Atmospheric Mercury Deposition during the Last 270 Years:  A Glacial Ice Core Record of Natural and Anthropogenic Sources

2002 ◽  
Vol 36 (11) ◽  
pp. 2303-2310 ◽  
Author(s):  
Paul F. Schuster ◽  
David P. Krabbenhoft ◽  
David L. Naftz ◽  
L. Dewayne Cecil ◽  
Mark L. Olson ◽  
...  
2014 ◽  
Vol 14 (5) ◽  
pp. 2233-2244 ◽  
Author(s):  
J. Zhu ◽  
T. Wang ◽  
R. Talbot ◽  
H. Mao ◽  
X. Yang ◽  
...  

Abstract. A comprehensive measurement study of mercury wet deposition and size-fractionated particulate mercury (HgP) concurrent with meteorological variables was conducted from June 2011 to February 2012 to evaluate the characteristics of mercury deposition and particulate mercury in urban Nanjing, China. The volume-weighted mean (VWM) concentration of mercury in rainwater was 52.9 ng L−1 with a range of 46.3–63.6 ng L−1. The wet deposition per unit area was averaged 56.5 μg m−2 over 9 months, which was lower than that in most Chinese cities, but much higher than annual deposition in urban North America and Japan. The wet deposition flux exhibited obvious seasonal variation strongly linked with the amount of precipitation. Wet deposition in summer contributed more than 80% to the total amount. A part of contribution to wet deposition of mercury from anthropogenic sources was evidenced by the association between wet deposition and sulfates, as well as nitrates in rainwater. The ions correlated most significantly with mercury were formate, calcium, and potassium, which suggested that natural sources including vegetation and resuspended soil should be considered as an important factor to affect the wet deposition of mercury in Nanjing. The average HgP concentration was 1.10 ± 0.57 ng m−3. A distinct seasonal distribution of HgP concentrations was found to be higher in winter as a result of an increase in the PM10 concentration. Overall, more than half of the HgP existed in the particle size range less than 2.1 μm. The highest concentration of HgP in coarse particles was observed in summer, while HgP in fine particles dominated in fall and winter. The size distribution of averaged mercury content in particulates was bimodal, with two peaks in the bins of < 0.7 μm and 4.7–5.8 μm. Dry deposition per unit area of HgP was estimated to be 47.2 μg m−2 using meteorological conditions and a size-resolved particle dry deposition model. This was 16.5% less than mercury wet deposition. Compared to HgP in fine particles, HgP in coarse particles contributed more to the total dry deposition due to higher deposition velocities. Negative correlation between precipitation and the HgP concentration reflected the effect of scavenging of HgP by precipitation.


2013 ◽  
Vol 13 (4) ◽  
pp. 9849-9893 ◽  
Author(s):  
H. Lei ◽  
X.-Z. Liang ◽  
D. J. Wuebbles ◽  
Z. Tao

Abstract. Atmospheric mercury is a toxic air and water pollutant that is of significant concern because of its effects on human health and ecosystems. A mechanistic representation of the atmospheric mercury cycle is developed for the state-of-the-art global climate-chemistry model, CAM-Chem (Community Atmospheric Model with Chemistry). The model simulates the emission, transport, transformation and deposition of atmospheric mercury (Hg) in three forms: elemental mercury (Hg(0)), reactive mercury (Hg(II)), and particulate mercury (PHg). Emissions of mercury include those from human, land, ocean, biomass burning and volcano related sources. Land emissions are calculated based on surface solar radiation flux and skin temperature. A simplified air–sea mercury exchange scheme is used to calculate emissions from the oceans. The chemistry mechanism includes the oxidation of Hg(0) in gaseous phase by ozone with temperature dependence, OH, H2O2 and chlorine. Aqueous chemistry includes both oxidation and reduction of Hg(0). Transport and deposition of mercury species are calculated through adapting the original formulations in CAM-Chem. The CAM-Chem model with mercury is driven by present meteorology to simulate the present mercury air quality during the 1999–2001 periods. The resulting surface concentrations of total gaseous mercury (TGM) are then compared with the observations from worldwide sites. Simulated wet depositions of mercury over the continental United States are compared to the observations from 26 Mercury Deposition Network stations to test the wet deposition simulations. The evaluations of gaseous concentrations and wet deposition confirm a strong capability for the CAM-Chem mercury mechanism to simulate the atmospheric mercury cycle. The results also indicate that mercury pollution in East Asia and Southern Africa is very significant with TGM concentrations above 3.0 ng m−3. The comparison to wet deposition indicates that wet deposition patterns of mercury are more affected by the spatial variability of precipitation. The sensitivity experiments show that 22% of total mercury deposition and 25% of TGM concentrations in the United States are resulted from domestic anthropogenic sources, but only 9% of total mercury deposition and 7% of TGM concentrations are contributed by transpacific transport. However, the contributions of domestic and transpacific sources on the western United States levels of mercury are of comparable magnitude.


2018 ◽  
Vol 18 (16) ◽  
pp. 12345-12361 ◽  
Author(s):  
Christian M. Zdanowicz ◽  
Bernadette C. Proemse ◽  
Ross Edwards ◽  
Wang Feiteng ◽  
Chad M. Hogan ◽  
...  

Abstract. Black carbon aerosol (BC), which is emitted from natural and anthropogenic sources (e.g., wildfires, coal burning), can contribute to magnify climate warming at high latitudes by darkening snow- and ice-covered surfaces, and subsequently lowering their albedo. Therefore, modeling the atmospheric transport and deposition of BC to the Arctic is important, and historical archives of BC accumulation in polar ice can help to validate such modeling efforts. Here we present a > 250-year ice-core record of refractory BC (rBC) deposition on Devon ice cap, Canada, spanning the years from 1735 to 1992. This is the first such record ever developed from the Canadian Arctic. The estimated mean deposition flux of rBC on Devon ice cap for 1963–1990 is 0.2 mg m−2 a−1, which is at the low end of estimates from Greenland ice cores obtained using the same analytical method ( ∼ 0.1–4 mg m−2 a−1). The Devon ice cap rBC record also differs from the Greenland records in that it shows only a modest increase in rBC deposition during the 20th century. In the Greenland records a pronounced rise in rBC is observed from the 1880s to the 1910s, which is largely attributed to midlatitude coal burning emissions. The deposition of contaminants such as sulfate and lead increased on Devon ice cap in the 20th century but no concomitant rise in rBC is recorded in the ice. Part of the difference with Greenland could be due to local factors such as melt–freeze cycles on Devon ice cap that may limit the detection sensitivity of rBC analyses in melt-impacted core samples, and wind scouring of winter snow at the coring site. Air back-trajectory analyses also suggest that Devon ice cap receives BC from more distant North American and Eurasian sources than Greenland, and aerosol mixing and removal during long-range transport over the Arctic Ocean likely masks some of the specific BC source–receptor relationships. Findings from this study suggest that there could be a large variability in BC aerosol deposition across the Arctic region arising from different transport patterns. This variability needs to be accounted for when estimating the large-scale albedo lowering effect of BC deposition on Arctic snow/ice.


2006 ◽  
Vol 6 (4) ◽  
pp. 5905-5931 ◽  
Author(s):  
T. M. Jenk ◽  
S. Szidat ◽  
M. Schwikowski ◽  
H. W. Gäggeler ◽  
S. Brütsch ◽  
...  

Abstract. Long-term concentration records of carbonaceous particles (CP) are of increasing interest in climate research due to their not yet completely understood effects on climate. Nevertheless, only poor data on their concentrations and sources in the past is available. We present a first long-term record of organic carbon (OC) and elemental carbon (EC) concentrations - the two main fractions of CP – along with the corresponding fraction of modern carbon (fM) derived from radiocarbon (14C) analysis. The combination of concentration measurements with 14C analysis of CP allows a distinction and quantification of natural, biogenic and anthropogenic fossil sources in the past. CP were extracted from an ice archive, with resulting carbon quantities in the microgram range. Analysis of 14C by accelerator mass spectrometry (AMS) was therefore highly demanding. We analysed 33 samples of 0.4 to 1 kg ice from a 150.5 m long ice core retrieved at Fiescherhorn glacier in December 2002 (46°33'3.2" N, 08°04'0.4'' E; 3900 m a.s.l.). Samples were taken from below the firn/ice transition down to bedrock, covering the time period 1650–1940 and thus the transition from the pre-industrial to the industrial era. Before 1800, OC was of pure biogenic origin with a mean concentration of 21±2 μg kg−1}. In 1940, OC concentration was more than a factor of 3 higher than this biogenic background, almost half of it originating from anthropogenic sources, i.e. from combustion of fossil fuels. The biogenic EC concentration was nearly constant over the examined time period with 6±1 μg kg−1. In 1940, the additional anthropogenic input of atmospheric EC was about 50 μg kg−1.


Geosciences ◽  
2018 ◽  
Vol 8 (10) ◽  
pp. 374 ◽  
Author(s):  
Marta Pérez-Rodríguez ◽  
Olga Margalef ◽  
Juan Corella ◽  
Alfonso Saiz-Lopez ◽  
Sergi Pla-Rabes ◽  
...  

The study of mercury accumulation in peat cores provides an excellent opportunity to improve the knowledge on mercury cycling and depositional processes at remote locations far from pollution sources. We analyzed mercury concentrations in 150 peat samples from two cores from Rano Aroi (Easter Island, 27° S) and in selected vegetation samples of present-day flora of the island, in order to characterize the mercury cycling for the last ~71 ka BP. The mercury concentrations showed values ranging between 35 and 200 ng g−1, except for a large maxima (~1000 ng g−1) which occurred at the end of the Last Glacial Maximum (LGM, ~20 ka cal BP) in both peat cores. Low temperatures during the LGM would accelerate the atmospheric oxidation of Hg(0) to divalent mercury that, coupled with higher rainfall during this period, most likely resulted in a very efficient surface deposition of atmospheric mercury. Two exceptional short-lived Hg peaks occurred during the Holocene at 8.5 (350 ng g−1) and 4.7 (1000 ng g−1) ka cal BP. These values are higher than those recorded in most peat records belonging to the industrial period, highlighting that natural factors played a significant role in Hg accumulation—sometimes even more so than anthropogenic sources. Our results suggest that wet deposition, linked to atmospheric oxidation, was the main process controlling the short-lived Hg events, both in the mire and in the catchment soils.


2017 ◽  
Author(s):  
Christian M. Zdanowicz ◽  
Bernadette C. Proemse ◽  
Ross Edwards ◽  
Wang Feiteng ◽  
Chad M. Hogan ◽  
...  

Abstract. Black carbon aerosol (BC) emitted from natural and anthropogenic sources (e.g., wildfires, coal burning) can contribute to magnify climate warming at high latitudes by darkening snow- and ice-covered surfaces, thus lowering their albedo. Modeling the atmospheric transport and deposition of BC to the Arctic is therefore important, and historical archives of BC accumulation in polar ice can help to validate such modeling efforts. Here we present a 190-year ice-core record of refractory BC (rBC) deposition on Devon ice cap, Canada, spanning calendar years 1810–1990, the first such record ever developed from the Canadian Arctic. The estimated mean deposition flux of rBC on Devon ice cap for 1963–1990 is 0.2 mg m−2 a−1, which is low compared to most Greenland ice-core sites over the same period. The Devon ice cap rBC record also differs from existing Greenland records in that it shows no evidence of a substantial increase in rBC deposition during the early-mid 20th century, which, for Greenland, has been attributed to mid-latitude coal burning emissions. The deposition of other contaminants such as sulfate and Pb increased on Devon ice cap in the 20th century but without a concomitant rise in rBC. Part of the difference with Greenland may be due to local factors such as wind scouring of winter snow at the coring site on Devon ice cap. Air back-trajectory analyses also suggest that Devon ice cap receives BC from more distant North American and Eurasian sources than Greenland, and aerosol mixing and removal during long-range transport over the Arctic Ocean likely masks some of the specific BC source-receptor relationships. Findings from this study underscore the large variability in BC aerosol deposition across the Arctic region that may arise from different transport patterns. This variability needs to be accounted for when estimating the large-scale albedo lowering effect of BC deposition on Arctic snow/ice.


2013 ◽  
Vol 13 (11) ◽  
pp. 28309-28341 ◽  
Author(s):  
J. Zhu ◽  
T. Wang ◽  
R. Talbot ◽  
H. Mao ◽  
X. Yang ◽  
...  

Abstract. A comprehensive measurement study of mercury wet deposition and size-fractioned particulate mercury (HgP) concurrent with meteorological variables was conducted from June 2011 to February 2012 to evaluate the characteristics of mercury deposition and particulate mercury in urban Nanjing, China. The volume weighted mean (VWM) concentration of mercury in rainwater was 52.9 ng L−1 with a range of 46.3–63.6 ng L−1. The wet deposition per unit area was averaged 56.5 μg m−2 over 9 months, which was lower than that in most Chinese cities, but much higher than annual deposition in urban America and Japan. The wet deposition flux exhibited obvious seasonal variation strongly linked with the amount of precipitation. Wet deposition in summer contributed more than 80% to the total amount. A part of contribution to wet deposition of mercury from anthropogenic sources was evidenced by the association between wet deposition and sulfates, and nitrates in rainwater. The ions correlated most significantly with mercury were formate, calcium and potassium, which suggested that natural sources including vegetation and resuspended soil should be considered as an important factor to affect the wet deposition of mercury in Nanjing. The average HgP concentration was 1.10 ± 0.57 ng m−3. A distinct seasonal distribution of HgP concentrations was found to be higher in winter as a result of an increase in the PM10 concentration. Overall, more than half of HgP existed in the particle size range less than 2.1 μm. The highest concentration of HgP in coarse particles was observed in summer while HgP in fine particles dominated in fall and winter. The size distribution of averaged mercury content in particulates was bimodal with two peaks in the bins of <0.7 μm and 4.7–5.8 μm. Dry deposition per unit area of HgP was estimated to be 47.2 μg m−2 using meteorological conditions and a size-resolved particle dry deposition model. This was 16.5% less than mercury wet deposition. Compared to HgP in fine particles, HgP in coarse particles contributed more to the total dry deposition due to higher deposition velocities. Negative correlation between precipitation and the HgP concentration reflected the effect of scavenging of HgP by precipitation.


2013 ◽  
Vol 13 (21) ◽  
pp. 10807-10825 ◽  
Author(s):  
H. Lei ◽  
X.-Z. Liang ◽  
D. J. Wuebbles ◽  
Z. Tao

Abstract. Atmospheric mercury is a toxic air and water pollutant that is of significant concern because of its effects on human health and ecosystems. A mechanistic representation of the atmospheric mercury cycle is developed for the state-of-the-art global climate-chemistry model, CAM-Chem (Community Atmospheric Model with Chemistry). The model simulates the emission, transport, transformation and deposition of atmospheric mercury (Hg) in three forms: elemental mercury (Hg(0)), reactive mercury (Hg(II)), and particulate mercury (PHg). Emissions of mercury include those from human, land, ocean, biomass burning and volcano related sources. Land emissions are calculated based on surface solar radiation flux and skin temperature. A simplified air–sea mercury exchange scheme is used to calculate emissions from the oceans. The chemistry mechanism includes the oxidation of Hg(0) in gaseous phase by ozone with temperature dependence, OH, H2O2 and chlorine. Aqueous chemistry includes both oxidation and reduction of Hg(0). Transport and deposition of mercury species are calculated through adapting the original formulations in CAM-Chem. The CAM-Chem model with mercury is driven by present meteorology to simulate the present mercury air quality during the 1999–2001 period. The resulting surface concentrations of total gaseous mercury (TGM) are then compared with the observations from worldwide sites. Simulated wet depositions of mercury over the continental United States are compared to the observations from 26 Mercury Deposition Network stations to test the wet deposition simulations. The evaluations of gaseous concentrations and wet deposition confirm a strong capability for the CAM-Chem mercury mechanism to simulate the atmospheric mercury cycle. The general reproduction of global TGM concentrations and the overestimation on South Africa indicate that model simulations of TGM are seriously affected by emissions. The comparison to wet deposition indicates that wet deposition patterns of mercury are more affected by the spatial variability of precipitation. The sensitivity experiments show that 22% of total mercury deposition and 25% of TGM concentrations in the United States result from domestic anthropogenic sources, but only 9% of total mercury deposition and 7% of TGM concentrations are contributed by transpacific transport. However, the contributions of domestic and transpacific sources on the western United States levels of mercury are of comparable magnitude.


2008 ◽  
Vol 35 (5) ◽  
Author(s):  
E. Osterberg ◽  
P. Mayewski ◽  
K. Kreutz ◽  
D. Fisher ◽  
M. Handley ◽  
...  

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