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1.
This study, for the first time, investigates and quantifies the influence of slight changes in solution pH and ionic strength (IS) on colloidal microsphere deposition site coverage by Suwannee River Humic Acid (SRHA) in a column matrix packed with saturated iron-oxide coated sand.Triple pulse experimental (TPE) results show adsorbed SRHA enhances microsphere mobility more at higher pH and lower IS and covers more sites than at higher IS and lower pH. Random sequential adsorption (RSA) modelling of experimental data suggests 1 μg of adsorbed SRHA occupied 9.28 ± 0.03 × 109 sites at pH7.6 and IS of 1.6 mMol but covered 2.75 ± 0.2 × 109 sites at pH6.3 and IS of 20 mMol. Experimental responses are suspected to arise from molecular conformation changes whereby SRHA extends more at higher pH and lower ionic strength but is more compact at lower pH and higher IS. Results suggest effects of pH and IS on regulating SRHA conformation were additive.  相似文献   

2.
The estimated annual throughfall deposition flux of Hg in a northern mixed-hardwood forest in the Lake Huron Watershed was 10.5±1.0 μg m−2 compared to an annual precipitation Hg flux of 8.7±0.5 μg m−2 (June 1996–June 1997). The source of this additional Hg in throughfall is often attributed to wash-off of dry deposition, but foliar leaching of Hg may also be important. To determine the influence of both dry deposition and foliar leaching of Hg and other elements in throughfall, we measured a suite of trace elements (Hg, Al, Mg, V, Mn, Cu, Zn, As, Rb, Sr, Cd, Ba, La, Ce, and Pb) in throughfall, precipitation, and ambient air samples from a northern mixed-hardwood forest. Based on a multiple linear regression model, dry deposition had the most important influence on Hg, Al, La, Ce, V, As, Cu, Zn, Cd, and Pb fluxes while foliar leaching strongly influenced Mg, Mn, Rb, Sr, and Ba fluxes in net throughfall. The Hg dry deposition flux was estimated using gaseous and aerosol Hg measurements and modeled deposition velocities. The calculated dry deposition flux (∼12–14 μg m−2) of Hg to the canopy indicated that atmospheric deposition of Hg could easily account for all of the Hg deposited in net throughfall (1.9±0.1 μg m−2). Although there is a large uncertainty associated with these techniques, the modeling estimates indicate that atmospheric Hg may account for all of the Hg deposited in litterfall (11.4±2.8 μg m−2).  相似文献   

3.
Daily ozone deposition flux to a Norway spruce forest in Czech Republic was measured using the gradient method in July and August 2008. Results were in good agreement with a deposition flux model. The mean daily stomatal uptake of ozone was around 47% of total deposition. Average deposition velocity was 0.39 cm s−1 and 0.36 cm s−1 by the gradient method and the deposition model, respectively. Measured and modelled non-stomatal uptake was around 0.2 cm s−1. In addition, net ecosystem production (NEP) was measured by using Eddy Covariance and correlations with O3 concentrations at 15 m a.g.l., total deposition and stomatal uptake were tested. Total deposition and stomatal uptake of ozone significantly decreased NEP, especially by high intensities of solar radiation.  相似文献   

4.
It has been postulated that atmospheric pathways may comprise a significant source of nitrogen for aquatic ecosystems and excess atmospheric deposition to coastal areas may be a major cause of eutrophication. Dry deposition of nitrogen containing particles is a potential, but poorly quantified pathway, for atmospheric nitrogen flux. This pathway is not well quantified because deposition velocities for particles are difficult to calculate and incorporate substantial uncertainties. Herein we employ an amended version of the Hummelshøj et al. (1992, Proceedings of the 5th International Conference on Precipitation Scavenging and Atmosphere–Surface Exchange Processes. AMS, Richland, Washington, USA, 12pp.) model to calculate size-segregated dry deposition of particle inorganic nitrogen compounds to the western Baltic during the late Spring of 1997 based on data collected as part of the Air–Sea Exchange Process Study (ASEPS). The results show that over a 15 d period in April and May dry deposition fluxes varied between 30 and 400 μg m-2 d-1 for nitrate and 1 and 120 μg m-2 d-1 for ammonium. Sensitivity analyses run to assess the potential bounds on actual dry deposition indicate that, for reasonable variation of model parameters and formulation, particle nitrogen dry deposition may be varied by up to an order of magnitude. The primary sources of uncertainty are identified and are discussed in the context of alternative model formulations.  相似文献   

5.
《Chemosphere》2013,90(11):1414-1418
Nano-MgO is a good bactericide but with strong alkalinity in water due to its rapid hydrolysis. To control its hydrolysis rate and keep its bactericidal properties, we synthesized nano-MgO microspheres using chitosan–alginate system in this study. The synthesized nano-MgO release-controlled microspheres (nMgO-RCM) were with 0.98–1.20 mm of particle sizes. Also, their embedding ratio and loading percentage was 63.52% and 12.27%, respectively. Based on the characterization results, nano-MgO was only observed on surface of the nMgO-RCM. Its release rate from the nMgO-RCM could be controlled by the chitosan–alginate system, and the observed rate constant (kobs) increased from 0.0289 h−1 to 0.0358 h−1 with the increment of the dosage from 10 mg L−1 to 80 mg L−1. Furthermore, the nMgO-RCM could maintain pH value lower than 8.5 and colony counts less than 20 CFU mL−1 for at least 120 h.  相似文献   

6.
Seasonal patterns of atmospheric mercury (Hg) fluxes measured over vegetated terrestrial systems can provide insight into the underlying process controlling emission and deposition of Hg to vegetated surfaces. Gaseous elemental Hg fluxes were measured for week-long periods in each season (spring, summer, fall, and winter) over an uncontaminated high-elevation wetland meadow in Shenandoah National Park, Virginia using micrometeorological methods. Mean net deposition was observed in the spring (?4.8 ng m?2 h?1), emission in the summer (2.5 ng m?2 h?1), near zero flux in the fall (0.3 ng m?2 h?1), and emission in the winter (4.1 ng m?2 h?1). Nighttime deposition (when stomata are closed) and the poor correlation between Hg fluxes and canopy conductance during periods of active vegetation growth suggest that stomatal processes are not the dominant mechanism for ecosystem-level GEM exchange at this site. The strong springtime deposition relative to summer implies that young vegetation is better at scavenging Hg, with the highest deposition occurring at night possibly via a cuticular pathway. These results suggest that spring is a period of GEM deposition while other seasons exhibit net emission, emphasizing the importance of capturing GEM flux seasonality when determining total Hg budgets.  相似文献   

7.
Numerical sensitivity tests and four months of complete model runs have been conducted for the Routine Deposition Model (RDM). The influence of individual model inputs on dry deposition velocity as a function of land-use category (LUC) and pollutant (SO2, O3, SO2−4 and HNO3) were examined over a realistic range of values for solar radiation, stability and wind speed. Spatial and temporal variations in RDM deposition velocity (Vd) during June – September 1996 time period generated using meteorological input from a mesoscale model run at 35 km resolution over north-eastern North America were also examined. Comparison of RDM Vd values to a variety of measurements of dry deposition velocities of SO2, O3, SO2−4 and NHO3 that have been reported in the literature demonstrated that RDM produces realistic results. Over northeastern NA RDM monthly averaged dry deposition velocities for SO2 vary from 0.2 to 3.0 cm s−1 with the highest deposition velocities over water surfaces. For O3, the monthly averaged dry deposition velocities are from 0.05 to 1.0 cm s−1 with the lowest values over water surfaces and the highest over forested areas. For HNO3, the monthly averaged dry deposition velocities have the range of 0.5 to 6 cm s−1, with the highest values for forested areas. For SO2−4, they range from 0.05–1.5 cm s−1, with the lowest values over water and the highest over forest. The monthly averaged dry deposition velocities for SO2 and O3 are higher in the growing season compared to the fall, but this behaviour is not apparent for HNO3 and sulphate. In the daytime, the hourly averaged dry deposition velocities for SO2, O3, SO2−4 and HNO3 are higher than that in the nighttime over most of the vegetated area. The diurnal variation is most evident for surfaces with large values for leaf area index (LAI), such as forests. Based on the results presented in this paper, it is concluded that RDM Vd values can be combined with measured air concentrations over hourly, daily or weekly periods to determine dry deposition amounts and with wet deposition measurements to provide seasonal estimates of total deposition and estimates of the relative importance of dry deposition.  相似文献   

8.
Because aerosol particle deposition is an important factor in indoor air quality, many empirical and theoretical studies have attempted to understand the process. In this study, we estimated the deposition rate of aerosol particles on smooth aluminum surfaces inside a test chamber. We investigated the influence of turbulent intensity due to ventilation and fan operation. We also investigated two important processes in particle deposition: turbophoresis, which is significant for micron particles, and coagulation, which is relevant to ultrafine particles (UFP diameter <0.1 μm) at high particle concentrations. Our analysis included semi-empirical estimates of the deposition rates that were compared to available deposition models and verified with simulations of an aerosol dynamics model. In agreement with previous studies, this study found that induced turbulent intensity greatly enhanced deposition rates of fine particles (FP diameter <1 μm). The deposition rate of FP was proportional to the ventilation rate, and it increased monotonically with fan speed. With our setup, turbophoresis was very important for coarse particles larger than 5 μm. The coagulation of aerosol particles was insignificant when the particle concentration was less than 104 cm?3 during fan operation. The model simulation results verified that the aerosol dynamics module incorporated in our Multi-Compartment and Size-Resolved Indoor Aerosol Model (MC-SIAM) was valid. The behavior of aerosol particles inside our chamber was similar to that found in real-life conditions with the same ventilation rates (0.018–0.39 h?1) and similar air mixing modes. Therefore, our findings provide insight into indoor particle behavior.  相似文献   

9.
Tests of the dry deposition of ozone to the surfaces of a concrete floor tile and an activated carbon cloth (ACC) sample were performed in a deposition chamber. The time-dependent deposition of ozone to the material surfaces was modelled with an adsorption, desorption, reaction model. This made it possible to find deposition velocities at equilibrium, at t=∞, from shorter time runs of 48 h. The total equilibrium deposition velocity on the concrete floor tile was found to decrease from 0.08(10) to 0.057(10) cm s−1 in three consecutive runs on the same sample, and was found to be 0.137(8) cm s−1 on an ACC. All at a linear airflow velocity of 0.092 cm s−1, RH=50% and T=22°C. Varying the airflow in the deposition chamber, the surface deposition velocity was found to equal to the total deposition velocity for the concrete floor tile. A surface deposition velocity of 0.186(8) cm s−1 was found for the ACC sample. The total real area and the reaction rate constant for the decomposition of ozone was found to be larger, and the adsorption rate constant, the desorption rate constant and the mass of ozone on the surface smaller, on the ACC sample than on the concrete floor tile.  相似文献   

10.
The potential of alpine moss-sedge heath to recover from elevated nitrogen (N) deposition was assessed by transplanting Racomitrium lanuginosum shoots and vegetation turfs between 10 elevated N deposition sites (8.2-32.9 kg ha−1 yr−1) and a low N deposition site, Ben Wyvis (7.2 kg ha−1 yr−1). After two years, tissue N of Racomitrium shoots transplanted from higher N sites to Ben Wyvis only partially equilibrated to reduced N deposition whereas reciprocal transplants almost matched the tissue N of indigenous moss. Unexpectedly, moss shoot growth was stimulated at higher N deposition sites. However, moss depth and biomass increased in turfs transplanted to Ben Wyvis, apparently due to slower shoot turnover (suggested to result partly from decreased tissue C:N slowing decomposition), whilst abundance of vascular species declined. Racomitrium heath has the potential to recover from the impacts of N deposition; however, this is constrained by the persistence of enhanced moss tissue N contents.  相似文献   

11.
The Metropolitan Area of Buenos Aires (MABA) is the third mega-city in Latin America. Atmospheric N emitted in the area deposits to coastal waters of de la Plata River. This study describes the parameterizations included in DAUMOD-RD (v.3) model to evaluate concentrations of nitrogen compounds (nitrogen dioxide, gaseous nitric acid and nitrate aerosol) and their total (dry and wet) deposition to a water surface. This model is applied to area sources and CALPUFF model to point sources of NOx in the MABA. The models are run for 3 years of hourly meteorological data, with a spatial resolution of 1 km2. Mean annual deposition is 69, 728 kg-N year?1 over 2 339 km2 of river. Dry deposition contributions of N-NO2, N-HNO3 and N-NO3? to this value are 44%, 22% and 20%, respectively. Wet deposition of N-HNO3 and N-NO3? represents 3% and 11% of total annual value, respectively. This very low contribution results from the rare occurrence of rainy hours with wind blowing from the city to the river. Monthly dry deposition flux estimated for coastal waters of MABA varies between 7 and 13 kg-N km?2 month?1. These results are comparable to values reported for other coastal zones in the world.  相似文献   

12.
Dry atmospheric deposition contributes a significant amount of phosphorus to the Everglades of South Florida. Measurement of this deposition is problematic, because samples often are contaminated to varying degrees by bird droppings and other foreign materials. This study attempted to detect and remove the outliers in phosphorus (P) flux rates measured from dry deposition samples. Visual inspection of the samples, recorded in field notes, found that 30.1% of the samples contained animal droppings and frogs. Some of the samples with droppings and frogs (2.3%) had P values greater than 884 μg P m−2 d−1 (a value twice the standard deviation of the raw data mean), and were removed from further analysis. Outlier detection statistics based on a linear regression were then used for additional data screening. Eight stations in the network of 19 were removed because high contamination precluded the use of the regression model. Of the remaining samples, 15.7% were identified through the regression procedure as contaminated and were removed. The 11 station mean for P dry deposition was 85.8±79.0 μg P m−2 d−1, prior to the regression analysis, and 74.8±75.1 μg P m−2 d−1 after removal.  相似文献   

13.
Increases in reactive nitrogen deposition are a growing concern in the U.S. Rocky Mountain west. The Rocky Mountain Airborne Nitrogen and Sulfur (RoMANS) study was designed to improve understanding of the species and pathways that contribute to nitrogen deposition in Rocky Mountain National Park (RMNP). During two 5-week field campaigns in spring and summer of 2006, the largest contributor to reactive nitrogen deposition in RMNP was found to be wet deposition of ammonium (34% spring and summer), followed by wet deposition of nitrate (24% spring, 28% summer). The third and fourth most important reactive nitrogen deposition pathways were found to be wet deposition of organic nitrogen (17%, 12%) and dry deposition of ammonia (14%, 16%), neither of which is routinely measured by air quality/deposition networks operating in the region. Total reactive nitrogen deposition during the spring campaign was determined to be 0.45 kg ha−1 and more than doubled to 0.95 kg ha−1 during the summer campaign.  相似文献   

14.
For more than a decade, anthropogenic sulfur (S) and nitrogen (N) deposition has been identified as a key pollutant in the Arctic. In this study new critical loads of acidity (S and N) were estimated for terrestrial ecosystems north of 60° latitude by applying the Simple Mass Balance (SMB) model using two critical chemical criteria (Al/Bc = 1 and ANCle = 0). Critical loads were exceeded in large areas of northern Europe and the Norilsk region in western Siberia during the 1990s, with the more stringent criterion (ANCle = 0) showing the larger area of exceedance. However, modeled deposition estimates indicate that mean concentrations of sulfur oxides and total S deposition within the Arctic almost halved between 1990 and 2000. The modeled exceeded area is much reduced when currently agreed emission reductions are applied, and almost disappears under the implementation of maximum technically feasible reductions by 2020. In northern North America there was no exceedance under any of the deposition scenarios applied. Modeled N deposition was less than 5 kg ha−1 y−1 almost across the entire study area for all scenarios; and therefore empirical critical loads for the eutrophying impact of nitrogen are unlikely to be exceeded. The reduction in critical load exceedances is supported by observed improvements in surface water quality, whereas the observed extensive damage of terrestrial vegetation around the mining and smelter complexes in the area is mainly caused by direct impacts of air pollution and metals.  相似文献   

15.
The Florida Everglades Dry-Deposition Study (FEDDS) was designed to test the viability of using new and existing measurement techniques in the estimation of the dry-depositional loading of speciated mercury (elemental gaseous, reactive gaseous and particulate) to a mixed sawgrass (Cladium jamaicense) and cattail (Typha domingensis) stand within the Florida Everglades. Measurement intensives were performed during 24 February–04 March 1999 and 05–21 June 2000, which corresponded to the climatological dry and wet seasons in South Florida, respectively. During these intensives, direct measurements of mercury dry-deposition were made using a newly developed surrogate water surface technique. These direct measurements were compared with modeled estimates of mercury dry-deposition to the site that were obtained through the use of an inferential or “bigleaf” model that was modified for use with speciated mercury. On-site measurements of ambient speciated mercury concentrations and numerous micrometeorological variables were used as input to the model.The average mercury dry-deposition measured during the 1999 FEDDS measurement intensive was 13.3±4.0 ng m−2 day−1, while the modeled deposition for this period was 3.4±2.3 ng m−2 day−1. The average mercury dry-deposition measured during the 2000 FEDDS measurement intensive was lower, 5.9±2.8 ng m−2 day−1, while the average modeled deposition for this period was 1.8±0.6 ng m−2 day−1. A least-squares linear regression suggests that the model was able to explain 74% and 73% of the variability in the datasets for the 1999 and 2000 FEDDS intensives, respectively. While reported reductions in total mercury emissions across South Florida between study periods could explain the reductions in both the measured and predicted mercury dry-deposition estimates, the increased presence of cumulus convection during the summer-intensive could have also resulted in a removal of reactive and particulate mercury species within the atmosphere of South Florida.  相似文献   

16.
Adsorption of natural organic matter (NOM) on nanoparticles can have dramatic impacts on particle dispersion resulting in altered fate and transport as well as bioavailability and toxicity. In this study, the adsorption of Suwannee River humic acid (SRHA) on silver nanoparticles (nano-Ag) was determined and showed a Langmuir adsorption at pH 7 with an adsorption maximum of 28.6 mg g−1 nano-Ag. It was also revealed that addition of <10 mg L−1 total organic carbon (TOC) increased the total Ag content suspended in the aquatic system, likely due to increased dispersion. Total silver content decreased with concentrations of NOM greater than 10 mg TOC L−1 indicating an increase in nanoparticle agglomeration and settling above this concentration. However, SRHA did not have any significant effect on the equilibrium concentration of ionic Ag dissolved in solution. Exposure of Daphnia to nano-Ag particles (50 μg L−1 and pH 7) produced a linear decrease in toxicity with increasing NOM. These results clearly indicate the importance of water chemistry on the fate and toxicity of nanoparticulates.  相似文献   

17.
We investigate how a recently suggested pathway for production of secondary organic aerosol (SOA) affects the consistency of simulated organic aerosol (OA) mass in a global three-dimensional model of oxidant-aerosol chemistry (GEOS-Chem) versus surface measurements from the interagency monitoring of protected visual environments (IMPROVE) network. Simulations in which isoprene oxidation products contribute to SOA formation, with a yield of 2.0% by mass reduce a model bias versus measured OA surface mass concentrations. The resultant increase in simulated OA mass concentrations during summer of 0.6–1.0 μg m−3 in the southeastern United States reduces the regional RMSE to 0.88 μg m−3 from 1.26 μg m−3. Spring and fall biases are also reduced, with little change in winter when isoprene emissions are negligible.  相似文献   

18.
A 60-m flux tower was built on a 2100 m mountain for the measurement of the air pollutant concentration and the evaluation of dry deposition velocity in Central Taiwan. The tower was constructed in an evergreen broadleaf forest, which is the dominant species of forest in the world. Multiple-level SO2 concentrations and meteorological variables at the site were measured from February to April 2008. The results showed that the mean dry deposition velocities of SO2 were 0.61 cm s?1 during daytime and 0.27 cm s?1 during nighttime. From the comparison of the monthly data, a tendency was observed that the dry deposition velocity increases with LAI and solar radiation. Furthermore, it was observed that the deposition velocity was larger over wet canopy than over dry canopy, and that higher deposition velocities in the wet season were mainly caused by non-stomatal uptake of wet canopy. Over wet canopy, the mean dry deposition velocities of SO2 were estimated to be 0.83 cm s?1 during daytime and 0.47 cm s?1 during nighttime; and 0.44 cm s?1 during daytime and 0.19 cm s?1 during nighttime over dry canopy. There is good agreement between the results of this study and those in other studies and the predictions of Zhang et al. (2003a). The medians (geometric means) of derived rc during daytime are 233 (266) m s?1 over dry canopy and 147 (146) m s?1 over wet canopy. It was found that solar radiation is the critical important meteorological variable determining stomatal resistance during daytime. For non-stomatal resistance, clear dependencies were observed on the friction velocity and relative humidity.  相似文献   

19.
A survey of 153 acid grasslands from the Atlantic biogeographic region of Europe indicates that chronic nitrogen deposition is changing plant species composition and soil and plant-tissue chemistry. Across the deposition gradient (2-44 kg N ha−1 yr−1) grass richness as a proportion of total species richness increased whereas forb richness decreased. Soil C:N ratio increased, but soil extractable nitrate and ammonium concentrations did not show any relationship with nitrogen deposition. The above-ground tissue nitrogen contents of three plant species were examined: Agrostis capillaris (grass), Galium saxatile (forb) and Rhytidiadelphus squarrosus (bryophyte). The tissue nitrogen content of neither vascular plant species showed any relationship with nitrogen deposition, but there was a weak positive relationship between R. squarrosus nitrogen content and nitrogen deposition. None of the species showed strong relationships between above-ground tissue N:P or C:N and nitrogen deposition, indicating that they are not good indicators of deposition rate.  相似文献   

20.
Atmospheric deposition of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) was investigated at four locations, namely at Yuancun, Wushan, Haizhu and Changban in Guangzhou City, Guangdong Province. The annual deposition fluxes of tetra- to octa-CDD/Fs (total PCDD/Fs) were found to range from 170 to 3000 (mean 1500) pg m−2 day−1, and the fluxes of total 2, 3, 7, 8-substituted PCDD/F congeners ranged from 2.1 to 41 (mean 20) pg WHO-TEQ m−2 day−1 at Wushan. The average deposition fluxes of total 2, 3, 7, 8-substituted PCDD/F congeners in rainy season were found to be 37, 27 and 28 pg WHO-TEQ m−2 day−1 at Yuancun, Haizhu and Changban, respectively, and the PCDD/F deposition fluxes behaved obviously higher in rainy season than in dry season. Results from regression analysis showed that number of rainy days, the amount of wet precipitation, PCDD/F concentrations in particles and organic carbon content played important roles in the variation of PCDD/F deposition fluxes. Monthly average temperatures change little over the year. Therefore, it only played a minor role in monthly variation of PCDD/F deposition fluxes. Particle deposition fluxes were generally not considered as the factor that could cause the differences in PCDD/F deposition fluxes between rainy and dry season, but were found to be related with PCDD/F deposition fluxes in rainy season or dry season. It was found that the profiles of PCDD/F homologs or congeners in the samples were the same either spatially or temporally, indicating that the PCDD/F emission sources were similar to one another. The similarities in PCDD/F homolog patterns and the differences in deposition fluxes between samples collected from heavy-traffic roadside and nearby residence house roof indicated that vehicle exhaust might be an important source for PCDD/F in Guangzhou. PCDD/F concentrations and profiles of PCDD/F homologs in atmospheric deposition were compared with those in both total suspended particles in air and soils, and conclusions indicated that atmospheric deposition possibly tended to remove lower-chlorinated DD/Fs from air and was one of sources for PCDD/Fs in soils.  相似文献   

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