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1.
Sci Total Environ ; 707: 135575, 2020 Mar 10.
Artigo em Inglês | MEDLINE | ID: mdl-31784172

RESUMO

The atmosphere is a key component of the biogeochemical cycle of mercury, acting as a reservoir, transport mechanism, and facilitator of chemical reactions. The chemical and physical behavior of atmospheric mercury determines how, when, and where emitted mercury pollution impacts ecosystems. In this review, we provide current information about what is known and what remains uncertain regarding mercury in the atmosphere. We discuss new ambient, laboratory, and theoretical information about the chemistry of mercury in various atmospheric media. We review what is known about mercury in and on solid- and liquid-phase aerosols. We present recent findings related to wet and dry deposition and spatial and temporal trends in atmospheric mercury concentrations. We also review atmospheric measurement methods that are in wide use and those that are currently under development.

2.
Sci Rep ; 9(1): 17611, 2019 11 26.
Artigo em Inglês | MEDLINE | ID: mdl-31772229

RESUMO

Coastal marine atmospheric fog has recently been implicated as a potential source of ocean-derived monomethylmercury (MMHg) to coastal terrestrial ecosystems through the process of sea-to-land advection of foggy air masses followed by wet deposition. This study examined whether pumas (Puma concolor) in coastal central California, USA, and their associated food web, have elevated concentrations of MMHg, which could be indicative of their habitat being in a region that is regularly inundated with marine fog. We found that adult puma fur and fur-normalized whiskers in our marine fog-influenced study region had a mean (±SE) total Hg (THg) (a convenient surrogate for MMHg) concentration of 1544 ± 151 ng g-1 (N = 94), which was three times higher (P < 0.01) than mean THg in comparable samples from inland areas of California (492 ± 119 ng g-1, N = 18). Pumas in California eat primarily black-tailed and/or mule deer (Odocoileus hemionus), and THg in deer fur from the two regions was also significantly different (coastal 28.1 ± 2.9, N = 55, vs. inland 15.5 ± 1.5 ng g-1, N = 40). We suggest that atmospheric deposition of MMHg through fog may be contributing to this pattern, as we also observed significantly higher MMHg concentrations in lace lichen (Ramalina menziesii), a deer food and a bioindicator of atmospheric deposition, at sites with the highest fog frequencies. At these ocean-facing sites, deer samples had significantly higher THg concentrations compared to those from more inland bay-facing sites. Our results suggest that fog-borne MMHg, while likely a small fraction of Hg in all atmospheric deposition, may contribute, disproportionately, to the bioaccumulation of Hg to levels that approach toxicological thresholds in at least one apex predator. As global mercury levels increase, coastal food webs may be at risk to the toxicological effects of increased methylmercury burdens.

3.
Environ Sci Technol ; 52(5): 2527-2537, 2018 03 06.
Artigo em Inglês | MEDLINE | ID: mdl-29401398

RESUMO

Water samples from marine stratus clouds were collected during 16 aircraft flights above the Pacific Ocean near the Central California coast during the summer of 2016. These samples were analyzed for total mercury (THg), monomethyl mercury (MMHg), and 32 other chemical species in addition to aerosol physical parameters. The mean concentrations of THg and MMHg in the cloudwater samples were 9.2 ± 6.0 ng L-1 (2.3-33.8 ng L-1) ( N = 97) and 0.87 ± 0.66 ng L-1 (0.17-2.9 ng L-1) ( N = 22), respectively. This corresponds to 9.5% (3-21%) MMHg as a fraction of THg. Low and high nonsea salt calcium ion (nss-Ca2+) concentrations in cloudwater were used to classify flights as "marine" and "continental", respectively. Mean [MMHg]marine was significantly higher ( p < 0.05) than [MMHg]continental consistent with an ocean source of dimethyl Hg (DMHg) to the atmosphere. Mean THg in cloudwater was not significantly different between the two categories, indicating multiple emissions sources. Mean [THg]continental was correlated with pH, CO, NO3-, NH4+, and other trace metals, whereas [THg]marine was correlated with MMHg and Na+. THg concentrations were negatively correlated with altitude, consistent with ocean and land emissions, coupled with removal at the cloud-top due to drizzle formation.


Assuntos
Mercúrio , Compostos de Metilmercúrio , Poluentes Químicos da Água , Aeronaves , California , Monitoramento Ambiental , Oceano Pacífico
4.
Environ Sci Technol ; 50(23): 12864-12873, 2016 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-27934281

RESUMO

Dry deposition of atmospheric mercury (Hg) to various land covers surrounding 24 sites in North America was estimated for the years 2009 to 2014. Depending on location, multiyear mean annual Hg dry deposition was estimated to range from 5.1 to 23.8 µg m-2 yr-1 to forested canopies, 2.6 to 20.8 µg m-2 yr-1 to nonforest vegetated canopies, 2.4 to 11.2 µg m-2 yr-1 to urban and built up land covers, and 1.0 to 3.2 µg m-2 yr-1 to water surfaces. In the rural or remote environment in North America, annual Hg dry deposition to vegetated surfaces is dominated by leaf uptake of gaseous elemental mercury (GEM), contrary to what was commonly assumed in earlier studies which frequently omitted GEM dry deposition as an important process. Dry deposition exceeded wet deposition by a large margin in all of the seasons except in the summer at the majority of the sites. GEM dry deposition over vegetated surfaces will not decrease at the same pace, and sometimes may even increase with decreasing anthropogenic emissions, suggesting that Hg emission reductions should be a long-term policy sustained by global cooperation.


Assuntos
Poluentes Atmosféricos , Mercúrio , Monitoramento Ambiental , Florestas , Estações do Ano
5.
Sci Total Environ ; 568: 546-556, 2016 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-26803218

RESUMO

This study examined the spatial and temporal trends of mercury (Hg) in wet deposition and air concentrations in the United States (U.S.) and Canada between 1997 and 2013. Data were obtained from the National Atmospheric Deposition Program (NADP) and Environment Canada monitoring networks, and other sources. Of the 19 sites with data records from 1997-2013, 53% had significant negative trends in Hg concentration in wet deposition, while no sites had significant positive trends, which is in general agreement with earlier studies that considered NADP data up until about 2010. However, for the time period 2007-2013 (71 sites), 17% and 13% of the sites had significant positive and negative trends, respectively, and for the time period 2008-2013 (81 sites) 30% and 6% of the sites had significant positive and negative trends, respectively. Non-significant positive tendencies were also widespread. Regional trend analyses revealed significant positive trends in Hg concentration in the Rocky Mountains, Plains, and Upper Midwest regions for the recent time periods in addition to significant positive trends in Hg deposition for the continent as a whole. Sulfate concentration trends in wet deposition were negative in all regions, suggesting a lower importance of local Hg sources. The trend in gaseous elemental Hg from short-term datasets merged as one continuous record was broadly consistent with trends in Hg concentration in wet deposition, with the early time period (1998-2007) producing a significantly negative trend (-1.5±0.2%year(-1)) and the recent time period (2008-2013) displaying a flat slope (-0.3±0.1%year(-1), not significant). The observed shift to more positive or less negative trends in Hg wet deposition primarily seen in the Central-Western regions is consistent with the effects of rising Hg emissions from regions outside the U.S. and Canada and the influence of long-range transport in the free troposphere.


Assuntos
Poluentes Atmosféricos/análise , Mercúrio/análise , Poluição do Ar/estatística & dados numéricos , Canadá , Monitoramento Ambiental , Estados Unidos
6.
Sci Total Environ ; 530-531: 519-525, 2015 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-25934382

RESUMO

Ozone as an atmospheric pollutant is largely produced by anthropogenic precursors and can significantly impact human and ecosystem health, and climate. The U.S. Environmental Protection Agency has recently proposed lowering the ozone standard from 75 ppbv (MDA8 = Maximum Daily 8-Hour Average) to between 65 and 70 ppbv. This will result in remote areas of the Intermountain West that includes many U.S. National Parks being out of compliance, despite a lack of significant local sources. We used Pb isotope fingerprinting and back-trajectory analysis to distinguish sources of imported ozone to Great Basin National Park in eastern Nevada. During discrete Chinese Pb events (> 1.1 ng/m(3) & > 80% Asian Pb) trans-Pacific transported ozone was 5 ± 5.5 ppbv above 19 year averages for those dates. In contrast, concentrations during regional transport from the Los Angeles and Las Vegas areas were 15 ± 2 ppbv above the long-term averages, and those characterized by high-altitude transport 3 days prior to sampling were 19 ± 4ppbv above. However, over the study period the contribution of trans-Pacific transported ozone increased at a rate of 0.8 ± 0.3 ppbv/year, suggesting that Asian inputs will exceed regional and high altitude sources by 2015-2020. All of these sources will impact regulatory compliance with a new ozone standard, given increasing global background.


Assuntos
Poluentes Atmosféricos/análise , Monitoramento Ambiental , Chumbo/análise , Ozônio/análise , Poluição do Ar/estatística & dados numéricos , Atmosfera/química , Política Ambiental , Los Angeles , Nevada , Estados Unidos , United States Environmental Protection Agency
7.
Bull Environ Contam Toxicol ; 94(4): 425-30, 2015 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-25549909

RESUMO

The aim of this project was to obtain a baseline understanding and investigate the concentration of mercury (Hg) in the tissue of terrestrial arthropods. The 4-month sampling campaign took place around Monterey Bay, California. Total mercury (HgT) concentrations (x ± SD, dry weight) for the captured specimens ranged from 22 to 188 ng g(-1) in the Jerusalem crickets (Orthoptera: Stenopelmatidae); 65-233 ng g(-1) in the camel crickets (Orthoptera: Rhaphidophoridae); 25-227 ng g(-1) in the pill bugs (Isopoda: Armadillidiidae); 19-563 ng g(-1) in the ground beetles (Coleoptera: Carabidae); 140-441 ng g(-1) in the variegated meadowhawk dragonflies (Odonata: Libellulidae); 607-657 ng g(-1) in the pacific spiketail dragonflies (Odonata: Cordulegastridae); and 81-1,249 ng g(-1) in the wolf spiders (Araneae: Lycosidae). A subset of samples analyzed for monomethyl mercury (MMHg) suggest detrital pill bugs have a higher MMHg/HgT ratio than predatory ground beetles.


Assuntos
Artrópodes/metabolismo , Monitoramento Ambiental , Mercúrio/análise , Metais Pesados/análise , Poluentes do Solo/análise , Animais , California
9.
Sci Total Environ ; 470-471: 1099-113, 2014 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-24252197

RESUMO

The Western Airborne Contaminants Assessment Project showed that USA National Parks had fish mercury (Hg) concentrations above threshold concentrations set for wildlife. Since significant areas of the Western USA are arid, we hypothesized that dry deposition would be important. The primary question was whether sources of Hg were local and thus, easily addressed, or regional (from within the United States), or global (long range transport), and more difficult to address. To investigate this, surrogate surfaces and passive samplers for the measurement of GOM deposition and concentration, respectively, were deployed from the coast of California to the eastern edge of Nevada. Meteorological data, back trajectory modeling, and ozone concentrations were applied to better understand potential sources of Hg. Lowest seasonal mean Hg deposition (0.2 to 0.4 ng m(-2)h(-1)) was observed at low elevation (<100 m) Pacific Coast sites. Highest values were recorded at Lick Observatory, a high elevation coastal site (1,279 m), and Great Basin National Park (2,062 m) in rural eastern Nevada (1.5 to 2.4 ng m(-2)h(-1)). Intermediate values were recorded in Yosemite and Sequoia National Parks (0.9 to 1.2 ng m(-2)h(-1)). Results indicate that local, regional and global sources of air pollution, specifically oxidants, are contributing to observed deposition. At Great Basin National Park air chemistry was influenced by regional urban and agricultural emissions and free troposphere inputs. Dry deposition contributed ~2 times less Hg than wet deposition at the coastal locations, but 3 to 4 times more at the higher elevation sites. Based on the spatial trends, oxidation in the marine boundary layer or ocean sources contributed ~0.4 ng m(-2)h(-1) at the coastal locations. Regional pollution and long range transport contributed 1 to 2 ng m(-2)h(-1) to other locations, and the source of Hg is global and as such, all sources are important to consider.


Assuntos
Poluentes Atmosféricos/análise , Monitoramento Ambiental , Mercúrio/análise , Poluição do Ar/estatística & dados numéricos , Atmosfera/química , California , Modelos Químicos , Nevada , Ozônio/análise , Estados Unidos
10.
Environ Sci Technol ; 47(13): 7307-16, 2013 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-23651121

RESUMO

The chemical compounds that make up gaseous oxidized mercury (GOM) in the atmosphere, and the reactions responsible for their formation, are not well understood. The limitations and uncertainties associated with the current method applied to measure these compounds, the KCl-coated denuder, are not known due to lack of calibration and testing. This study systematically compared the uptake of specific GOM compounds by KCl-coated denuders with that collected using nylon and cation exchange membranes in the laboratory and field. In addition, a new method for identifying different GOM compounds using thermal desorption is presented. Different GOM compounds (HgCl2, HgBr2, and HgO) were found to have different affinities for the denuder surface and the denuder underestimated each of these compounds. Membranes measured 1.3 to 3.7 times higher GOM than denuders in laboratory and field experiments. Cation exchange membranes had the highest collection efficiency. Thermodesorption profiles for the release of GOM compounds from the nylon membrane were different for HgO versus HgBr2 and HgCl2. Application of the new field method for collection and identification of GOM compounds demonstrated these vary as a function of location and time of year. Understanding the chemistry of GOM across space and time has important implications for those developing policy regarding this environmental contaminant.


Assuntos
Poluentes Atmosféricos/análise , Brometos/análise , Monitoramento Ambiental/instrumentação , Cloreto de Mercúrio/análise , Compostos de Mercúrio/análise , Óxidos/análise , Adsorção , Resinas de Troca de Cátion/química , Monitoramento Ambiental/métodos , Membranas Artificiais , Nylons/química , Oxirredução , Cloreto de Potássio/química
11.
Environ Sci Technol ; 37(17): 3755-63, 2003 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-12967093

RESUMO

In this study, gas-phase elemental mercury (Hg0) and related species (including inorganic reactive gaseous mercury (RGM) and particulate mercury (PHg)) were measured at Cheeka Peak Observatory (CPO), Washington State, in the marine boundary layer during 2001-2002. Air of continental origin containing anthropogenic pollutants from the urban areas to the east contained on average 5.3% lower Hg0 levels as compared to the marine background. This result is difficult to reconcile since it is known that industrial emissions in our region are sources of Hg0. The rate of removal of Hg0 from a pollution plume necessary to account for our observations is inconsistent with the accepted view of Hg0 as a stable atmospheric pollutant. The largest and most frequent Hg0 loss events occurred in the presence of increased ozone (O3) during the summer. Hg0 and O3 also display diurnal cycles that are out-of-phase with one another. In other seasons Hg0 behavior is less consistent, as we observe weak positive correlations with O3 and occasional Hg0 enhancements in local pollution. RGM and PHg concentrations are enhanced only slightly during Hg0 loss events, comprising a small fraction of the mercury pool (approximately 3%). Long-range transported pollution of Asian origin was also detected at CPO, and this contains both higher and lower levels of Hg0 as compared to the background with maximum changes being <20%. Here, the more photochemically processed the air mass, as determined by propane/ethane ratios, the more likely we are to observe Hg0 loss. Air from the marine background in summer displays a significant diurnal cycle with a phase that matches the diurnal cycles seen in polluted air masses. A Junge lifetime for Hg0 in the clean marine boundary layer is calculated to be 7.1 months, which is on the low end of previous estimates (0.5-2 yr).


Assuntos
Poluentes Atmosféricos/análise , Mercúrio/análise , Poluentes Atmosféricos/química , Monitoramento Ambiental , Gases , Mercúrio/química , Oxidantes Fotoquímicos/análise , Ozônio/análise , Tamanho da Partícula , Periodicidade , Estações do Ano
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