases in open lake concentrations of PCBs in water and air from spring to summer were consistent with ongoing volatilization from the surface layer as the main cause. Conversely, α-endosulfan was consistently deposited into the surface water of Lake Superior. Results indicated that PCBs were depleted in the surface mixed layer, implying a physical limit on evasive fluxes. This was corroborated with measurements from a vertical profile, displaying greater PCB concentrations at depth.


Subject(s)
Air Pollutants , Hydrocarbons, Chlorinated , Pesticides , Polychlorinated Biphenyls , Water Pollutants, Chemical , Environmental Monitoring , Lakes , North America , Water
19.
Environ Sci Technol ; 52(11): 6208-6216, 2018 06 05.
Article in English | MEDLINE | ID: mdl-29787253

ABSTRACT

Organophosphate esters (OPEs) have been found in remote environments at unexpectedly high concentrations, but very few measurements of OPE concentrations in seawater are available, and none are available in subsurface seawater. In this study, passive polyethylene samplers (PEs) deployed on deep-water moorings in the Fram Strait and in surface waters of Canadian Arctic lakes and coastal sites were analyzed for a suite of common OPEs. Total OPEs ( ∑11OPE) at deep-water sites were dominated by chlorinated OPEs, and ranged from 6.3 to 440 pg/L. Concentrations were similar in eastern and western Fram Strait. Chlorinated OPEs were also dominant in Canadian Arctic surface waters (mean concentration ranged from < DL to 4400 pg/L), while nonhalogenated alkyl/aryl-substituted OPEs remained low (1.3-55 pg/L), possibly due to the greater long-range transport potential of chlorinated OPEs. Polybrominated diphenyl ethers (PBDEs) were found at much lower concentrations than OPEs (

Subject(s)
Flame Retardants , Halogenated Diphenyl Ethers , Arctic Regions , Canada , Environmental Monitoring , Esters , Organophosphates
SELECTION OF CITATIONS
SEARCH DETAIL