Modeling Atmospheric Mercury Deposition in the Vicinity of Power Plants

Abstract

Two mathematical models of the atmospheric fate and transport of mercury (Hg), an Eulerian grid–based model and a Gaussian plume model, are used to calculate the atmospheric deposition of Hg in the vicinity (i.e., within 50 km) of five coal–fired power plants. The former is applied using two different horizontal resolutions: coarse (84 km) and fine (16.7 km). More than 96% of the power plant Hg emissions are calculated with the plume model to be transported beyond 50 km from the plants. The grid–based model predicts a lower fraction to be transported beyond 50 km: >91% with a coarse resolution and >95% with a fine resolution. The contribution of the power plant emissions to total Hg deposition within a radius of 50 km from the plants is calculated to be <8% with the plume model, <14% with the Eulerian model with a coarse resolution, and <10% with the Eulerian model with a fine resolution. The Eulerian grid–based model predicts greater local impacts than the plume model because of artificially enhanced vertical dispersion; the former predicts about twice as much Hg deposition as the latter when the area considered is commensurate with the resolution of the grid–based model. If one compares the local impacts for an area that is significantly less than the grid–based model resolution, then the grid–based model may predict lower local deposition than the plume model, because two compensating errors affect the results obtained with the grid–based model: initial dilution of the power plant emissions within one or more grid cells and enhanced vertical mixing to the ground.     

Trends of perfluorochemicals in Greenland ringed seals and polar bears: Indications of shifts to decreasing trends

Time-series of perfluorinated alkylated substances (PFASs) in East Greenland polar bears and East and West Greenland ringed seals were updated in order to deduce whether a response to the major reduction in perfluoroalkyl production in the early 2000s had occurred. Previous studies had documented an exponential increase of perfluorooctane sulphonate (PFOS) in liver tissue from both species. In the present study, PFOS was still the far most dominant compound constituting 92% (West Greenland ringed seals), 88% (East Greenland ringed seals) and 85% (East Greenland polar bears). The PFOS concentrations increased up to 2006 with doubling times of approximately 6 years for the ringed seal populations and 14 years in case of polar bears. Since then a rapid decrease has occurred with clearing half-lives of approximately 1, 2 and 4 years, respectively. In polar bears perfluorohexane sulphonate (PFHxS) and perfluorooctane sulphonamide (PFOSA) also showed decreasing trends in recent years as do perfluorodecanoic acid (PFDA) and perfluoroundecanoic acid (PFUnA). For the West Greenland ringed seal population perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), PFDA and PFUnA peaked in the mid 2000s, whereas PFNA, PFDA and PFUnA in the East Greenland population have been stable or increasing in recent years. The peak of PFASs in Greenland ringed seals and polar bears occurred at a later time than in Canadian seals and polar bears and considerably later than observed in seal species from more southern latitudes. We suggest that this could be explained by the distance to emission hot-spots and differences in long-range transport to the Arctic.     

Integrated methodology for assessing the HCH groundwater pollution at the multi-source contaminated mega-site Bitterfeld/Wolfen

A large-scale groundwater contamination characterises the Pleistocene groundwater system of the former industrial and abandoned mining region Bitterfeld/Wolfen, Eastern Germany. For more than a century, local chemical production and extensive lignite mining caused a complex contaminant release from local production areas and related dump sites. Today, organic pollutants (mainly organochlorines) are present in all compartments of the environment at high concentration levels. An integrated methodology for characterising the current situation of pollution as well as the future fate development of hazardous substances is highly required to decide on further management and remediation strategies. Data analyses have been performed on regional groundwater monitoring data from about 10 years, containing approximately 3,500 samples, and up to 180 individual organic parameters from almost 250 observation wells. Run-off measurements as well as water samples were taken biweekly from local creeks during a period of 18 months. A kriging interpolation procedure was applied on groundwater analytics to generate continuous distribution patterns of the nodal contaminant samples. High-resolution geological 3-D modelling serves as a database for a regional 3-D groundwater flow model. Simulation results support the future fate assessment of contaminants. A first conceptual model of the contamination has been developed to characterise the contamination in regional surface waters and groundwater. A reliable explanation of the variant hexachlorocyclohexane (HCH) occurrence within the two local aquifer systems has been derived from the regionalised distribution patterns. Simulation results from groundwater flow modelling provide a better understanding of the future pollutant migration paths and support the overall site characterisation. The presented case study indicates that an integrated assessment of large-scale groundwater contaminations often needs more data than only from local groundwater monitoring. The developed methodology is appropriate to assess POP-contaminated mega-sites including, e.g. HCH deposits. Although HCH isomers are relevant groundwater pollutants at this site, further organochlorine pollutants are present at considerably higher levels. The study demonstrates that an effective evaluation of the current situation of contamination as well as of the related future fate development requires detailed information of the entire observed system.     

Toxicity of hydroquinone to different freshwater phototrophs is influenced by time of exposure and pH

The interaction of natural organic matter with phytoplankton communities in freshwater ecosystems is an intensively studied subject matter. Previous studies showed that apparently plant-derived phenols were able to inhibit algal and cyanobacterial growth. Furthermore, it was also assumed that humic substances (HS), which comprise the major part of dissolved organic carbon in freshwater ecosystems, directly interact with freshwater phototrophs. For example, quinoid building blocks of HS were thought to be algicidal. To identify key environmental variable for the toxic action of potential quinone algicides, we tested the toxicity of hydroquinone (HQ) to different eukaryotic and prokaryotic freshwater phototrophs in terms of growth performance and investigated also the effect of HQ oxidation at different pH values on its algicidal potential. It was shown that cyanobacterial species were much more susceptible to hydroquinone than coccal green algal species were, with Microcystis aeruginosa being the most sensitive species by far. In addition, it was obvious that the aging of hydroquinone-stock solution at pH 11 led to polymerization and, by this process, to a total loss of toxicity; whereas the algicidal potential sustained if the polyphenol was kept at pH 7. Since most lakes with heavy blooms of phototrophs possess pH values clearly above 7.0, it is questionable, if polyphenols in general and quinones in particular are the effective chemicals and if litter and straw leachates are applied as means to combat algal and cyanobacterial blooms.     

Uptake of 14C-atropine and/or its transformation products from soil by wheat (Triticum aestivum var Kronjet) and their translocation to shoots

Plant uptake of toxins and their translocation to edible plant parts are important processes in the transfer of contaminants into the food chain. Atropine, a highly toxic muscarine receptor antagonist produced by Solanacea species, is found in all plant tissues and can enter the soil and hence be available for uptake by crops. The absorption of atropine and/or its transformation products from soil by wheat (Triticum aestivum var Kronjet) and its distribution to shoots was investigated by growing wheat in soil spiked with unlabeled or ¹⁴C-labeled atropine. Radioactivity attributable to ¹⁴C-atropine and its transformation products was measurable in plants sampled at 15 d after sowing (DAS) and thereafter until the end of experiment. The highest accumulation of ¹⁴C-atropine and/or its transformation products by plants was detected in leaves (between 73 and 90% of the total accumulated) with lower amounts in stems, roots, and seeds (approximately 14%, 9%, and 3%, respectively). ¹⁴C-Atropine and/or its transformation products were detected in soil leachate at 30, 60, and 90 DAS and were strongly adsorbed to soil, with 60% of the applied dose adsorbed at 30 DAS, plateauing at 70% from 60 DAS. Unlabeled atropine was detected in shoots 30 DAS at a concentration of 3.9 ± 0.1 μg kg^?1 (mean ± SD). The observed bioconcentration factor was 2.3 ± 0.04. The results suggest a potential risk of atropine toxicity to consumers.     

A correlation between the fate and non-extractable residue formation of 14C-metalaxyl and enzymatic activities in soil

Extracellular, oxidative soil enzymes like monophenol oxidases and peroxidases play an important role in transformation of xenobiotics and the formation of organic matter in soil. Additionally, these enzymes may be involved in the formation of non-extractable residues (NERs) of xenobiotics during humification processes. To examine this correlation, the fate of the fungicide ¹⁴C metalaxyl in soil samples from Ultuna (Sweden) was studied. Using different soil sterilization techniques, it was possible to differentiate between free, immobilized, and abiotic (“pseudoenzyme”-like) oxidative activities. A correlation between the formation of metalaxyl NER and soil organic matter content, biotic activities, as well as extracellular phenoloxidase and peroxidase activities in the bulk soil and its particle size fractions was determined. Extracellular soil-bound enzymes were involved in NER formation (up to 8% of applied radioactivity after 92 days) of the fungicide independently from the presence of living microbes and different distributions of the NER in the soil humic subfractions.     

Ozone Formation in California's San Joaquin Valley: A Critical Assessment of Modeling and Data Needs

ABSTRACT

Data from the 1990 San Joaquin Valley Air Quality Study/ Atmospheric Utility Signatures, Predictions, and Experiments (SJVAQS/AUSPEX) field program in California's San Joaquin Valley (SJV) suggest that both urban and rural areas would have difficulty meeting an 8-hr average O₃ standard of 80 ppb. A conceptual model of O₃ formation and accumulation in the SJV is formulated based on the chemical, meteorological, and tracer data from SJVAQS/ AUSPEX. Two major phenomena appear to lead to high O₃ concentrations in the SJV: (1) transport of O₃ and precursors from upwind areas (primarily the San Francisco Bay Area, but also the Sacramento Valley) into the SJV, affecting the northern part of the valley, and (2) emissions of precursors, mixing, transport (including long-range transport), and atmospheric reactions within the SJV responsible for regional and urban-scale (e.g., downwind of Fresno and Bakersfield) distributions of O₃. Using this conceptual model, we then conduct a critical evaluation of the meteorological model and air quality model. Areas of model improvements and data needed to understand and properly simulate O₃ formation in the SJV are highlighted.     

Forest law compliance and enforcement: the case of on-farm timber extraction in Ghana

The paper investigates law compliance in case of on-farm timber extraction in Ghana. It empirically investigates compliance with rules that (i) require timber operators to obtain prior and informed consent from the farmers, (ii) require timber operators to pay appropriate and timely compensation for crop damage caused by timber extraction and (iii) ban chainsaw lumbering. The study documents a low level of compliance in all three domains. Subsequently, the paper discusses the underlying causes for the observed low compliance. The low compliance level is attributed to a legislation, and enforcement, that provides huge financial incentives for non-compliance for both farmers and timber operators, and in the latter case both with and without legal permits. At the same time the regulation is perceived to violate their moral values. The paper underlines the interests of the political elite as decisive in shaping the current regulation and the way it is implemented on the ground. It asserts that eliciting compliance requires consideration of both the instrumental and normative perspectives; else it becomes illusive. The study thus challenges the typical response of governments in developing countries, who, supported by donor agencies, attempt to elicit compliance through enhanced law enforcement efforts. The results presented on the Ghana case suggest that such an approach is unlikely to elicit compliance.     

Organochlorines and polybrominated diphenyl ethers in four geographically separated populations of Atlantic salmon (Salmo salar)

Atlantic salmon (Salmon salar) populations from four locations, two from isolated Swedish lake systems, one of the Baltic Sea and one of the North Atlantic, were analyzed to determine the concentrations and spatial variations of polybrominated diphenyl ethers (PBDEs) and organochlorines (DDT, PCB and HCH). Levels in both liver and muscle were in the same range as previously reported in Atlantic salmon, except for elevated concentrations found per lipid weight (lw) in the muscle samples of salmon from the North Atlantic ( summation PBDE 263 ng g(-1) lw, summation PCB 3262 ng g(-1) lw, summation DDT 4063 ng g(-1) lw summation HCH 131 ng g(-1)). In general, elevated concentrations in the muscles compared to the liver were observed, especially in lipid depleted migrating salmon, possibly caused by a faster lipid depletion compared with the redistribution of PBDEs, PCBs and DDTs. These findings indicated that the life stage and thereby the lipid dynamics of the fish must be considered prior to comparison based on lipid weight, especially as Atlantic salmon experience large variations in lipid content during periods of migration. The dominating PBDE congener was BDE-47, representing more than 25% in all fish. The PBDE pattern changed between locations, with a significant separation of the fish from the freshwater and marine environment when analyzed using principal component analysis.     

Source to sink tracking of selected human pharmaceuticals from two Oslo city hospitals and a wastewater treatment works

The occurrence of twenty pharmaceutical compounds was quantitatively determined in effluents from two major Oslo city hospitals, Rikshospitalet and Ullev?l, along with influent, sludge and final effluent from the city's VEAS wastewater treatment works (WTW). Composite hospital effluents were collected over a twelve week period and were showed to contain paracetamol, metoprolol, diclofenac, ibuprofen, 17beta-Estradiol, estriol, estrone, oxytetracycline, tetracycline, doxycycline, chlorotetracycline, demeclocycline, trimethoprim, ciprofloxacin, sulfamethoxazole, cyclophosphamide and ifosfamide. Three pharmaceuticals were not detected above the limit of detection; cefuroxime, 17alpha-ethinylestradiol and meclocycline. Composite influent, sludge and effluent samples were collected from VEAS WTW over a seven week period. The influent into VEAS WTW contained all of the same selected substances detected in the hospital effluents, except for oxytetracycline, chlorotetracycline, demeclocycline, cyclophosphamide and ifosfamide. The percentage of pharmaceuticals entering the works from the hospitals was <10% for all of the selected compounds. VEAS sludge samples contained a different profile of substances reflecting their physico-chemical properties. Hydrophobic antibiotics, such as oxytetracycline, tetracycline and ciprofloxacin, were detected in all of the collected sludge samples. Their absence in the collected influent samples suggests that they enter the works bound to effluent particles, with the dissolved fraction observed in the hospital effluents partitioning onto particulate matter within the sewerage network. The final effluent from VEAS WTW contained reduced concentrations of many pharmaceuticals, including paracetamol, ibuprofen and sulfamethoxazole. For other compounds, such as metoprolol, diclofenac and trimethoprim, there were often higher concentrations in the effluent than the influent. These effluent concentrations represent median inputs varying from low g day(-1) (e.g. paracetamol and ibuprofen) to nearly 200 g day(-1) (e.g. metoprolol and trimethoprim) into Oslofjord. A simple risk assessment showed that the antibiotic ciprofloxacin may at times pose an acute risk to the Oslofjord aquatic environment.