Deposition and removal of fugitive dust in the arid southwestern United States: measurements and model results

This work was motivated by the need to better reconcile emission factors for fugitive dust with the amount of geologic material found on ambient filter samples. The deposition of particulate matter with aerodynamic diameter less than or equal to 10 microm (PM10), generated by travel over an unpaved road, over the first 100 m of transport downwind of the road was examined at Ft. Bliss, near El Paso, TX. The field conditions, typical for warm days in the arid southwestern United States, represented sparsely vegetated terrain under neutral to unstable atmospheric conditions. Emission fluxes of PM10 dust were obtained from towers downwind of the unpaved road at 7, 50, and 100 m. The horizontal flux measurements at the 7 m and 100 m towers indicated that PM10 deposition to the vegetation and ground was too small to measure. The data indicated, with 95% confidence, that the loss of PM10 between the source of emission at the unpaved road, represented by the 7 m tower, and a point 100 m downwind was less than 9.5%. A Gaussian model was used to simulate the plume. Values of the vertical standard deviation sigma(z) and the deposition velocity Vd were similar to the U.S. Environmental Protection Agency (EPA) ISC3 model. For the field conditions, the model predicted that removal of PM10 unpaved road dust by deposition over the distance between the point of emission and 100 m downwind would be less than 5%. However, the model results also indicated that particles larger than 10 microm (aerodynamic diameter) would deposit more appreciably. The model was consistent with changes observed in size distributions between 7 m and 100 m downwind, which were measured with optical particle counters. The Gaussian model predictions were also compared with another study conducted over rough terrain and stable atmospheric conditions. Under such conditions, measured PM10 removal rates over 95 m of downwind transport were reported to be between 86% and 89%, whereas the Gaussian model predicted only a 30% removal. One explanation for the large discrepancy between measurements and model results was the possibility that under the conditions of the study, the dust plume was comparable in vertical extent to the roughness elements, thereby violating one of the model assumptions. Results of the field study reported here and the previous work over rough terrain bound the extent of particle deposition expected to occur under most unpaved road emission scenarios.     

Long-term aerosol particle flux observations part I: Uncertainties and time-average statistics

Long-term eddy covariance particle flux measurements for the size range starting from 10 nm were performed at a boreal forest site in Southern Finland. The large variability in turbulent flux estimates is inherent to the particle flux observations and thus long-term particle flux measurements enable to obtain statistically significant results by a suitable averaging. The particle flux random errors were estimated and a parameterisation for the integral time scale of turbulent flux was proposed. Application of flux errors for classification according to statistical significance of single flux values leads to systematically different deposition estimates on ensemble average basis. This must be avoided for determination of unbiased average deposition fluxes. The role of storage term in particle deposition evaluation was analysed. It was empirically determined that the method of storage term estimation discussed by [Finnigan, J., 2006. The storage term in eddy flux calculations. Agric. Forest Meteorol., 136, 108–113.] is not sensitive to the selection of the concentration averaging window in both ends of the flux averaging period. It is argued that the storage change in real atmospheric conditions results from boundary layer development as well as source–sink activity and therefore the filtering effect arising from averaging the concentration is of less importance. Diurnal, seasonal and annual variability of particle fluxes was analysed and it was observed that particle deposition rates are higher in winter. More detailed analysis of functional dependencies of particle deposition on environmental factors as well as dependence on size will be done in the second part of the paper.     

Simulation of the evolution of particle size distributions containing coarse particulate in the atmospheric surface layer with a simple convection-diffusion-sedimentation model

The Fugitive Dust Model (FDM) and Industrial Source Complex (ISC), widely used coarse particulate dispersion models, have been shown inaccurate due to the neglect of vertical variations in atmospheric wind speed and turbulent diffusivity (Vesovic et al., 2001), omission of the gravitational advection velocity, and an underestimation of the ground deposition velocity (Kim and Larson, 2001). A simple, transient two-dimensional convection-diffusion-sedimentation model is proposed to simulate the evolution in particle size distribution of an aerosol ‘puff’ containing coarse particulate in the atmospheric surface layer. Monin-Okhubov similarity theory, accompanied by empirical observations made by Businger et al. (1971), is adopted to characterize the surface layer wind speed and turbulent diffusivity profiles over a wide range of atmospheric conditions. A first order analysis of the crossing trajectories effect suggests simulation data presented here are not significantly affected by particle inertia. The model is validated against Suffield experimental data in which coarse particulate deposition was measured out to a distance of 800 m from the source (Walker, 1965). Good agreement is found for the decay in ground deposits with distance from the source for stable atmospheres. Deposition data was also simulated for unstable atmospheric stratification and the current model was determined to modestly underestimate the peak concentration with increasing accuracy further downwind of the release. The current model's effective deposition velocity was compared to that suggested by Kim et al. (2000) and shows improvement with respect to FDM. Lastly, the model was used to simulate the dispersion of nine lognormal aerosol puffs in the lowest 50 m of the atmospheric surface layer for four classes of atmospheric stability. The simulated mass median aerodynamic diameters (MMAD) at multiple downwind sampling locations were calculated and plotted with distance from the source. The first 50 m from the source was found to have a substantial impact on the evolution of MMAD for stable atmospheric conditions. Away from the source, it was observed that particle size distributions were truncated by removal of all particles larger than about 60 μm. A particle Peclet number was also defined to quantify the relative importance of turbulent dispersion and sedimentation on particle motion in the vertical direction.     

Apply appropriate models in the study of dry deposition fluxes of particulate matter and polycyclic aromatic hydrocarbons (PAHs) in Tsukuba, Japan

In this study, plates for downward flux and upward flux were used to measure atmospheric dry deposition fluxes for particulate mass and polycyclic aromatic hydrocarbons (PAHs) in TERC (Tsukuba), Japan. Ambient particles concentrations were also collected using a high-volume air sampler, and ambient particle size distributions between 0.01 μm and 13.1 μm were measured using a low-pressure cascade impactor to characterise the PAHs levels and dry deposition. The results indicated that the average cumulative fraction of dry deposition flux for particles and PAHs which attached with them was caused by the particle size of greater than 1.2-6.3 μm (97%).     

Overall dry deposition velocities of trace elements measured at harbor and traffic site in central Taiwan

For reasonable and convenient assessments of the characteristics of the dry deposition velocities between Taichung harbor site and Wuchi town site in central Taiwan, the overall dry deposition velocities of several metallic elements were calculated as the particulate diameter (D(p)) distributions of large particles (D(p) > 10 microm), coarse particles (10 microm < D(p) < 2.5 microm), and fine particles (D(p) < 2.5 microm) based on the ambient measurements during March-December of 2004. In this work, the dry deposition fluxes showed the higher correlation with coarse particle concentrations than large particle concentrations; however, the least well correlation was observed between the dry deposition fluxes and the fine particle concentrations. The calculated best-fit overall dry deposition velocities obtained using coarse particle concentrations varied from approximately 0.2 cm s(-1) for Cr to 1.5 cm s(-1) for Pb and 0.2 cm s(-1) for Fe to 2.6 cm s(-1) for Pb at Taichung harbor and Wuchi town site, respectively. In general, the crustal elements had higher deposition velocities than anthropogenic elements. In addition, overall dry deposition velocities for crustal elements were higher in Wuchi town site than in Taichung harbor site. The results identified the dry deposition flux was mainly contributed from large and coarse particles due to their high deposition velocities. The results also indicated that the best approach to estimate overall dry deposition was by depending on the characteristics of particles with diameters larger than 2.5 microm.     

Polycyclic aromatic hydrocarbon (PAH) deposition to and exchange at the air-water interface of Luhu, an urban lake in Guangzhou, China

Urban lakes are vulnerable to the accumulation of semivolatile organic compounds, such as PAHs from wet and dry atmospheric deposition. Little was reported on the seasonal patterns of atmospheric deposition of PAHs under Asian monsoon climate. Bulk (dry + wet) particle deposition, air-water diffusion exchange, and vapour wet deposition of PAHs in a small urban lake in Guangzhou were estimated based on a year-round monitoring. The total PAH particle deposition fluxes observed were 0.44-3.46 μg m⁻² day⁻¹. The mean air-water diffusive exchange flux was 20.7 μg m⁻² day⁻¹. The vapour deposition fluxes of PAHs ranged 0.15-8.26 μg m⁻² day⁻¹. Remarkable seasonal variations of particulate PAH deposition, air-water exchange fluxes and vapour wet deposition were influenced by seasonal changes in meteorological parameters. The deposition fluxes were predominantly controlled by the precipitation intensity in wet season whereas by atmospheric concentration in dry season.     

Dry deposition (downward, upward) concentration study of particulates and heavy metals during daytime, nighttime period at the traffic sampling site of Sha-Lu, Taiwan

Downward, upward dry deposition fluxes and total suspended particulate of particulate heavy metals (Fe, Pb, Zn, Cu, Mg and Mn) were measured in daytime and nighttime period in Sha-Lu, a small city in the central Taiwan during summer period of 2003. The results showed that the total suspended particulate concentrations of particulate mass in the daytime period (averaged 996.2 g/m3) were higher than in nighttime period (averaged 560.7 g/m3). And the downward dry deposition fluxes (averaged 54.07 g/m2s) were about two times as that of upward dry deposition fluxes (averaged 26.48 g/m2s) in the daytime period. Furthermore, the average downward dry deposition fluxes (averaged 26.22 g/m2s) were also about two times as that of upward dry deposition fluxes (averaged 12.11 g/m2s) in the nighttime period. In addition, the average downward dry deposition fluxes are greater than the upward dry deposition fluxes for all the heavy metals in either daytime or nighttime period. The proposed reasons are that the wind speed and concentration difference for daytime and nighttime period lead to these results at the traffic sampling site of central Taiwan. In addition, the deposition velocity for mass, heavy metals (Fe, Pb, Zn, Cu, Mg and Mn) during daytime and nighttime period were also calculated. The average daytime dry deposition velocity for downward particulate mass, upward particulate mass, Fe, Pb, Zn, Cu, Mg and Mn were 5.56, 2.66, 1.71, 0.18, 1.06, 0.24, 0.47 and 0.11 (cm/s), respectively. And the average nighttime dry deposition velocity for downward particulate mass, upward particulate mass, Fe, Pb, Zn, Cu, Mg and Mn were 4.70, 2.11, 1.66, 0.18, 0.86, 0.23, 0.32 and 0.07 (cm/s), respectively at traffic sampling site of central Taiwan.     

Comparison of annual dry and wet deposition fluxes of selected pesticides in Strasbourg, France

This work summarizes the results of a study of atmospheric wet and dry deposition fluxes of Deisopropyl-atrazine (DEA), Desethyl-atrazine (DET), Atrazine, Terbuthylazine, Alachlor, Metolachlor, Diflufenican, Fenoxaprop-p-ethyl, Iprodione, Isoproturon and Cymoxanil pesticides conducted in Strasbourg, France, from August 2000 through August 2001. The primary objective of this work was to calculate the total atmospheric pesticide deposition fluxes induced by atmospheric particles. To do this, a modified one-dimensional cloud water deposition model was used. All precipitation and deposition samples were collected at an urban forested park environment setting away from any direct point pesticide sources. The obtained deposition fluxes induced by atmospheric particles over a forested area showed that the dry deposition flux strongly contributes to the total deposition flux. The dry particle deposition fluxes are shown to contribute from 4% (DET) to 60% (cymoxanil) to the total deposition flux (wet + dry).     

Effect of atmospheric electricity on dry deposition of airborne particles from atmosphere

The electric mechanism of dry deposition is well known in the case of unattached radon daughter clusters that are unipolar charged and of high mobility. The problematic role of the electric forces in deposition of aerosol particles is theoretically examined by comparing the fluxes of particles carried by different deposition mechanisms in a model situation. The electric mechanism of deposition appears essential for particles of diameter 10–200 nm in conditions of low wind speed. The electric flux of fine particles can be dominant on the tips of leaves and needles even in a moderate atmospheric electric field of a few hundred V m⁻¹ measured over the plane ground surface. The electric deposition is enhanced under thunderclouds and high voltage power lines. Strong wind suppresses the relative role of the electric deposition when compared with aerodynamic deposition. When compared with diffusion deposition the electric deposition appears less uniform: the precipitation particulate matter on the tips of leaves and especially on needles of top branches of conifer trees is much more intensive than on the ground surface and electrically shielded surfaces of plants. The knowledge of deposition geometry could improve our understanding of air pollution damage to plants.     

Dry deposition fluxes and deposition velocities of PAHs at an urban site in Turkey

Even though dry deposition and air–water exchange of semivolatile organic compounds (SOCs) are important for surfaces in and around the urban areas, there is still no generally accepted direct measurement technique for dry deposition. In this study, a modified water surface sampler (WSS) configuration, including a filter holder and an XAD-2 resin column, was employed to investigate the polycyclic aromatic hydrocarbon (PAH) dry deposition in an urban area. The measured total (particle+dissolved) PAH fluxes to the WSS averaged to be 34 960±16 540 ng m⁻² d⁻¹. Average particulate PAH flux, determined by analyzing the filter in the WSS, was about 8% of the total PAH flux. Temporal flux variations indicated that colder months (October–April) had the highest PAH fluxes. This increase could be attributed to the residential heating as well as meteorological effects including lower mixing height. A high volume air sampler was concurrently employed to collect ambient air concentrations. The average total (gas+particle) atmospheric PAH concentration (456±524 ng m⁻³) was within the range of previously measured values at different urban locations. PAH concentrations in urban areas are more than two orders of magnitude higher than those measured in pristine areas and this result may indicate that urban areas have major source sectors and greater deposition rates are expected near to these areas. The average contribution of particle phase was about 10% in total concentration. Simultaneous particulate phase dry deposition and ambient air samples were collected in this study. Then, particulate phase apparent dry deposition velocities were calculated using the fluxes and concentrations for each PAH compound and they ranged from 0.1 to 1.2 cm s⁻¹. These values are in good agreement with previously reported values.     

Size partitioning of particulate inorganic nitrogen species between the fine and coarse mode ranges and its implication to their deposition on the surface ocean

In order to discuss the dry deposition fluxes of atmospheric fixed nitrogen species, observations of aerosol chemistry including nitrate (NO₃^?) and ammonium (NH₄⁺) were conducted at two islands, Rishiri Island and Sado Island, over the Sea of Japan. Although the atmospheric concentrations of particulate NH₄⁺–N showed higher values than those of particulate NO₃^?–N at both sites, the dry deposition fluxes of the particulate NO₃^?–N were estimated to be higher than those of the particulate NH₄⁺–N. This was caused by the difference of particle sizes between the particulate NO₃^? and NH₄⁺; NH₄⁺ was almost totally contained in fine particles (d < 2.5 μm) with smaller deposition velocity, whereas NO₃^? was mainly contained in coarse particles (d > 2.5 μm) with greater deposition velocity. Fine mode NO₃^? was strongly associated with fine mode sea-salt and mineral particles, of which higher concentrations shifted the size of particulate NO₃^? toward the fine mode range. This size shift would decrease the dry deposition flux of the fixed nitrogen species on coastal waters and accelerate atmospheric transport of them to the remote oceanic areas.     

Analysis of atmospheric behavior of PCDDs/PCDFs by a one-compartment box model

The overall atmospheric behavior of PCDDs/PCDFs in the Kanto region, Japan, was simulated by a one-compartment box model. For each homologue the relative significance and temperature dependences of dry deposition, wet deposition, degradation, and advection in both gas and particulate phases were examined and compared. The results of the model calculation suggested that the rates for dry deposition are comparable to those for wet deposition, and the rates for advection are comparable to those for bulk (dry+wet) depositions in the Kanto region. On the other hand, the rates of degradation for PCDDs/PCDFs in the atmosphere in the Kanto region would be negligible. The emission rates and the bulk deposition fluxes in the entire Kanto region estimated by the model calculation based on observed air concentrations were 0.084-0.90 kg-TEQ/month and 0.045-0.43 kg-TEQ/month, respectively. These estimated emission rates and bulk deposition fluxes were slightly higher than the estimated emission rate based on observed emission concentrations and the estimated bulk deposition fluxes based on observed deposition fluxes collected on water deposition surface, respectively. This study showed the model calculation can be available for understanding of the overall atmospheric behavior, verification of the source inventory, and estimation of deposition flux on the actual environment including various deposition surfaces.     

Atmospheric deposition of polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs) in urban and suburban areas of Korea

Bulk atmospheric samples (wet and dry) were collected monthly throughout a year at urban and suburban areas of Korea to assess the deposition flux and seasonal variations of polychlorinated dibenzo-p-dioxins (PCDDs) and dibenzofurans (PCDFs). The PCDDs/DFs deposition fluxes ranged from 1.0 to 3.7 ng TEQ/m²/year in the urban area and from 0.5 to 4.6 ng TEQ/m²/year in the suburban area. The deposition fluxes of PCDDs/DFs in this study were comparable to or lower than those previously reported at different locations. The atmospheric deposition fluxes of particles and PCDDs/DFs in winter tended to be higher than those in summer. However, monthly variations between particle and PCDDs/DFs deposition fluxes were small, and the correlation coefficients between the deposition fluxes of air particles and each homologue group of PCDDs/DFs varied according to the degree of chlorination of the homologue group. The deposition velocity of PCDDs/DFs in the urban area was estimated at 0.04 cm/s, which is a lower value than those found in other studies. The two most likely factors affecting the monthly variation of deposition fluxes are the ambient temperature and the amount of precipitation. In particular, the ambient temperature had an influence on the lower chlorinated homologues of PCDDs/DFs while precipitation had an influence on the higher chlorinated PCDDs/DFs. The PCDDs/DFs profiles in atmospheric deposition bulk samples showed a similar pattern at the urban and suburban sites. The possibility of the loading of PCDDs/DFs by Asian dust events could be partly confirmed by investigation of homologue profiles.     

On the influence of the urban roughness sublayer on turbulence and dispersion

The concept of the urban roughness sublayer is discussed and this lowest atmospheric layer over a rough surface is shown to have a non-negligible vertical extension over typical urban surfaces. The existing knowledge on the turbulence and flow structure within an urban roughness sublayer is reviewed, focusing on the height dependence of turbulent fluxes and a scaling approach for turbulence statistics, such as velocity variances, in the above-roof part of the roughness sublayer. Finally, the implication of this turbulence and flow structure upon dispersion characteristics is investigated. The most prominent difference of explicitly taking into account the roughness sublayer in a dispersion simulation (as compared to assuming a `constant flux layer') is a clearly enhanced ground level concentration far downwind from the source. For the example of a tracer release experiment over a (sub) urban surface (Copenhagen) it is shown that introducing the roughness sublayer clearly improves the model performance.     

Atmospheric particle size distributions of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polycyclic aromatic hydrocarbons (PAHs) and their implications for wet and dry deposition

Concurrent measurements of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polycyclic aromatic hydrocarbons (PAHs) in different size fractions of atmospheric particulate matter are presented for a winter and a summer sampling period. The PCDD/Fs and PAHs were primarily associated with particles of <1.35 μm aerodynamic diameter. The particle size distributions were similar for the compounds within each substance group and, surprisingly, also between the PCDD/Fs and PAHs. Changes in the particle size distribution of particle mass were reflected in the particle size distributions of the PCDD/Fs and PAHs.The data were employed to identify those particle size fractions dominating the wet and dry particle bound deposition of PCDD/Fs and PAHs and, furthermore, to assess the relative contributions of wet and dry deposition to the total particle bound deposition fluxes. The calculations indicate that coarse particles contribute most to the dry deposition while, in contrast, the wet deposition of the PCDD/Fs and PAHs is dominated by fine particles. Furthermore, it is estimated that in Bayreuth wet deposition dominates the total particle bound deposition of PCDD/Fs and PAHs.     

Atmospheric deposition of polychlorinated dibenzo-p-dioxins, polychlorinated dibenzofurans, and dioxin-like polychlorinated biphenyls in the Kanto Region, Japan

The atmospheric bulk (dry and wet) deposition of dioxins was investigated at four locations (Tokyo, Yokohama, Tsukuba, and Tanzawa) in the Kanto region (in Japan) over one year using a stainless-steel pot. Annual average polychlorinated dibenzo-p-dioxins/polychlorinated dibenzofurans (PCDD/PCDF) deposition fluxes were estimated to be from 450 to 1300 ng/m2/yr, and the annual average TEQ fluxes from 5.7 to 17 ng-TEQ/m2/yr at the four locations. The PCDD/PCDF deposition flux was higher in winter than in summer. The deposition flux could be related to ambient temperature, particularly for less chlorinated PCDDs/PCDFs, while the deposition flux is not necessarily related to the amount of precipitation. The PCDD/PCDF deposition flux increased as the particle deposition flux increased, for the winter samples. Based on the ratio of the PCDD/PCDF deposition fluxes to the particle deposition fluxes, the contribution of the reentrainment of soil particles to the TEQ of PCDD/PCDF deposition was considered to be negligible in this region. Based on the air concentrations monitored near our deposition sampling points by the municipalities, the ratio of the annual deposition flux to the annual average air concentration was roughly estimated to be 0.082 cm/s. The range of deposition flux in the Kanto region was estimated to be from 1.5 to 31 (median: 9.8) ng-TEQ/m2/yr based on the range of air concentration data measured by the municipalities. The total annual deposition flux in the entire Kanto region was estimated to range from 50 to 900 g-TEQ/yr (median 320 g-TEQ/yr). This estimated flux was of the same order as the sum of estimated emissions from municipal solid waste incinerators and industrial waste incinerators in the Kanto region. The contributions of dioxin-like PCBs in Yokohama, Tsukuba, and Tanzawa depositions were less than 10% of the total TEQ; however, in Tokyo it was almost equal to or more than 50%.     

Characteristics and impacts of trace elements in atmospheric deposition at a high-elevation site,southern China

To investigate the regional background trace element (TE) level in atmospheric deposition (dry and wet), TEs (Fe, Al, V, Cr, Mn, Ni, Cu, Zn, As, Se, Mo, Cd, Ba, and Pb) in 52 rainwater samples and 73 total suspended particles (TSP) samples collected in Mt. Lushan, Southern China, were analyzed using inductively coupled plasma-mass spectrometry (ICP-MS). The results showed that TEs in wet and dry deposition of the target area were significantly elevated compared within and outside China and the volume weight mean pH of rainwater was 4.43. The relative contributions of wet and dry depositions of TEs vary significantly among elements. The wet deposition fluxes of V, As, Cr, Se, Zn, and Cd exceeded considerably their dry deposition fluxes while dry deposition dominated the removal of pollution elements such as Mo, Cu, Ni, Mn, and Al. The summed dry deposition flux was four times higher than the summed wet deposition flux. Prediction results based on a simple accumulation model found that the content of seven toxic elements (Cr, Ni, Cu, Zn, As, Cd, and Pb) in soils could increase rapidly due to the impact of annual atmospheric deposition, and the increasing amounts of them reached 0.063, 0.012, 0.026, 0.459, 0.076, 0.004, and 0.145 mg kg^?1, respectively. In addition, the annual increasing rates ranged from 0.05% (Cr and Ni) to 2.08% (Cd). It was also predicted that atmospheric deposition induced the accumulation of Cr and Cd in surface soils. Cd was the critical element with the greatest potential ecological risk among all the elements in atmospheric deposition.     

Local to regional emission sources affecting mercury fluxes to New York lakes

Lake-sediment records across the Northern Hemisphere show increases in atmospheric deposition of anthropogenic mercury (Hg) over the last 150 years. Most of the previous studies have examined remote lakes affected by the global atmospheric Hg reservoir. In this study, we present Hg flux records from lakes in an urban/suburban setting of central New York affected also by local and regional emissions. Sediment cores were collected from the Otisco and Skaneateles lakes from the Finger Lakes region, Cross Lake, a hypereutrophic lake on the Seneca River, and Glacial Lake, a small seepage lake with a watershed that corresponds with the lake area. Sediment accumulation rates and dates were established by ²¹⁰Pb. The pre-anthropogenic regional atmospheric Hg flux was estimated to be 3.0 μg m⁻² yr⁻¹ from Glacial Lake, which receives exclusively direct atmospheric deposition. Mercury fluxes peaked during 1971–2001, and were 3 to more than 30 times greater than pre-industrial deposition. Land use change and urbanization in the Otisco and Cross watersheds during the last century likely enhanced sediment loads and Hg fluxes to the lakes. Skaneateles and Glacial lakes have low sediment accumulation rates, and thus are excellent indicators for atmospheric Hg deposition. In these lakes, we found strong correlations with emission records for the Great Lakes region that markedly increased in the early 1900s, and peaked during WWII and in the early 1970s. Declines in modern Hg fluxes are generally evident in the core records. However, the decrease in sediment Hg flux at Glacial Lake was interrupted and has increased since the early 1990s probably due to the operation of new local emission sources. Assuming the global Hg reservoir tripled since the pre-industrial period, the contribution of local and regional emission sources to central New York lakes was estimated to about 80% of the total atmospheric Hg deposition.     

Estimating contribution of precipitation scavenging of atmospheric particulate mercury to mercury wet deposition in Japan

Mercury wet deposition is dependent on both the scavenging of divalent reactive gaseous mercury (RGM) and atmospheric particulate mercury (Hg(p)) by precipitation. Estimating the contribution of precipitation scavenging of RGM and Hg(p) is important for better understanding the causes of the regional and seasonal variations in mercury wet deposition. In this study, the contribution of Hg(p) scavenging was estimated on the basis of the scavenging ratios of other trace elements (i.e., Cd, Cu, Mn, Ni, Pb and V) existing entirely in particulate form. Their wet deposition fluxes and concentrations in air, which were measured concurrently from April 2004 to March 2005 at 10 sites in Japan, were used in this estimation. The monthly wet deposition flux of mercury at each site correlated with the amount of monthly precipitation, whereas the Hg(p) concentrations in air tended to decrease during summer. There was a significant correlation (P<0.001) among the calculated monthly average scavenging ratios of trace elements, and the values in each month at each site were similar. Therefore, it is assumed the monthly scavenging ratio of Hg(p) is equivalent to the mean value of other trace elements. Using this scavenging ratio (W), the wet deposition flux (F) due to Hg(p) scavenging in each month was calculated by F=WKP, where K and P are the Hg(p) concentration and amount of precipitation, respectively. Relatively large fluxes due to Hg(p) scavenging were observed at a highly industrial site and at sites on the Japan Sea coast, which are strongly affected by the local sources and the long-range transport from the Asian continent, respectively. However, on average, at the 10 sites, the contribution of Hg(p) scavenging to the annual mercury deposition flux was 26%, suggesting that mercury wet deposition in Japan is dominated by RGM scavenging. This RGM should originate mainly from the in situ oxidation of Hg⁰ in the atmosphere.     

Concentration, size distribution, and dry deposition rate of particle-associated metals in the Los Angeles region

Daily averaged atmospheric concentrations and dry deposition fluxes of particulate metals were measured seasonally at six urban sites and one non-urban coastal site in the Los Angeles region using a conventional total suspended particulate matter (TSP) filter, surrogate surface deposition plates, and a Noll Rotary Impactor (NRI), which provides information about particle size distribution in four size ranges above 6 μm. With the exception of the non-urban site, particulate metal concentrations and deposition fluxes were remarkably uniform spatially and temporally. At all sites there were significant metal concentrations on particles greater than 10 μm, a commonly used upper limit for many air quality monitoring studies, and these large particles were estimated to be responsible for most of the deposited mass of metals. Annual averaged values of deposition rates measured with a surrogate surface were in good agreement with values estimated using theoretical deposition velocities in conjunction with measured size-segregated particle concentrations. Image analysis of particles deposited on NRI stage A, which collects all particles greater than 6 μm, indicated nighttime metal concentrations and deposition at the non-urban coastal site was higher than in the day time due to offshore advection of urban air associated with the diurnal land breeze. Measured enrichments of crustal elements and metals were correlated, indicating efficient mixing of natural and anthropogenic material from different sources, hypothesized to be the result of cyclical resuspension and deposition of dust by moving vehicles and wind.