scholarly journals A synthesis review on atmospheric wet deposition of particulate elements: scavenging ratios, solubility and flux measurements

2021 ◽  
Author(s):  
Irene Cheng ◽  
Abdulla Al Mamun ◽  
Leiming Zhang

Atmospheric dry and wet deposition of particulate matter controls its lifetime in air and contributes to the environmental burden of toxic pollutants, and thus has important implications on human and ecosystem health. This synthesis review focused on atmospheric wet deposition of particulate elements and analyzed their scavenging ratios (i.e. concentration in precipitation to that in ambient air), solubility and wet deposition flux measurements based on published studies in literature, aiming to gather updated knowledge that can be used for modeling their wet deposition. Our analysis finds that scavenging ratios of a specific element have a narrow range. Overall, elemental scavenging ratios for snow are ~3 times higher than those for rain. Elements that are bound to coarse (PM2.5-10) particles have larger scavenging ratios than those bound to fine (PM2.5) particles except for Fe and Si. Solubility of elements in rainwater range from 8% (Fe) to 94% (Ca). Solubility is moderately correlated with scavenging ratio possibly explaining the lower scavenging ratios of Fe and Si compared to other elements with similar fine fraction. Data collected from North America, Europe, the Middle East, and Asia show that the wet fluxes of Al and Fe are orders of magnitude greater than those of routinely-monitored anthropogenic elements (Zn, Pb, Cu, Ni, Cd, Cr). Wet deposition fluxes of particulate elements in the Middle East exceed those in other regions, likely due to regional transport of dust and soil resuspension. Fluxes from all regions are a factor of 2-3 greater in industrialized and urban locations than rural and remote locations because of industrial, vehicular and soil and mineral dust emissions. Dry deposition fluxes are usually greater than wet deposition fluxes although to varying degrees according to co-located measurements. Based on the relationships between scavenging ratio and elemental PM2.5 fraction under rain and snow conditions, we derived regression equations for estimating scavenging ratios of particulate elements whose measurements are limited. Such knowledge and data improves the quantification of atmospheric deposition fluxes for an expanded list of metals and metalloids and the understanding of pathways contributing to ecological risk.

2014 ◽  
Vol 14 (2) ◽  
pp. 629-640 ◽  
Author(s):  
Z. W. Wang ◽  
J. C. Gallet ◽  
C. A. Pedersen ◽  
X. S. Zhang ◽  
J. Ström ◽  
...  

Abstract. Light-absorbing aerosol – particularly elemental carbon (EC) – while mixed with snow and ice is an important climate driver from the enhanced absorption of solar radiation. Currently, considerable efforts are being made to estimate its radiative forcing on a global scale, but several uncertainties remain, particularly those regarding its deposition processes. In this study, concurrent measurements of EC in air and snow are performed for three years (2009–2012) at Changbai station, northeastern China. The scavenging ratio and the wet- and dry-deposition fluxes of EC over the snow surface are estimated. The mean EC concentration in the surface snow is 1000 ± 1500 ng g−1, ranging from 7 to 7640 ng g−1. The mean value of the scavenging ratio of EC by snow is 140 ± 100, with a median value of 150, which is smaller than that reported in Arctic areas. A non-rimed snow process is a significant factor in interpreting differences with Arctic areas. Wet-deposition fluxes of EC are estimated to be 0.47 ± 0.37 μg cm−2 month−1 on average over the three snow seasons studied. Dry deposition is more than five times higher, with an average of 2.65 ± 1.93 μg cm−2 month−1; however, only winter period estimation is possible (December–February). During winter in Changbai, 87% of EC in snow is estimated to be due to dry deposition, with a mean dry deposition velocity of 6.44 × 10−3 m s−1 and median of 8.14 × 10−3 m s−1. Finally, the calculation of the radiative effect shows that 500 ng g−1 of dry-deposited EC to a snow surface absorbs three times more incoming solar energy than the same mass mixed in the snow through wet deposition. Deposition processes of an EC-containing snow surface are, therefore, crucial to estimate its radiative forcing better, particularly in northeastern China, where local emission strongly influences the level and gradient of EC in the snowpack, and snow-covered areas are cold and dry due to the atmospheric general circulation. Furthermore, this study builds on the knowledge to characterize the conditions in the snow-laden Chinese rural areas better as well as to constrain transport of EC to the Arctic better.


2009 ◽  
Vol 9 (6) ◽  
pp. 23465-23504 ◽  
Author(s):  
X. W. Fu ◽  
X. Feng ◽  
Z. Q. Dong ◽  
R. S. Yin ◽  
J. X. Wang ◽  
...  

Abstract. China is regarded as the largest contributor of mercury (Hg) to the global atmospheric Hg budget. However, concentration levels and depositions of atmospheric Hg in China are poorly known. Continuous measurements of atmospheric total gaseous mercury (TGM) were carried out from May 2008 to May 2009 at the summit of Mt. Leigong in south China. Wet and dry deposition fluxes of Hg were also calculated following collection of precipitation, throughfall and litterfall. Atmospheric TGM concentrations averaged 2.80±1.51 ng m−3, which was highly elevated compared to global background values but much lower than semi-rural and industrial/urban areas in China, indicating great emissions of Hg in central, south and southwest China. Seasonal and diurnal variations of TGM were observed, which reflected variations in source intensity, deposition processes and meteorological factors. Wet deposition of Hg was quite low, while its dry deposition of Hg (litterfall + throughfall-direct wet deposition) constituted a major portion of total deposition (~88% for total mercury (THg) and 84% for methyl mercury (MeHg)). This highlights the importance of vegetation to Hg atmospheric cycling. In a remote forest ecosystem of China, dry deposition of TGM, especially gaseous elemental mercury (GEM), was very important for the depletion of atmospheric Hg. Elevated TGM level in ambient air may accelerate the foliar uptake of Hg through air which may partly explain the elevated Hg dry deposition fluxes observed in Mt. Leigong.


2019 ◽  

<p>This paper analysis the contents and variation of heavy metals in wet and dry deposition in Changji (Xinjiang, China) revealed their reducing regularity for heavy metals in atmosphere in arid area. Samples (including 84 dry deposition samples and 16 wet deposition samples) were collected from January 2016 to December 2016, and the contents of heavy metals (Ni, Cu, Cd and Pb) were analyzed by AA-7000 atomic absorption spectrophotometer. The dry deposition fluxes of Ni, Cu, Cd and Pb are 3.70 mg/( m2.a), 4.81 mg/( m2. a), 0.53 mg/( m2•a) and 22.74 mg/( m2•a), respectively; the wet deposition fluxes of Ni, Cu, Cd and Pb are 0.77mg/( m2•a), 3.25mg/( m2•a), 0.04mg/( m2•a) and 0.11mg/( m2•a), respectively. Each of the four heavy metals deposition fluxes during heating period was higher than non-heating period, especially for Pb and Cd, which is mainly due to the emission of coal combustion for heating. During sampling periods, the ratio of wet deposition flux to total for Ni, Cu, Cd and Pb are 17.21%, 40.33%, 7.67% and 0.48%, respectively; the wet deposition flux is far less than dry deposition, especially for Pb. The rate of dry deposition is lower than wet deposition, however dry deposition plays an important role in scavenging heavy metals in arid region. Arid region has a low intensity and frequency of rain event, heavy metals were mainly scavenging by dry deposition attribute to its continuous and dependable process. Dry deposition has much more environmental effect on heavy metal in arid region.</p>


2013 ◽  
Vol 13 (5) ◽  
pp. 14221-14248 ◽  
Author(s):  
Z. W. Wang ◽  
C. A. Pedersen ◽  
X. S. Zhang ◽  
J. C. Gallet ◽  
J. Ström ◽  
...  

Abstract. Light absorbing aerosol, in particular elemental carbon (EC), in snow and ice enhance absorption of solar radiation, reduce the albedo, and is an important climate driver. In this study, measurements of EC concentration in air and snow are performed concurrently at Changbai Station, Northeastern China, from 2009 to 2012. The mean EC concentration for surface snow is 987 &amp;pm; 1510 ng g−1 with a range of 7 to 7636 ng g−1. EC levels in surface snow around (about 50 km) Changbai Mountain are lower than those collected on the same day at Changbai station, and decrease with distance from Changbai station, indicating that EC load in snow around Changbai Mountain is influenced by local source emissions. Scavenging ratios of EC by snow are calculated through comparing the concentrations of EC in fresh snow with those in air. The upper-limit of mean scavenging ratio is 137.4 &amp;pm; 99.7 with median 149.4, which is smaller than those reported from Arctic areas. The non-rimed snow process may be one of significant factors for interpreting the difference of scavenging ratio in this area with the Arctic areas. Finally, wet and dry depositional fluxes of EC have been estimated, and the upper-limit of EC wet deposition flux is 0.46 &amp;pm; 0.38 μg cm−2 month−1 during the three consecutive snow season, and 1.32 &amp;pm; 0.95 μg cm−2 month−1 for dry deposition flux from December to February during study period. During these three years, 77% of EC in snow is attributed to the dry deposition, indicating that dry deposition processes play a major role for EC load in snow in the area of Changbai, Northeastern China. Based on the dry deposition fluxes of EC and hourly black carbon (BC) concentrations in air, the estimated mean dry deposition velocity is 2.81 × 10−3 m s−1 with the mean median of 3.15 × 10−3 m s−1. These preliminary estimates for the scavenging ratio and dry deposition velocity of EC on snow surface will be beneficial for numerical models, and improve simulations of EC transport, fate and radiative forcing in order to ultimately make better climate prediction.


2021 ◽  
Author(s):  
Sudesh Yadav ◽  
Umesh Kulshrestha

&lt;p&gt;The chemical composition of rainwater is an indicator of the air quality and sources of influence. In this study, pH and ionic concentrations were measured in rain samples collected during monsoon season of 2018 at a rural agricultural site located in northern part of India. Wet deposition fluxes of reactive nitrogen species NH&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; over NO&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;-&lt;/sup&gt; were calculated to estimate their annual deposition. The pH of samples varied between 5.2 and 6.14, with an average value of 5.72 which is in alkaline range considering 5.6 as the neutral pH of cloud water with atmospheric CO&lt;sub&gt;2&lt;/sub&gt; equilibrium. These relatively high pH values indicate the neutralisation of acidity in precipitation. Samples were analysed for their cationic and anionic content using ion chromatography. The results showed that NH&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; concentrations were higher than NO&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;- &lt;/sup&gt;with the VWM concentrations of 187.23 &amp;#956;eql&lt;sup&gt;-1&lt;/sup&gt; and 26.79 &amp;#956;eql&lt;sup&gt;-1&lt;/sup&gt; respectively. Furthermore, wet deposition flux of NH&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt;-N was calculated as 4.25 kg ha&lt;sup&gt;-1&lt;/sup&gt; yr&lt;sup&gt;-1&lt;/sup&gt; while that of NO&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;-&lt;/sup&gt;-N was as 2.10 kg ha&lt;sup&gt;-1&lt;/sup&gt; yr&lt;sup&gt;-1&lt;/sup&gt;. VWM concentrations of major ions decreased in the following order NH&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; &gt; Ca&lt;sup&gt;2+&lt;/sup&gt; &gt; SO&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;2-&lt;/sup&gt; &gt; NO&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;-&lt;/sup&gt; &gt; K&lt;sup&gt;+&lt;/sup&gt; &gt; Cl&lt;sup&gt;-&lt;/sup&gt; &gt; Na&lt;sup&gt;+&lt;/sup&gt; &gt; Mg&lt;sup&gt;2+&lt;/sup&gt;. In this study, relatively high NH&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; concentrations in rainwater can be attributed to nearby agricultural activities, excreta and biomass burning.&lt;/p&gt;&lt;p&gt;&lt;strong&gt;Keywords:&lt;/strong&gt; Rainwater, Neutralisation, VWM concentration, Agricultural site, Reactive Nitrogen.&lt;/p&gt;


2012 ◽  
Vol 12 (14) ◽  
pp. 6207-6218 ◽  
Author(s):  
Z. H. Dai ◽  
X. B. Feng ◽  
J. Sommar ◽  
P. Li ◽  
X. W. Fu

Abstract. The legacy of long-term mining activities in Wanshan mercury (Hg) mining area (WMMA), Guizhou, China including a series of environmental issues related to Hg pollution. The spatial distribution of gaseous elemental mercury (Hg0) concentrations in ambient air were monitored using a mobile RA-915+ Zeeman Mercury Analyzer during daytime and night time in May 2010. The data imply that calcines and mine wastes piles located at Dashuixi and on-going artisanal Hg mining activities at Supeng were major sources of atmospheric mercury in WMMA. For a full year (May 2010 to May 2011), sampling of precipitation and throughfall were conducted on a weekly basis at three sites (Shenchong, Dashuixi, and Supeng) within WMMA. Hg in deposition was characterized by analysis of total Hg (THg) and dissolved Hg (DHg) concentrations. The corresponding data exhibit a high degree of variability, both temporarily and spatially. The volume-weighted mean THg concentrations in precipitation and throughfall samples were 502.6 ng l−1 and 977.8 ng l−1 at Shenchong, 814.1 ng l−1and 3392.1 ng l−1 at Dashuixi, 7490.1 ng l−1and 9641.5 ng l−1 at Supeng, respectively. THg was enhanced in throughfall compared to wet deposition samples by up to a factor of 7. The annual wet Hg deposition fluxes were 29.1, 68.8 and 593.1 μg m−2 yr−1 at Shenchong, Dashuixi and Supeng, respectively, while the annual dry Hg deposition fluxes were estimated to be 378.9, 2613.6 and 6178 μg m−2 yr−1 at these sites, respectively. Dry deposition played a dominant role in total atmospheric Hg deposition in WMMA since the dry deposition fluxes were 10.4–37.9 times higher than the wet deposition fluxes during the whole sample period. Our data showed that air deposition was still an important pathway of Hg contamination to the local environment in WMMA.


2016 ◽  
Vol 16 (12) ◽  
pp. 7653-7662 ◽  
Author(s):  
Jin-Su Han ◽  
Yong-Seok Seo ◽  
Moon-Kyung Kim ◽  
Thomas M. Holsen ◽  
Seung-Muk Yi

Abstract. In this study, mercury (Hg) was sampled weekly in dry and wet deposition and throughfall and monthly in litterfall, and as it was volatilized from soil from August 2008 to February 2010 to identify the factors influencing the amount of atmospheric Hg deposited to forested areas in a temperate deciduous forest in South Korea. For this location there was no significant correlation between the estimated monthly dry deposition flux (litterfall + throughfall – wet deposition) (6.7 µg m−2 yr−1) and directly measured dry deposition (9.9 µg m−2 yr−1) likely due primarily to Hg losses from the litterfall collector. Dry deposition fluxes in cold seasons (fall and winter) were lower than in warmer seasons (spring and summer). The volume-weighted mean (VWM) Hg concentrations in both precipitation and throughfall were highest in winter, likely due to increased scavenging by snow events. Since South Korea experiences abundant rainfall in summer, VWM Hg concentrations in summer were lower than in other seasons. Litterfall fluxes were highest in the late fall to early winter, when leaves were dropped from the trees (September to November). The cumulative annual Hg emission flux from soil was 6.8 µg m−2 yr−1. Based on these data, the yearly deposition fluxes of Hg calculated using two input approaches (wet deposition + dry deposition or throughfall + litterfall) were 6.8 and 3.6 µg m−2 yr−1, respectively. This is the first reported study which measured the amount of atmospheric Hg deposited to forested areas in South Korea, and thus our results provide useful information to compare against data related to Hg fate and transport in this part of the world.


2019 ◽  
Author(s):  
Aryeh Feinberg ◽  
Moustapha Maliki ◽  
Andrea Stenke ◽  
Bruno Sudret ◽  
Thomas Peter ◽  
...  

Abstract. An estimated 0.5–1 billion people globally have inadequate intakes of selenium (Se), due to a lack of bioavailable Se in agricultural soils. Deposition from the atmosphere, especially through precipitation, is an important source of Se to soils. However, very little is known about the atmospheric cycling of Se. It has therefore been difficult to predict how far Se travels in the atmosphere and where it deposits. To answer these questions, we have built the first global atmospheric Se model by implementing Se chemistry into an aerosol–chemistry–climate model, SOCOL-AER. In the model, we include information from the literature about the emissions, speciation, and chemical transformation of atmospheric Se. Natural processes and anthropogenic activities emit volatile Se compounds, which oxidize quickly and partition to the particulate phase. Our model tracks the transport and deposition of Se in 7 gas-phase species and 41 aerosol tracers. However, there are large uncertainties associated with many of the model's input parameters. In order to identify which model uncertainties are the most important for understanding the atmospheric Se cycle, we conducted a global sensitivity analysis with 34 input parameters related to Se chemistry, Se emissions, and the interaction of Se with aerosols. In the first bottom-up estimate of its kind, we have calculated a median global atmospheric lifetime of 4.4 d (days), ranging from 2.9–6.4 d (2nd–98th percentile) given the uncertainties of the input parameters. The uncertainty in the Se lifetime is mainly driven by the uncertainty in the carbonyl selenide (OCSe) oxidation rate and the lack of tropospheric aerosol species other than sulfate aerosols in SOCOL-AER. In contrast to uncertainties in Se lifetime, the uncertainty in deposition flux maps are governed by Se emission factors, with all four Se sources (volcanic, marine biosphere, terrestrial biosphere, and anthropogenic emissions) contributing equally to the uncertainty in deposition over agricultural areas. We evaluated the simulated Se wet deposition fluxes from SOCOL-AER with a compiled database of rainwater Se measurements, since wet deposition contributes around 80 % of total Se deposition. Despite difficulties in comparing a global, coarse resolution model with local measurements from a range of time periods, past Se wet deposition measurements are within the range of the model's 2nd–98th percentile at 79 % of background sites. This agreement validates the application of the SOCOL-AER model to identifying regions which are at risk of low atmospheric Se inputs. In order to constrain the uncertainty in Se deposition fluxes over agricultural soils we should prioritize field campaigns measuring Se emissions, rather than laboratory measurements of Se rate constants.


2020 ◽  
Vol 20 (3) ◽  
pp. 1363-1390 ◽  
Author(s):  
Aryeh Feinberg ◽  
Moustapha Maliki ◽  
Andrea Stenke ◽  
Bruno Sudret ◽  
Thomas Peter ◽  
...  

Abstract. An estimated 0.5–1 billion people globally have inadequate intakes of selenium (Se), due to a lack of bioavailable Se in agricultural soils. Deposition from the atmosphere, especially through precipitation, is an important source of Se to soils. However, very little is known about the atmospheric cycling of Se. It has therefore been difficult to predict how far Se travels in the atmosphere and where it deposits. To answer these questions, we have built the first global atmospheric Se model by implementing Se chemistry in an aerosol–chemistry–climate model, SOCOL-AER (modeling tools for studies of SOlar Climate Ozone Links – aerosol). In the model, we include information from the literature about the emissions, speciation, and chemical transformation of atmospheric Se. Natural processes and anthropogenic activities emit volatile Se compounds, which oxidize quickly and partition to the particulate phase. Our model tracks the transport and deposition of Se in seven gas-phase species and 41 aerosol tracers. However, there are large uncertainties associated with many of the model's input parameters. In order to identify which model uncertainties are the most important for understanding the atmospheric Se cycle, we conducted a global sensitivity analysis with 34 input parameters related to Se chemistry, Se emissions, and the interaction of Se with aerosols. In the first bottom-up estimate of its kind, we have calculated a median global atmospheric lifetime of 4.4 d (days), ranging from 2.9 to 6.4 d (2nd–98th percentile range) given the uncertainties of the input parameters. The uncertainty in the Se lifetime is mainly driven by the uncertainty in the carbonyl selenide (OCSe) oxidation rate and the lack of tropospheric aerosol species other than sulfate aerosols in SOCOL-AER. In contrast to uncertainties in Se lifetime, the uncertainty in deposition flux maps are governed by Se emission factors, with all four Se sources (volcanic, marine biosphere, terrestrial biosphere, and anthropogenic emissions) contributing equally to the uncertainty in deposition over agricultural areas. We evaluated the simulated Se wet deposition fluxes from SOCOL-AER with a compiled database of rainwater Se measurements, since wet deposition contributes around 80 % of total Se deposition. Despite difficulties in comparing a global, coarse-resolution model with local measurements from a range of time periods, past Se wet deposition measurements are within the range of the model's 2nd–98th percentiles at 79 % of background sites. This agreement validates the application of the SOCOL-AER model to identifying regions which are at risk of low atmospheric Se inputs. In order to constrain the uncertainty in Se deposition fluxes over agricultural soils, we should prioritize field campaigns measuring Se emissions, rather than laboratory measurements of Se rate constants.


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