scholarly journals Size distribution of atmospheric particulate mercury in marine and coastal atmospheres

2012 ◽  
Vol 12 (6) ◽  
pp. 14591-14621 ◽  
Author(s):  
D. M. Feddersen ◽  
R. Talbot ◽  
H. Mao ◽  
B. C. Sive

Abstract. A study was conducted to determine the size distribution of particulate mercury (HgP) at a marine and coastal site, and compare the seasonality at both sites. Data was collected during summer 2009 and 2010, winter 2010, and spring 2010. Two cascade impactors were used to collect HgP in ten size fractions ranging from >10 μm to <0.4 μm. During summer 2009, HgP was found mainly (50–60%) in coarse fractions, 1.1 to 5.8 μm, composed of sea salt particles at both our coastal site (Thompson Farm) and marine site (Appledore Island). In winter, HgP at Thompson Farm was dominated (65%) by fine particles, while in spring and summer 2010, at both sites, HgP was distributed across the coarse and fine fractions (40% each). Using bulk filters to collect total HgP during each campaign, we show a diurnal cycle that matches that of gaseous elemental mercury. Finally, dry deposition rates of HgP were calculated to be 1.7–2.8 ng m−2 day−1 in the summer, 4.6 ng m−2 day−1 in the winter, and 2.5 ng m−2 day−1 in the spring.

2012 ◽  
Vol 12 (22) ◽  
pp. 10899-10909 ◽  
Author(s):  
D. M. Feddersen ◽  
R. Talbot ◽  
H. Mao ◽  
B. C. Sive

Abstract. A study was conducted to determine the size distribution of particulate mercury (HgP) at a marine and coastal site, and to compare the seasonal variability at both sites. Data was collected during summer 2009 and 2010, winter 2010, and spring 2010. Two cascade impactors were used to collect HgP in ten size fractions ranging from > 10 μm to < 0.4 μm. During summer 2009, HgP was found mainly (50–60%) in coarse fractions, 1.1 to 5.8 μm, composed of sea salt particles at both our coastal site (Thompson Farm) and marine site (Appledore Island). In winter, HgP at Thompson Farm was dominated (65%) by fine particles, while in spring and summer 2010, at both sites, HgP was distributed across the coarse and fine fractions (40% each). Using bulk filters to collect total HgP, we show a diurnal cycle that matches that of gaseous elemental mercury. Finally, dry deposition rates of HgP were calculated to be 1.7–2.8 ng m−2 day−1 in the summer, 4.6 ng m−2 day−1 in the winter, and 2.5 ng m−2 day−1 in the spring.


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.


2016 ◽  
Author(s):  
Z. Ye ◽  
H. Mao ◽  
C.-J. Lin ◽  
S. Y. Kim

Abstract. A box model incorporating a state-of-the-art chemical mechanism for atmospheric mercury (Hg) cycling was developed to investigate oxidation of gaseous elemental mercury (GEM) at three locations in the northeastern United States: Appledore Island (marine), Thompson Farm (coastal, rural), and Pack Monadnock (inland, rural, elevated). The chemical mechanism improved model's ability to simulate the formation of gaseous oxidized mercury (GOM) at the study sites. At the coastal and inland sites, GEM oxidation was predominated by O3 and OH, contributing 80–99 % of total GOM production during daytime. H2O2 initiated GEM oxidation was significant (~ 33 % of the total GOM) at the inland site during nighttime. In the marine boundary layer (MBL), Br and BrO were dominant GEM oxidants contributing ~ 70 % of the total GOM production during mid-day, while O3 dominated GEM oxidation (50–90 % of GOM production) over the remaining day. Following the production of HgBr from GEM + Br, HgBr was oxidized by BrO, HO2, OH, ClO, and IO to form Hg(II) brominated GOM species. However, under atmospheric conditions, the prevalent GEM oxidants in the MBL could be Br / BrO or O3 / OH depending on Br and BrO mixing ratios. Relative humidity and products of the CH3O2 + BrO reaction possibly affected significantly the mixing ratios of Br or BrO radicals and subsequently GOM formation. Gas-particle partitioning could be potentially important in the production of GOM as well as Br and BrO at the marine site.


2011 ◽  
Vol 45 (4) ◽  
pp. 848-855 ◽  
Author(s):  
Andrew P. Rutter ◽  
James J. Schauer ◽  
Martin M. Shafer ◽  
Joel E. Creswell ◽  
Michael R. Olson ◽  
...  

2016 ◽  
Vol 16 (13) ◽  
pp. 8461-8478 ◽  
Author(s):  
Zhuyun Ye ◽  
Huiting Mao ◽  
Che-Jen Lin ◽  
Su Youn Kim

Abstract. A box model incorporating a state-of-the-art chemical mechanism for atmospheric mercury (Hg) cycling was developed to investigate the oxidation of gaseous elemental mercury (GEM) at three locations in the northeastern United States: Appledore Island (AI; marine), Thompson Farm (TF; coastal, rural), and Pack Monadnock (PM; inland, rural, elevated). The chemical mechanism in this box model included the most up-to-date Hg and halogen chemistry. As a result, the box model was able to simulate reasonably the observed diurnal cycles of gaseous oxidized mercury (GOM) and chemical speciation bearing distinct differences between the three sites. In agreement with observations, simulated GOM diurnal cycles at AI and TF showed significant daytime peaks in the afternoon and nighttime minimums compared to flat GOM diurnal cycles at PM. Moreover, significant differences in the magnitude of GOM diurnal amplitude (AI > TF > PM) were captured in modeled results. At the coastal and inland sites, GEM oxidation was predominated by O3 and OH, contributing 80–99 % of total GOM production during daytime. H2O2-initiated GEM oxidation was significant (∼ 33 % of the total GOM) at the inland site during nighttime. In the marine boundary layer (MBL) atmosphere, Br and BrO became dominant GEM oxidants, with mixing ratios reaching 0.1 and 1 pptv, respectively, and contributing ∼ 70 % of the total GOM production during midday, while O3 dominated GEM oxidation (50–90 % of GOM production) over the remaining day when Br and BrO mixing ratios were diminished. The majority of HgBr produced from GEM+Br was oxidized by NO2 and HO2 to form brominated GOM species. Relative humidity and products of the CH3O2+BrO reaction possibly significantly affected the mixing ratios of Br or BrO radicals and subsequently GOM formation. Gas–particle partitioning could potentially be important in the production of GOM as well as Br and BrO at the marine site.


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.


2012 ◽  
Vol 12 (9) ◽  
pp. 4327-4340 ◽  
Author(s):  
L. Zhang ◽  
P. Blanchard ◽  
D. A. Gay ◽  
E. M. Prestbo ◽  
M. R. Risch ◽  
...  

Abstract. Dry deposition of speciated mercury, i.e., gaseous oxidized mercury (GOM), particulate-bound mercury (PBM), and gaseous elemental mercury (GEM), was estimated for the year 2008–2009 at 19 monitoring locations in eastern and central North America. Dry deposition estimates were obtained by combining monitored two- to four-hourly speciated ambient concentrations with modeled hourly dry deposition velocities (Vd) calculated using forecasted meteorology. Annual dry deposition of GOM+PBM was estimated to be in the range of 0.4 to 8.1 μg m−2 at these locations with GOM deposition being mostly five to ten times higher than PBM deposition, due to their different modeled Vd values. Net annual GEM dry deposition was estimated to be in the range of 5 to 26 μg m−2 at 18 sites and 33 μg m−2 at one site. The estimated dry deposition agrees very well with limited surrogate-surface dry deposition measurements of GOM and PBM, and also agrees with litterfall mercury measurements conducted at multiple locations in eastern and central North America. This study suggests that GEM contributes much more than GOM+PBM to the total dry deposition at the majority of the sites considered here; the only exception is at locations close to significant point sources where GEM and GOM+PBM contribute equally to the total dry deposition. The relative magnitude of the speciated dry deposition and their good comparisons with litterfall deposition suggest that mercury in litterfall originates primarily from GEM, which is consistent with the limited number of previous field studies. The study also supports previous analyses suggesting that total dry deposition of mercury is equal to, if not more important than, wet deposition of mercury on a regional scale in eastern North America.


2013 ◽  
Vol 13 (12) ◽  
pp. 6031-6048 ◽  
Author(s):  
I. Cheng ◽  
L. Zhang ◽  
P. Blanchard ◽  
J. Dalziel ◽  
R. Tordon

Abstract. Regional and local sources contributing to gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particle-bound mercury (PBM) at an urban coastal site in Dartmouth, Nova Scotia, Canada were investigated using the Concentration-Weighted Trajectory model (CWT) and Conditional Probability Function. From 2010–2011, GEM, GOM, and PBM concentrations were 1.67 ± 1.01 ng m−3, 2.07 ± 3.35 pg m−3, and 2.32 ± 3.09 pg m−3, respectively. Seasonal variability was observed, with statistically higher GEM and PBM concentrations in winter and spring and higher GOM in spring. In the CWT, concentrations are the weighting factors for the trajectory residence time in modeled grid cells, which results in the identification of source areas based on the CWT values in the grid cells. Potential source areas were identified in regions with known industrial Hg sources particularly in the fall season, but also in regions without these sources (e.g. Atlantic Ocean, northern Ontario and Quebec). CWTs for GOM and PBM that were associated with ≥ 5 kg industrial Hg emissions from 2010–2011 were statistically larger than those with zero Hg emissions, despite a lack of strong correlations. A large proportion of elevated CWTs (85–97%) was in regions with zero industrial Hg sources indicating the potential role of non-point sources, natural emissions, and residential-scale combustion. Analysis of wind data suggests that a commercial harbor and vehicular traffic were potential local sources. Evaluating modeled source areas against Hg emissions inventories was not an ideal method for assessing the CWT model accuracy because of insufficient data on Hg emissions at more precise locations.


2019 ◽  
Author(s):  
Lei Zhang ◽  
Peisheng Zhou ◽  
Shuzhen Cao ◽  
Yu Zhao

Abstract. One of the most important processes in the global mercury biogeochemical cycling is the deposition of atmospheric mercury, including gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particulate-bound mercury (PBM), to terrestrial surfaces. In this paper, methods for the observation of wet, dry, litterfall, throughfall, and cloud/fog deposition and models for mercury dry deposition are reviewed. Surrogate surface methods with cation exchange membranes are widely used for GOM dry deposition measurements, while observation methods for GEM dry deposition are more diverse. The methodology for Hg wet deposition is more mature, but the influence of cloud/fog scavenging is easy to neglect. Dry deposition models for speciated mercury have high uncertainties owing to the presence of sensitive parameters related to GOM chemical forms. Observation networks for mercury wet deposition have been developed worldwide, with the Global Mercury Observation System (GMOS) covering the northern hemisphere, the tropics, and the southern hemisphere. Wet deposition implies the spatial distribution of atmospheric mercury pollution, while GOM dry deposition depends highly on the elevation. Litterfall Hg deposition is crucial to forests. Urban areas have high wet deposition and PBM dry deposition because of high reactive mercury levels. Grasslands and forests have significant GOM and GEM dry deposition, respectively. Evergreen broadleaf forests bear high litterfall Hg deposition. Future research needs have been proposed based on the current knowledge of global mercury deposition to terrestrial surfaces.


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