•Total Hg released to the environment from coal combustion is estimated to be 38Gg.•71% of this Hg was released into the atmosphere, while 31% went to land and water.•Most of the Hg from coal ...combustion was released in Asia and Europe (32% each).•The fraction of Hg released to the air as elemental Hg has steadily increased.•In the year 2010 about 1Gg of Hg was released worldwide to all media.
Display omitted
Coal combustion is one of the largest contemporary sources of anthropogenic mercury (Hg). It releases geologically sequestered Hg to the atmosphere, and fly ash can contaminate terrestrial and aquatic systems. We estimate that coal combustion has released a cumulative total of 38.0 (14.8–98.9, 80% C.I.) Gg (gigagrams, 109g or thousand tonnes) of Hg to air, land, and water up to the year 2010, most of which (97%) has occurred since 1850. The rate of release has grown by two orders of magnitude from 0.01Ggyr−1 in 1850 to 1Ggyr−1 in 2010. Geographically, Asia and Europe each account for 32% of cumulative releases and an additional 18% is from North America. About 26.3 (10.2–68.3) Gg, 71% of the total, were directly emitted to the atmosphere, mostly from the industrial (45%) and power generation (36%) sectors, while the remainder was disposed of to land and water bodies. While Europe and North America were the major contributing regions until 1950, Asia has surpassed both in recent decades. By 2010, Asia was responsible for 69% of the total releases of Hg from coal combustion to the environment. Control technologies installed on major emitting sources capture mainly particulate and divalent Hg, and therefore the fraction of elemental Hg in emissions from coal combustion has increased over time from 0.46 in 1850 to 0.61 in 2010. About 11.8 (4.6–30.6) Gg of Hg, 31% of the total, have been transferred to land and water bodies through the disposal or utilization of Hg-containing combustion waste and collected fly ash/FGD waste; approximately 8.8Gg of this Hg have simply been discarded to waste piles or ash ponds or rivers.
Full text
Available for:
GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Midlatitude anthropogenic mercury (Hg) emissions and discharge reach the Arctic Ocean (AO) by atmospheric and oceanic transport. Recent studies suggest that Arctic river Hg inputs have been a ...potentially overlooked source of Hg to the AO. Observations on Hg in Eurasian rivers, which represent 80% of freshwater inputs to the AO, are quasi-inexistent, however, putting firm understanding of the Arctic Hg cycle on hold. Here, we present comprehensive seasonal observations on dissolved Hg (DHg) and particulate Hg (PHg) concentrations and fluxes for two large Eurasian rivers, the Yenisei and the Severnaya Dvina. We find large DHg and PHg fluxes during the spring flood, followed by a second pulse during the fall flood. We observe well-defined water vs. Hg runoff relationships for Eurasian and North American Hg fluxes to the AO and for Canadian Hg fluxes into the larger Hudson Bay area. Extrapolation to pan-Arctic rivers and watersheds gives a total Hg river flux to the AO of 44 ± 4 Mg per year (1σ), in agreement with the recent model-based estimates of 16 to 46 Mg per year and Hg/dissolved organic carbon (DOC) observation-based estimate of 50 Mg per year. The river Hg budget, together with recent observations on tundra Hg uptake and AO Hg dynamics, provide a consistent view of the Arctic Hg cycle in which continental ecosystems traffic anthropogenic Hg emissions to the AO via rivers, and the AO exports Hg to the atmosphere, to the Atlantic Ocean, and to AO marine sediments.
Full text
Available for:
BFBNIB, NMLJ, NUK, PNG, SAZU, UL, UM, UPUK
Between 2013 and 2015, concentrations of poly- and perfluoroalkyl substances (PFAS) in public drinking water supplies serving at least six million individuals exceeded the level set forth in the ...health advisory established by the U.S. Environmental Protection Agency. Other than data reported for contaminated sites, no systematic or prospective data exist on the relative source contribution (RSC) of drinking water to human PFAS exposures.
This study estimates the RSC of tap water to overall PFAS exposure among members of the general U.S.
We measured concentrations of 15 PFAS in home tap water samples collected in 1989-1990 from 225 participants in a nationwide prospective cohort of U.S. women: the Nurses' Health Study (NHS). We used a one-compartment toxicokinetic model to estimate plasma concentrations corresponding to tap water intake of PFAS. We compared modeled results with measured plasma PFAS concentrations among a subset of 110 NHS participants.
Tap water perfluorooctanoic acid (PFOA) and perfluorononanoic acid (PFNA) were statistically significant predictors of plasma concentrations among individuals who consumed Formula: see text cups of tap water per day. Modeled median contributions of tap water to measured plasma concentrations were: PFOA 12% (95% probability interval 11%-14%), PFNA 13% (8.7%-21%), linear perfluorooctanesulfonic acid (nPFOS) 2.2% (2.0%-2.5%), branched perfluorooctanesulfonic acid (brPFOS) 3.0% (2.5%-3.2%), and perfluorohexanesulfonic acid (PFHxS) 34% (29%-39%). In five locations, comparisons of PFASs in community tap water collected in the period 2013-2016 with samples from 1989-1990 indicated increases in quantifiable PFAS and extractable organic fluorine (a proxy for unquantified PFAS).
Our results for 1989-1990 compare well with the default RSC of 20% used in risk assessments for legacy PFAS by many agencies. Future evaluation of drinking water exposures should incorporate emerging PFAS. https://doi.org/10.1289/EHP4093.
Full text
Available for:
CEKLJ, DOBA, IZUM, KILJ, NUK, OILJ, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK, VSZLJ
Abstract
When released to the biosphere, mercury (Hg) is very mobile and can take millennia to be returned to a secure, long-term repository. Understanding where and when Hg was released as a result ...of human activities allows better quantification of present-day reemissions and future trajectories of environmental concentrations. In this work, we estimate the time-varying releases of Hg in seven world regions over the 500 year period, 1510–2010. By our estimation, this comprises 95% of all-time anthropogenic releases. Globally, 1.47 Tg of Hg were released in this period, 23% directly to the atmosphere and 77% to land and water bodies. Cumulative releases have been largest in Europe (427 Gg) and North America (413 Gg). In some world regions (Africa/Middle East and Oceania), almost all (>99%) of the Hg is relatively recent (emitted since 1850), whereas in South America it is mostly of older vintage (63% emitted before 1850). Asia was the greatest-emitting region in 2010, while releases in Europe and North America have declined since the 1970s, as recognition of the risks posed by Hg have led to its phase-out in commercial usage. The continued use of Hg in artisanal and small-scale gold mining means that the Africa/Middle East region is now a major contributor. We estimate that 72% of cumulative Hg emissions to air has been in the form of elemental mercury (Hg
0
), which has a long lifetime in the atmosphere and can therefore be transported long distances. Our results show that 83% of the total Hg has been released to local water bodies, onto land, or quickly deposited from the air in divalent (Hg
II
) form. Regionally, this value ranges from 77% in Africa/Middle East and Oceania to 89% in South America. Results from global biogeochemical modeling indicate improved agreement of the refined emission estimates in this study with archival records of Hg accumulation in estuarine and deep ocean sediment.
We develop an empirically constrained multicompartment box model for mercury cycling in open ocean regions to investigate changes in concentrations resulting from anthropogenic perturbations of the ...global mercury cycle. Using Monte Carlo simulations, we explicitly consider the effects of variability in measured parameters on modeled seawater concentrations. Our simulations show that anthropogenic enrichment in all surface (25%) and deep ocean waters (11%) is lower than global atmospheric enrichment (300–500%) and varies considerably among geographic regions, ranging from >60% in parts of the Atlantic and Mediterranean to <1% in the deep Pacific. Model results indicate that open ocean mercury concentrations do not rapidly equilibrate with atmospheric deposition and on average will increase if anthropogenic emissions remain at their present level. We estimate the temporal lag between changes in atmospheric deposition and ocean mercury concentrations will vary from decades in most of the Atlantic up to centuries in parts of the Pacific.
Full text
Available for:
FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Drinking water contaminated by per- and polyfluoroalkyl substances (PFAS) is a widespread public health concern, and exposure–response relationships are known to vary across sociodemographic groups. ...However, research on disparities in drinking water PFAS exposures and the siting of PFAS sources in marginalized communities is limited. Here, we use monitoring data from 7873 U.S. community water systems (CWS) in 18 states to show that PFAS detection is positively associated with the number of PFAS sources and proportions of people of color who are served by these water systems. Each additional industrial facility, military fire training area, and airport in a CWS watershed was associated with a 10–108% increase in perfluorooctanoic acid and a 20–34% increase in perfluorooctane sulfonic acid in drinking water. Waste sector sources were also significantly associated with drinking water PFAS concentrations. CWS watersheds with PFAS sources served higher proportions of Hispanic/Latino and non-Hispanic Black residents compared to those without PFAS sources. CWS serving higher proportions of Hispanic/Latino and non-Hispanic Black residents had significantly increased odds of detecting several PFAS. This likely reflects disparities in the siting of PFAS contamination sources. Results of this work suggest that addressing environmental justice concerns should be a component of risk mitigation planning for areas affected by drinking water PFAS contamination.
Full text
Available for:
IJS, KILJ, NUK, PNG, UL, UM
Anthropogenic mercury (Hg(0)) emissions oxidize to gaseous Hg(II) compounds, before deposition to Earth surface ecosystems. Atmospheric reduction of Hg(II) competes with deposition, thereby modifying ...the magnitude and pattern of Hg deposition. Global Hg models have postulated that Hg(II) reduction in the atmosphere occurs through aqueous-phase photoreduction that may take place in clouds. Here we report that experimental rainfall Hg(II) photoreduction rates are much slower than modelled rates. We compute absorption cross sections of Hg(II) compounds and show that fast gas-phase Hg(II) photolysis can dominate atmospheric mercury reduction and lead to a substantial increase in the modelled, global atmospheric Hg lifetime by a factor two. Models with Hg(II) photolysis show enhanced Hg(0) deposition to land, which may prolong recovery of aquatic ecosystems long after Hg emissions are lowered, due to the longer residence time of Hg in soils compared with the ocean. Fast Hg(II) photolysis substantially changes atmospheric Hg dynamics and requires further assessment at regional and local scales.
Drinking water contamination with poly- and perfluoroalkyl substances (PFASs) poses risks to the developmental, immune, metabolic, and endocrine health of consumers. We present a spatial analysis of ...2013–2015 national drinking water PFAS concentrations from the U.S. Environmental Protection Agency’s (US EPA) third Unregulated Contaminant Monitoring Rule (UCMR3) program. The number of industrial sites that manufacture or use these compounds, the number of military fire training areas, and the number of wastewater treatment plants are all significant predictors of PFAS detection frequencies and concentrations in public water supplies. Among samples with detectable PFAS levels, each additional military site within a watershed’s eight-digit hydrologic unit is associated with a 20% increase in PFHxS, a 10% increase in both PFHpA and PFOA, and a 35% increase in PFOS. The number of civilian airports with personnel trained in the use of aqueous film-forming foams is significantly associated with the detection of PFASs above the minimal reporting level. We find drinking water supplies for 6 million U.S. residents exceed US EPA’s lifetime health advisory (70 ng/L) for PFOS and PFOA. Lower analytical reporting limits and additional sampling of smaller utilities serving <10000 individuals and private wells would greatly assist in further identifying PFAS contamination sources.
Full text
Available for:
IJS, KILJ, NUK, PNG, UL, UM
The mechanism for spread of SARS-CoV-2 has been attributed to large particles produced by coughing and sneezing. There is controversy whether smaller airborne particles may transport SARS-CoV-2. ...Smaller particles, particularly fine particulate matter (≤ 2.5 µm in diameter), can remain airborne for longer periods than larger particles and after inhalation will penetrate deeply into the lungs. Little is known about the size distribution and location of airborne SARS-CoV-2 RNA.
As a measure of hospital-related exposure, air samples of three particle sizes (> 10.0 µm, 10.0-2.5 µm, and ≤ 2.5 µm) were collected in a Boston, Massachusetts (USA) hospital from April to May 2020 (N = 90 size-fractionated samples). Locations included outside negative-pressure COVID-19 wards, a hospital ward not directly involved in COVID-19 patient care, and the emergency department.
SARS-CoV-2 RNA was present in 9% of samples and in all size fractions at concentrations of 5 to 51 copies m
. Locations outside COVID-19 wards had the fewest positive samples. A non-COVID-19 ward had the highest number of positive samples, likely reflecting staff congregation. The probability of a positive sample was positively associated (r = 0.95, p < 0.01) with the number of COVID-19 patients in the hospital. The number of COVID-19 patients in the hospital was positively associated (r = 0.99, p < 0.01) with the number of new daily cases in Massachusetts.
More frequent detection of positive samples in non-COVID-19 than COVID-19 hospital areas indicates effectiveness of COVID-ward hospital controls in controlling air concentrations and suggests the potential for disease spread in areas without the strictest precautions. The positive associations regarding the probability of a positive sample, COVID-19 cases in the hospital, and cases in Massachusetts suggests that hospital air sample positivity was related to community burden. SARS-CoV-2 RNA with fine particulate matter supports the possibility of airborne transmission over distances greater than six feet. The findings support guidelines that limit exposure to airborne particles including fine particles capable of longer distance transport and greater lung penetration.
Full text
Available for:
DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
PDF
