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Widespread detection of N, N-diethyl-m-toluamide in U.S. streams: Comparison with concentrations of pesticides, personal care products, and other organic wastewater compounds

One of the most frequently detected organic chemicals in a nationwide study concerning the effects of wastewater on stream water quality conducted in the year 2000 was the widely used insect repellant N , N -diethyl- m -toluamide (DEET). It was detected at levels of 0.02 μg/L or greater in 73% of the stream sites sampled, with the selection of sampling sites being biased toward streams thought to be subject to wastewater contamination (i.e., downstream from intense urbanization and livestock production). Although DEET frequently was detected at all sites, the median concentration was low (0.05 μg/L). The highest concentrations of DEET were found in streams from the urban areas (maximum concentration, 1.1 μg/L). The results of the present study suggest that the movement of DEET to streams through wastewater-treatment systems is an important mechanism that might lead to the exposure of aquatic organisms to this chemical.

Environmental Toxicology and Chemistry

A field assessment of long-term laboratory sediment toxicity tests with the amphipod Hyalella azteca

Response of the amphipod Hyalella azteca exposed to contaminated sediments for 10 to 42 d in laboratory toxicity tests was compared to responses observed in controlled three-month invertebrate colonization exposures conducted in a pond. Sediments evaluated included a sediment spiked with dichlorodiphenyldichloroethane (DDD) or dilutions of a field sediment collected from the Grand Calumet River (GCR) in Indiana (USA) (contaminated with organic compounds and metals). Consistent effects were observed at the highest exposure concentrations (400 ??g DDD/goc [DDD concentrations normalized to grams of organic carbon (goc) in sedimentl or 4% GCR sediment) on survival, length, and reproduction of amphipods in the laboratory and on abundance of invertebrates colonizing sediments in the field. Effect concentrations for DDD observed for 10-d length and 42-d reproduction of amphipods (e.g., chronic value [ChV] of 66 ??g DDD/goc and 25% inhibition concentration [IC25] of 68 ??g DDD/goc for reproduction) were similar to the lowest effect concentrations for DDD measured on invertebrates colonizing sediment the field. Effect concentrations for GCR sediment on 28-d survival and length and 42-d reproduction and length of amphipods (i.e., ChVs of 0.20-0.66% GCR sediment) provided more conservative effect concentrations compared to 10-d survival or length of amphipods in the laboratory or the response of invertebrates colonizing sediment in the field (e.g., ChVs of 2.2% GCR sediment). Results of this study indicate that use of chronic laboratory toxicity tests with H. azteca and benthic colonization studies should be used to provide conservative estimates of impacts on benthic communities exposed to contaminated sediments. Bioaccumulation of DDD by oligochaetes colonizing the DDD-spiked sediment was similar to results of laboratory sediment tests previously conducted with the oligochaete Lumbriculus variegates, confirming that laboratory exposures can be used to estimate bioaccumulation by oligochaetes exposed in the field. ?? 2005 SETAC.

Environmental Toxicology and Chemistry

Acute and chronic toxicity of lead in water and diet to the amphipod Hyalella azteca

We evaluated the influence of waterborne and dietary lead (Pb) exposure on the acute and chronic toxicity of Pb to the amphipod Hyalella azteca . Test solutions were generated by a modified diluter with an extended (24‐h) equilibration period. Acute (96‐h) toxicity of Pb varied with water hardness in the range of 71 to 275 mg/L as CaCO 3 , despite similar dissolved Pb concentrations. Acute toxicity was greatest in soft test water, with less than 50% survival at the lowest dissolved Pb concentration (151 μg/L). Survival also was significantly reduced in medium‐hardness water but not in hard test water. In chronic (42‐d) studies, amphipods were exposed to waterborne Pb and fed either a control diet or a diet equilibrated with waterborne Pb levels. For animals fed the control diet, the median lethal concentration (LC50) for Pb was 24 μg/L (as dissolved Pb), and significant reductions in survival occurred at 16 μg/L. Exposure to Pb‐treated diets significantly increased toxicity across a wide range of dissolved Pb concentrations, with a LC50 of 16 μg/L and significant reductions in growth and reproduction at 3.5 μg/L. Significant effects on growth and reproduction occurred at dissolved Pb concentrations close to the current U.S. chronic water‐quality criterion. Our results suggest that both aqueous‐ and dietary‐exposure pathways contribute significantly to chronic Pb exposure and toxic effects in aquatic biota.

Environmental Toxicology and Chemistry

Absorption of p,p'-dichlorodiphenyldichloroethylene and dieldrin in largemouth bass from a 60-D slow-release pellet and detection using a novel enzyme-linked immunosorbent assay method for blood plasma

This work describes the uptake of two organochlorine pesticides from slow-release pellets by largemouth bass and the utility of a blood plasma enzyme-linked immunosorbent assay (ELISA) method for exposure verification. We measured blood and tissue levels by gas chromatography/mass spectrometry and by a novel ELISA method, and present a critical comparison of the results.

Environmental Toxicology and Chemistry

Influence of water temperature on acetylcholinesterase activity in the pacific tree frog ( Hyla regilla )

This investigation evaluated whether acetylcholinesterase (AChE) in Pacific tree frogs ( Hyla regilla ) from different geographical locations was influenced by different temperatures during early aquatic life stages, independent of pesticide exposure. Tadpoles were collected from both a California coastal pond and a Sierra Nevada mountain range pond, USA. Groups of frogs from each location were raised in temperatures representative of either the Sierra Nevada (8°C) or the coastal (19°C) location. Metamorphs from both locations raised as tadpoles at 19°C had AChE activities of 42.3 and 38.7 nm/min/mg protein, while those raised as tadpoles at 8°C had activities of 26.9 and 28.2 nm/min/mg protein. A two-way analysis of variance revealed temperature to be the significant factor in determining AChE activity ( F = 22.3, p < 0.001), although origin was not important ( F = 0.09, p = 0.75). Interpretations regarding the influence of pesticides upon AChE activity in Pacific tree frogs must consider the influence of environmental temperature to enable cross-population comparisons.

Environmental Toxicology and Chemistry

Metamorphosis of two amphibian species after chronic cadmium exposure in outdoor aquatic mesocosms

Amphibian larvae at contaminated sites may experience an alteration of metamorphic traits and survival compared to amphibians in uncontaminated conditions. Effects of chronic cadmium (Cd) exposure on the metamorphosis of American toads ( Bufo americanus ) and southern leopard frogs ( Rana sphenocephala ) were determined. The two species were reared separately from shortly after hatching through metamorphosis in outdoor mesocosms (1,325-L polyethylene cattle tanks) that simulated natural ponds and enhanced environmental realism relative to the laboratory. Both species exhibited a decrease in survival with increasing initial nominal aqueous Cd concentration. Cadmium treatment did not influence mass at metamorphosis for either species when survival was included as a covariate, but increased the age at metamorphosis for the American toads. The whole body Cd content of metamorphs increased with aqueous Cd treatment level for both species, and the American toads tended to possess more elevated residues. Cadmium quickly partitioned out of the water column and accumulated in and altered the abundance of the tadpoles' diet. Cadmium-contaminated sites may produce fewer metamorphs, and those that survive will metamorphose later and contain Cd. Interspecific differences in the response variables illustrate the importance of testing multiple species when assessing risk.

Environmental Toxicology and Chemistry

Delineating copper accumulation pathways for the freshwater bivalve Corbicula using stable copper isotopes

Delineation of metal uptake routes in aquatic invertebrates is critical for characterizing bioaccumulation dynamics and assessing risks associated with metal exposure. Here we demonstrate that Cu stable isotopic ratios can be manipulated in both exposure media and algae to determine the efflux rate constant ( k e ) and to estimate Cu assimilation efficiency (AE) from ingested food in a freshwater bivalve ( Corbicula fluminea ). The Cu AE in Corbicula fed 65 Cu‐spiked Cryptomonas ozolini was 38%. Copper uptake routes had no significant influence on efflux; k e of 0.004 per day characterized the slowest component of efflux following short‐term exposures to 65 Cu in water or in both food and water. Incorporation of the physiological parameters for dietary and dissolved uptake as well as rate constants of loss into a bioaccumulation model allowed for assessing the relative contribution of water and food as Cu sources. At [ 65 Cu 2+ ] of 6.7 μg/L, Corbicula accumulated twice as much Cu from diet as from water. In most freshwater systems, the dietary pathway is likely to act as the major Cu uptake route for Corbicula . Extrapolation of our laboratory results to the San Francisco Bay—Delta (California, USA) indicated that our biodynamic model and the laboratory‐derived parameters for dietary 65 Cu uptake provided a realistic representation of the processes involved in Cu accumulation by the bivalve Corbicula .

Environmental Toxicology and Chemistry

Interlaboratory evaluation of Hyalella azteca and Chironomus tentans short-term and long-term sediment toxicity tests

Methods for assessing the long-term toxicity of sediments to Hyalella azteca and Chironomus tentans can significantly enhance the capacity to assess sublethal effects of contaminated sediments through multiple endpoints. Sublethal tests allow us to begin to understand the relationship between short-term and long-term effects for toxic sediments. We present an interlaboratory evaluation with long-term and 10-d tests using control and contaminated sediments in which we assess whether proposed and existing performance criteria (test acceptability criteria [TAC]) could be achieved. Laboratories became familiar with newly developed, long-term protocols by testing two control sediments in phase 1. In phase 2, the 10-d and long-term tests were examined with several sediments. Laboratories met the TACs, but results varied depending on the test organism, test duration, and endpoints. For the long-term tests in phase 1, 66 to 100% of the laboratories consistently met the TACs for survival, growth, or reproduction using H. azteca , and 70 to 100% of the laboratories met the TACs for survival and growth, emergence, reproduction, and hatchability using C. tentans . In phase 2, fewer laboratories participated in long-term tests: 71 to 88% of the laboratories met the TAC for H. azteca , whereas 50 to 67% met the TAC for C. tentans . In the 10-d tests with H. azteca , and C. tentans , 82 and 88% of the laboratories met the TAC for survival, respectively, and 80% met the TAC for C. tentans growth. For the 10-d and long-term tests, laboratories predicted similar toxicity. Overall, the interlaboratory evaluation showed good precision of the methods, appropriate endpoints were incorporated into the test protocols, and tests effectively predicted the toxicity of sediments.

Environmental Toxicology and Chemistry

Source apportionment modeling of volatile organic compounds in streams

It often is of interest to understand the relative importance of the different sources contributing to the concentration cw of a contaminant in a stream; the portions related to sources 1, 2, 3, etc. are denoted cw,1, cw,2, cw,3, etc. Like c w, 'he fractions ??1, = cw,1/c w, ??2 = cw,2/cw, ??3 = cw,3/cw, etc. depend on location and time. Volatile organic compounds (VOCs) can undergo absorption from the atmosphere into stream water or loss from stream water to the atmosphere, causing complexities affecting the source apportionment (SA) of VOCs in streams. Two SA rules are elaborated. Rule 1: VOC entering a stream across the air/water interface exclusively is assigned to the atmospheric portion of cw. Rule 2: VOC loss by volatilization, flow loss to groundwater, in-stream degradation, etc. is distributed over cw,1 cw,2, c w,3, etc. in proportion to their corresponding ?? values. How the two SA rules are applied, as well as the nature of the SA output for a given case, will depend on whether transport across the air/water interface is handled using the net flux F convention or using the individual fluxes J convention. Four hypothetical stream cases involving acetone, methyl-tert-butyl ether (MTBE), benzene, chloroform, and perchloroethylene (PCE) are considered. Acetone and MTBE are sufficiently water soluble from air for a domestic atmospheric source to be capable of yielding cw values approaching the common water quality guideline range of 1 to 10 ??g/L. For most other VOCs, such levels cause net outgassing (F > 0). When F > 0 in a given section of stream, in the net flux convention, all of the ??j, for the compound remain unchanged over that section while cw decreases. A characteristic time ??d can be calculated to predict when there will be differences between SA results obtained by the net flux convention versus the individual fluxes convention. Source apportionment modeling provides the framework necessary for comparing different strategies for mitigating contamination at points of interest along a stream. ?? 2006 SETAC.

Environmental Toxicology and Chemistry

Influence of metal exposure history on the bioaccumulation and subcellular distribution of aqueous cadmium in the insect Hydropsyche californica

The influence of metal exposure history on rates of aqueous Cd accumulation, elimination, and subcellular distribution was examined in the aquatic insect Hydropsyche californica . Specimens were obtained from a reference site and a metal‐contaminated site and returned to the laboratory where they were continuously exposed to aqueous Cd (518 ng/L, nominal) for 6 d, followed by 9 d of depuration. Rates of Cd accumulation and elimination were similar in insects from the two sites. Efflux rate constants, k e , ranged from 0.20 to 0.24/d ( t 1/2 ≈ 3 d). Immediately following exposure, the cytosol accounted for 40% of the body burden in insects from both sites; however, 89 ± 2% of the cytosolic Cd was associated with metallothionein‐like proteins (MTLP) in insects from the contaminated site, compared to 60 ± 0% in insects from the reference site. The concentration of Cd bound to non‐MTLPs (representing potentially Cd‐sensitive proteins) was significantly greater in the insects from the reference site (134 ± 7 ng/g) than in those from the contaminated site (42 ± 2 ng/g). At the end of the depuration period, 90% of the accumulated Cd body burden had been eliminated, and Cd concentrations in MTLPs and non‐MTLPs were similar between the sites. Results suggested that differences in exposure history had no influence on the bioaccumulation of Cd, but did affect the concentrations of Cd bound to MTLP during Cd exposure in these insects.

Environmental Toxicology and Chemistry

Dietary exposure of mink (Mustela vison) to fish from the Housatonic River, Berkshire County, Massachusetts, USA: Effects on organ weights and histology and hepatic concentrations of polychlorinated biphenyls and 2,3,7,8-tetrachlorodibenzo-p-dioxin toxic equivalence

The effects of feeding ranch mink ( Mustela vison ) diets containing polychlorinated biphenyl (PCB)-contaminated fish (88 gold fish [ Carassius auratus ] weighing a total of 70.3 kg and 16 carp [ Cyprinus carpio ] weighing a total of 77.3 kg) collected from the Housatonic River (HR; Berkshire County, MA, USA) in October 1999 on organ weights and histology and hepatic concentrations of total PCBs (&Sigma;PCBs) and 2,3,7,8-tetrachlorodibenzo- p -dioxin toxic equivalence (TEQ) were evaluated. Diets contained 0.22 to 3.54% HR fish, which provided 0.34 to 3.7 &mu;g &Sigma;PCBs/g feed (3.5-69 pg TEQ/g feed). Female mink were fed the diets eight weeks before breeding through weaning of kits at six weeks of age. Offspring were maintained on their respective diets for an additional 180 d. The dietary concentration of PCBs that caused a decrease in kit survival (3.7 &mu;g &Sigma;PCBs/g feed [69 pg TEQ/g]) resulted in a maternal hepatic concentration of 3.1 &mu;g &Sigma;PCBs/g wet weight (218 pg TEQ/g). Organ weights were not consistently affected. Mandibular and maxillary squamous cell proliferation was apparent in 31-week-old juveniles exposed to as low as 0.96 (xg &Sigma;PCBs/g feed (9.2 pg TEQ/g). Juveniles in this treatment group had a liver concentration of 1.7 &mu;g &Sigma;PCBs/g wet weight (40 pg TEQ/g). Because inclusion of PCB-contaminated fish, which comprised approximately 1% of the diet, resulted in mandibular and maxillary squamous cell proliferation, it is possible that consumption of up to 30-fold that quantity of HR fish, as could be expected for wild mink, would result in more severe lesions characterized by loss of teeth, thus impacting survivability.

Environmental Toxicology and Chemistry

Biomarkers of exposure and effects of environmental contaminants on swallows nesting along the Rio Grande, Texas, USA

We collected adult cave swallows (Petrochelidon fulva) and cliff swallows (P. pyrrhonota) during the breeding seasons in 1999 and 2000 from eight locations along the Rio Grande from Brownsville to El Paso (unless otherwise specified, all locations are Texas, USA) and an out-of-basin reference location. Body mass, spleen mass, hepatosomatic index (HSI), gonadosomatic index (GSI), thyroxine (T4) in plasma, DNA damage measured as the half-peak coefficient of variation of DNA content (HPCV) in blood cells, as well as acetylcholinesterase and butyrylcholinesterase in brain were compared with concentrations of organochlorines, metals, and metalloids in carcasses to determine potential effects of contaminants on swallows during the breeding season. Concentrations of 1,1-dichloro-2,2-bis(p-chlorophenyl)ethylene (p,p???-DDE) were significantly greater in swallows from El Paso than in those from most locations, except for Pharr and Llano Grande. All swallows from these three locations had p,p???-DDE concentrations of 3 ??g/g wet weight or greater. Swallows from El Paso either had or shared the highest concentrations of p,p???-DDE, polychlorinated biphenyls, and 13 inorganic elements. Swallows from El Paso exhibited greater spleen mass and HPCV values as well as lower T4 values compared with those from other locations. Thyroxine was a potential biomarker of contaminant exposure in swallows of the Rio Grande, because it was negatively correlated with p,p???-DDE and Se. Spleen mass was positively correlated with selenium and HSI and negatively correlated with body mass, GSI, Mn, and Ni. Overall, the present study suggests that insectivorous birds living in areas of high agricultural and industrial activity along the Rio Grande bioaccumulate environmental contaminants. These contaminants, particularly p,p???-DDE, may be among multiple factors that impact endocrine and hematopoietic function in Rio Grande swallows. ?? 2006 SETAC.

Environmental Toxicology and Chemistry

Comparison of selenium bioaccumulation in the clams Corbicula fluminea and Potamocorbula amurensis: A bioenergetic modeling approach

Selenium uptake from food (assimilation efficiency) and dissolved phase (influx rate) as well as loss kinetics (efflux rate) were compared between two bivalves, Corbicula fluminea and Potamocorbula amurensis. The effects of salinity and temperature on these kinetic parameters for both clam species also were evaluated. The Asiatic clam, C. fluminea, more efficiently assimilated Se associated with algae (66-87%) than Se associated with oxic sediments (20-37%). However, no consistent difference was found between Se assimilation efficiencies from both food types (19-60%) for P. amurensis. The temperature and salinity had a minor influence on the Se assimilation from ingested food. However, the effects of temperature and salinity were more evident in the uptake from dissolved sources. The influx rate of Se(IV) increased by threefold with the increase of temperature from 5 to 21??C for C. fluminea. The increase of salinity from 4 to 20 psu decreased the uptake rate constant (ku) of Se in P. amurensis from 0.011 to 0.005 L/g/h, whereas salinity change (0-8 psu) had a negligible effect on the Se influx rate of C. fluminea. The Se influx rate of P. amurensis decreased by half with the 3.5-fold increase in tissue dry weight. The rate constant of loss was greater for P. amurensis (0.029/d at 8 psu) than for C. fluminea (0.014/d at 0 psu and 0.01/d at 8 psu). A bioenergetic model suggests that dietary uptake is the dominant pathway for Se bioaccumulation in the two clams in San Francisco Bay and that interspecies differences in Se bioaccumulation can be explained by differences in food ingestion rates. ?? 2006 SETAC.

Environmental Toxicology and Chemistry

DNA damage and external lesions in brown bullheads (Ameiurus nebulosus) from contaminated habitats

The Comet assay was used to compare levels of DNA damage in brown bullheads ( Ameiurus nebulosus ) collected from three known contaminated locations, the Cuyahoga River (OH, USA), Ashtabula River (OH, USA; both tributaries to Lake Erie, USA), and Ashumet Pond (Cape Cod, MA, USA), with brown bullheads collected from three paired reference sites, Old Woman Creek (OH, USA), Conneaut River (OH, USA; both tributaries to Lake Erie), and Great Herring Pond (mainland MA, USA), respectively. Blood was sampled from each fish, and the Comet assay was conducted on erythrocytes. The assay results demonstrate that fish from the three contaminated sites each suffered higher DNA damage compared with fish from their respective reference sites. The results also show that the genetic damage was associated with the occurrence of external lesions and deformities in fish. The Comet assay is sufficiently sensitive to detect exposure of natural fish populations to environmental levels of genotoxic contaminants.

Environmental Toxicology and Chemistry

Effects of acid-volatile sulfide on metal bioavailability and toxicity to midge (Chironomus tentans) larvae in black shale sediments

Metal bioavailability and toxicity to aquatic organisms are greatly affected by variables such as pH, hardness, organic matter, and sediment acid-volatile sulfide (AVS). Sediment AVS, which reduces metal bioavailability and toxicity by binding and immobilizing metals as insoluble sulfides, has been studied intensely in recent years. Few studies, however, have determined the spatial variability of AVS and its interaction with simultaneously extracted metals (SEM) in sediments containing elevated concentrations of metals resulting from natural geochemical processes, such as weathering of black shales. We collected four sediment samples from each of four headwater bedrock streams in northcentral Arkansa (USA; three black shale-draining streams and one limestone-draining stream). We conducted 10-d acute whole-sediment toxicity tests using the midge Chironomus tentans and performed analyses for AVS, total metals, SEMs, and organic carbon. Most of the sediments from shale-draining streams had similar total metal and SEM concentrations but considerable differences in organic carbon and AVS. Zinc was the leading contributor to the SEM molar sum, averaging between 68 and 74%, whereas lead and cadmium contributed less than 3%. The AVS concentration was very low in all but two samples from one of the shale streams, and the sum of the SEM concentrations was in molar excess of AVS for all shale stream sediments. No significant differences in mean AVS concentrations between sediments collected from shale-draining or limestone-draining sites were noted (p > 0.05). Midge survival and growth in black shale-derived sediments were significantly less (p < 0.001) than that of limestone-derived sediments. On the whole, either SEM alone or SEM-AVS explained the total variation in midge survival and growth about equally well. However, survival and growth were significantly greater (p < 0.05) in the two sediment samples that contained measurable AVS compared with the two sediments from the same stream that contained negligible AVS. ?? 2007 SETAC.

Environmental Toxicology and Chemistry

Impacts of aircraft deicer and anti-icer runoff on receiving waters from Dallas/Fort Worth International Airport, Texas, USA

From October 2002 to April 2004, data were collected from Dallas/Fort Worth (DFW) International Airport (TX, USA) outfalls and receiving waters (Trigg Lake and Big Bear Creek) to document the magnitude and potential effects of aircraft deicer and anti-icer fluid (ADAF) runoff on water quality. Glycol concentrations at outfalls ranged from less than 18 to 23,800 mg/L, whereas concentrations in Big Bear Creek were less because of dilution, dispersion, and degradation, ranging from less than 18 to 230 mg/L. Annual loading results indicate that 10 and 35% of what was applied to aircraft was discharged to Big Bear Creek in 2003 and 2004, respectively. Glycol that entered Trigg Lake was diluted and degraded before reaching the lake outlet. Dissolved oxygen (DO) concentrations at airport outfalls sometimes were low (<2.0 mg/L) but typical of what was measured in an urban reference stream. In comparison, the DO concentration at Trigg Lake monitoring sites was consistently greater than 5.5 mg/L during the monitoring period, probably because of the installation of aerators in the lake by DFW personnel. The DO concentration in Big Bear Creek was very similar at sites upstream and downstream of airport influence (>5.0 mg/L). Results of toxicity tests indicate that effects on Ceriodaphnia dubia, Pimephales promelas, and Selanastrum capricornutum are influenced by type IV ADAF (anti-icer), not just type I ADAF (deicer) as is more commonly assumed. ?? 2006 SETAC.

Environmental Toxicology and Chemistry

Use of the oligochaete, Lumbriculus variegatus, as a prey organism for toxicant exposure of fish through the diet

The oligochaete, Lumbriculus variegatus, has several characteristics that make it desirable as a prey organism for conducting dietary exposure studies with fish. We conducted 21- and 30-d experiments with young fathead minnows (Pimephales promelas) and rainbow trout (Oncorhynchus mykiss), respectively, to determine whether a diet consisting solely of L. variegatus would support normal growth and to compare performance with standard diets (Artemia nauplii, frozen brine shrimp, or trout chow). All diets were readily accepted, and fish survived and grew well. Food conversion in both fathead minnows and rainbow trout was as high as or higher for the oligochaete diet compared with others, although this comparison is influenced by differences in ration, ingestion rate, or both. The oligochaete diet had gross nutritional analysis similar to the other diets, and meets fish nutrition guidelines for protein and essential amino acids. Methodologies and practical considerations for successfully using oligochaetes as an experimental diet are discussed. Considering their ready acceptance by fish, their apparent nutritional sufficiency, the ease of culturing large numbers, and the ease with which they can be loaded with exogenous chemicals, we believe that L. variegatus represents an excellent choice of exposure vector for exposing fish to toxicants via the diet. ?? 2006 SETAC.

Environmental Toxicology and Chemistry

Evasion of added isotopic mercury from a northern temperate lake

Isotopically enriched Hg (90% 202Hg) was added to a small lake in Ontario, Canada, at a rate equivalent to approximately threefold the annual direct atmospheric deposition rate that is typical of the northeastern United States. The Hg spike was thoroughly mixed into the epilimnion in nine separate events at two-week intervals throughout the summer growing season for three consecutive years. We measured concentrations of spike and ambient dissolved gaseous Hg (DGM) concentrations in surface water and the rate of volatilization of Hg from the lake on four separate, week-long sampling periods using floating dynamic flux chambers. The relationship between empirically measured rates of spike-Hg evasion were evaluated as functions of DGM concentration, wind velocity, and solar illumination. No individual environmental variable proved to be a strong predictor of the evasion flux. The DGM-normalized flux (expressed as the mass transfer coefficient, k) varied with wind velocity in a manner consistent with existing models of evasion of volatile solutes from natural waters but was higher than model estimates at low wind velocity. The empirical data were used to construct a description of evasion flux as a function of total dissolved Hg, wind, and solar illumination. That model was then applied to data for three summers for the experiment to generate estimates of Hg re-emission from the lake surface to the atmosphere. Based on ratios of spike Hg to ambient Hg in DGM and dissolved total Hg pools, ratios of DGM to total Hg in spike and ambient Hg pools, and flux estimates of spike and ambient Hg, we concluded that the added Hg spike was chemically indistinguishable from the ambient Hg in its behavior. Approximately 45% of Hg added to the lake over the summer was lost via volatilization.

Ontario