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1.
The abilities of a screening-level model to predict variations in elemental mercury (Hg0) air emissions from soils in terrestrial landscapes are examined by comparing simulation results to published observational data and by performing sensitivity analyses. Despite uncertainties and simplifications, the model results obtained offer some degree of confidence in the model's joint ability to relate readily available environmental parameters to airborne emissions of Hg predicted by coupling simple atmospheric and soil parameters with Hg cycling and transport algorithms. The model reasonably predicted the observational data in the considered data sets except for one site for which significant uncertainty was associated with model input data. Predictions are consistent with many trends observed in the field studies; better predictions were obtained for nonvegetated systems (relative errors between 0.4 and 9.7%) than for shaded-soil landscapes (relative errors between 2.3 and 27%). The model reflected field data showing that daily average emission rates of Hg0, formed by the reduction of Hg(II), are primarily controlled by changes in solar radiation, soil moisture, temperature, and, to a lesser extent, wind conditions. The model may have potential use in several preliminary studies to characterize trends of airborne Hg emitted from terrestrial sources to the atmosphere.  相似文献   

2.
To improve the accuracy and applicability of vehicular emission models, this study proposes a speed and vehicle-specific power (VSP) modeling method to estimate vehicular emissions and fuel consumption using data gathered by a portable emissions monitoring system (PEMS). The PEMS data were categorized into discrete speed-VSP bins on the basis of the characteristics of vehicle driving conditions and emissions in Chinese cities. Speed-VSP modal average rates of emissions (or fuel consumption) and the time spent in the corresponding speed-VSP bins were then used to calculate the total trip emissions (or fuel consumption) and emission factors (or fuel economy) under specific average link speeds. The model approach was validated by comparing it against measured data with prediction errors within 20% for trip emissions and link-speed-based emission factors. This analysis is based on the data of light-duty gasoline vehicles in China; however, this research approach could be generalized to other vehicle fleets in other countries. This modeling method could also be coupled with traffic demand models to establish high-resolution emissions inventories and evaluate the impacts of traffic-related emission control measures.  相似文献   

3.
Ammonia emissions contribute to the formation of secondary particulate matter (PM) and violations of the National Ambient Air Quality Standard. Ammonia mass concentration measurements were made in February 1999 upwind and downwind of an open-lot dairy in California, using a combination of active bubbler and passive filter samplers. Ammonia fluxes were calculated from concentrations measured at 2, 4, and 10 m above ground at three locations on the downwind edge of the dairy, using micrometeorological techniques. A new method was developed to interpolate fluxes at six additional locations from ammonia concentrations measured at a single height, providing measurements at sufficient spatial resolution along the downwind border of the dairy to account for the heterogeneity of the source. PM measured up- and downwind of the dairy demonstrated insignificant ammonium particle formation in the immediate vicinity of the dairy and negligible contribution of dissociated ammonium nitrate to measured ammonia concentrations. Ammonium nitrate concentrations measured downwind of the dairy ranged from 26 to 0.26 microg m(-3) and from 2 to 43% of total PM2.5 mass concentrations. Measured ammonia fluxes showed that liquid manure retention ponds represented relatively minor sources of ammonia in winter on the dairy studied. Ammonia emission factors derived from the measurements ranged from 19 to 143 g head(-1) day(-1), showing an increase with warmer, drier weather and a decrease with increased relative humidity and lower temperatures.  相似文献   

4.
This paper characterizes the emission rates of size fractionated particulate matter, inorganic aerosols, acid gases, ammonia and methane measured over four flocks at a commercial broiler chicken facility. Mean emission rates of each pollutant, along with sampling notes, were reported in this paper, the first in a series of two. Sampling notes were needed because inherent gaps in data may bias the mean emission rates.The mean emission rates of PM10 and PM2.5 were 5.0 and 0.78 g day?1 [Animal Unit, AU]?1, respectively, while inorganic aerosols mean emission rates ranged from 0.15 to 0.46 g day?1 AU?1 depending on the season. The average total acid gas emission rate was 0.43 g day?1 AU?1 with the greatest contribution from nitrous and nitric acids and little contribution from sulfuric acid (as SO2).Ammonia emissions were seasonally dependent, with a mean emission rate of 66.0 g day?1 AU?1 in the cooler seasons and 94.5 g day?1 AU?1 during the warmer seasons. Methane emissions were relatively consistent with a mean emission rate of 208 g day?1 AU?1.The diurnal pattern in each pollutant’s emission rate was relatively consistent after normalizing the hourly emissions according to each daily mean emission rate. Over the duration of a production cycle, all the measured pollutants’ emissions increased proportionally to the total live mass of birds in the house, with the exception of ammonia.Interrelationships between pollutants provide evidence of mutually dependent release mechanisms, which suggests that it may be possible to fill data gaps with minimal data requirements. In the second paper (Roumeliotis, T.S., Dixon, B.J., Van Heyst, B.J. Characterization of gaseous pollutants and particulate matter emission rates from a commercial broiler operation part II: correlated emission rates. Atmospheric Environment, 2010.), regression correlations are developed to estimate daily mean emission rates for data gaps and, using the normalized hourly diurnal patterns from this paper, emission factors were generated for each pollutant.  相似文献   

5.
This paper describes a project that assessed the potential for mercury (Hg) release to air and water from soil amended with combustion products to simulate beneficial use. Combustion products (ash) derived from wood, sewage sludge, subbituminous coal, and a subbituminous coal-petroleum coke mixture were added to soil as agricultural supplements, soil stabilizers, and to develop low-permeability surfaces. Hg release was measured from the latter when intact and after it was broken up and mixed into the soil. Air-substrate Hg exchange was measured for all materials six times over 24 hr, providing data that reflected winter, spring, summer, and fall meteorological conditions. Dry deposition of atmospheric Hg and emission of Hg to the atmosphere were both found to be important fluxes. Measured differences in seasonal and diel (24 hr) fluxes demonstrated that to establish an annual estimate of air-substrate flux from these materials data on both of these time steps should be collected. Air-substrate exchange was highly correlated with soil and air temperature, as well as incident light. Hg releases to the atmosphere from coal and wood combustion product-amended soils to simulate an agricultural application were similar to that measured for the unamended soil, whereas releases to the air for the sludge-amended materials were higher. Hg released to soil solutions during the Synthetic Precipitation Leaching Procedure for ash-amended materials was higher than that released from soil alone. On the basis of estimates of annual releases of Hg to the air from the materials used, emissions from coal and wood ash-amended soil to simulate an agricultural application could simply be re-emission of Hg deposited by wet processes from the atmosphere; however, releases from sludge-amended materials and those generated to simulate soil stabilization and disturbed low-permeability pads include Hg indigenous to the material.  相似文献   

6.
Laboratory batch experiments were carried out to study the adsorption of arsenate on 16 Chinese soils with different physicochemical properties. Wide differences in arsenate adsorption were observed, and the Jiangxi and Hubei soils were more effective sorbents for arsenate than other soils. The Langmuir one-surface and two-surface equations were used to model the arsenate adsorption data. Except for the Jiangxi and Hubei soils, the Langmuir one-surface equation gave reasonably good fits to the arsenate adsorption data. However, the Langmuir two-surface equation generally provided a better fit than the Langmuir one-surface equation. For soils with relative high organic matter (OM), dissolved organic carbon (DOC) or extractable phosphate, the Langmuir one-surface and two-surface equations described the adsorption isotherms similarly. In contrast, for soils with relatively low contents of OM, DOC or extractable phosphate, the Langmuir two-surface equation gave the better fit to the arsenate adsorption data.  相似文献   

7.
Waste distribution and compaction at the working face of municipal waste landfills releases mercury vapor (Hg(o)) to the atmosphere, as does the flaring of landfill gas. Waste storage and processing before its addition to the landfill also has the potential to release Hg(o) to the air if it is initially present or formed by chemical reduction of Hg(II) to Hg(o) within collected waste. We measured the release of Hg vapor to the atmosphere during dumpster and transfer station activities and waste storage before landfilling at a municipal landfill operation in central Florida. We also quantified the potential contribution of specific Hg-bearing wastes, including mercury (Hg) thermometers and fluorescent bulbs, and searched for primary Hg sources in sorted wastes at three different landfills. Surprisingly large fluxes were estimated for Hg losses at transfer facilities (approximately 100 mg/hr) and from dumpsters in the field (approximately 30 mg/hr for 1000 dumpsters), suggesting that Hg emissions occurring before landfilling may constitute a significant fraction of the total emission from the disposal/landfill cycle and a need for more measurements on these sources. Reducing conditions of landfill burial were obviously not needed to generate strong Hg(o) signals, indicating that much of the Hg was already present in a metallic (Hg(o)) form. Attempts to identify specific Hg sources in excavated and sorted waste indicated few readily identifiable sources; because of effective mixing and diffusion of Hg(o), the entire waste mass acts as a source. Broken fluorescent bulbs and thermometers in dumpsters emitted Hg(o) at 10 to >100 microg/hr and continued to act as near constant sources for several days.  相似文献   

8.
A methodology for estimating vehicular emissions comprising a car simulator, a basic traffic model, and a geographical information system is capable of estimating vehicle emissions with high time and space resolution. Because of the extent of the work conducted, this article comprises two sections: In Part 1 of this work, we describe the system and its components and use examples for testing it. In Part 2 we will study in more detail the emissions of the sample fleet using the system and will make comparisons with another emission model. The experimental data for the car simulator is obtained using on-board measuring equipment and laboratory Fourier transform IR (FTIR) measurements with a dynamometer following typical driving cycles. The car simulator uses this data to generate emission factors every second. These emission factors, together with information on car activity and velocity profiles of highways and residential and arterial roads in Mexico City in conjunction with a basic traffic model, provide emissions per second of a sample fleet. A geographical information system is used to localize these road emissions.  相似文献   

9.
Emission rates of ammonia, acid gases, inorganic aerosols, methane, and size fractionated particulate matter were measured from a commercial broiler facility. This paper discusses the statistically influential parameters on numerous pollutants’ emission from a broiler chicken facility and generates emission correlations to fill data gaps and develop averaged emission factors.Live mass of the birds was commonly a significant variable to each pollutant’s emission. Some variables significantly impacted the pollutants’ emissions, such as litter moisture content, but were measured discretely and cannot be used for filling in data gaps.House parameter correlations were, therefore, developed using parameters measured at the facility, such as indoor temperature, relative humidity, and the live mass of the birds, and relied on the mutual behaviour of discretely measured explanatory parameters and continuously monitored confounding variables. The live mass and the difference in the indoor temperature and the house set-point temperature were the most significant variables in each pollutant’s correlation.The correlations predicted each pollutants emission to within 20% (total mass basis) over most broiler production cycles. Their validation on independent datasets also successfully estimated the flocks’ emissions to within 3%.Emission factors (EFs) were developed for methane, ammonia, and size fractionated particulate matter using measured data and correlated emissions to fill in data gaps. PM10 (particulate matter ≤10 microns) EFs were estimated to be 4.6 and 5.9 g d?1 [Animal Unit, AU]?1 for five and six week production cycles, respectively. PM2.5 (PM ≤ 2.5 microns) EFs were 0.8 and 1.4 g d?1 AU?1 for five and six week cycles, respectively. Ammonia and methane emission factors were estimated at 120.8 and 197.0 g d?1 AU?1, respectively for a five week production cycle.  相似文献   

10.
Methane emissions from a flock of 14, 1-year old sheep grazing on a grass and legume pasture were measured using a micrometeorological mass-balance method and a sulphur hexaflouride (SF6) tracer technique. The former measured the mean emission, over 45 min intervals, from all the sheep within a fenced 24 m×24 m enclosure, from the enrichment of methane (CH4) in air as it passed over the sheep. The tracer technique measured emissions from a subset of 7 individual animals over 24 h periods from measurements of CH4 and SF6 concentrations in air exhaled by the sheep, and from the known rate of release of SF6 from small permeation tubes placed in the animals’ rumens. Both methods gave highly similar results for 4 out of 5 days. When the species composition of dietary intake was steady during the last two days of measurement, the mean emission rate from the mass-balance method was 11.9±1.5 (SEM) g CH4 sheep-1 d-1, while the rate from the tracer technique was 11.7±0.4 (SEM) g CH4 sheep-1 d-1. These rates are for sheep with mean live mass of 27 kg, with a measured dry matter intake of 508 g sheep-1 d-1 and pasture dry matter digestibility of 69.5%. There was close agreement between these measurements and estimates from algorithms used to predict methane emissions from sheep for the Australian National Greenhouse Gas Inventory.  相似文献   

11.
Mercury-bearing material enters municipal landfills from a wide array of sources, including fluorescent lights, batteries, electrical switches, thermometers, and general waste; however, the fate of mercury (Hg) in landfills has not been widely studied. Using automated flux chambers and downwind atmospheric sampling, we quantified the primary pathways of Hg vapor releases to the atmosphere at six municipal landfill operations in Florida. These pathways included landfill gas (LFG) releases from active vent systems, passive emissions from landfill surface covers, and emissions from daily activities at each working face (WF). We spiked the WF at two sites with known Hg sources; these were readily detected downwind, and were used to test our emission modeling approaches. Gaseous elemental mercury (Hg(O)) was released to the atmosphere at readily detectable rates from all sources measured; rates ranged from approximately 1-10 ng m(-2) hr(-1) over aged landfill cover, from approximately 8-20 mg/hr from LFG flares (LFG included Hg(O) at microg/m3 concentrations), and from approximately 200-400 mg/hr at the WF. These fluxes exceed our earlier published estimates. Attempts to identify specific Hg sources in excavated and sorted waste indicated few readily identifiable sources; because of effective mixing and diffusion of Hg(O), the entire waste mass acts as a source. We estimate that atmospheric Hg releases from municipal landfill operations in the state of Florida are on the order of 10-50 kg/yr, substantially larger than our original estimates, but still a small fraction of current overall anthropogenic losses.  相似文献   

12.
This paper presents a sensitivity analysis of a microscale emission factor model (MicroFacCO) for predicting real-time site-specific motor vehicle CO emissions to input variables, as well as a limited field study evaluation of the model. The sensitivity analysis has shown that MicroFacCO emission estimates are very sensitive to vehicle fleet composition, speed, and ambient temperature. For the present U.S. traffic fleet, the CO emission rate (g/mi) is increased by more than 500% at 5 mph in comparison with a speed greater than 40 mph and by approximately 67% at ambient temperatures of 45 degrees F and > or = 95 degrees F in comparison with an ambient temperature of 75 degrees F. The input variable "emission failure standard rate" is more sensitive to estimating emission rates in the 1990s than in the 2000s. The estimation of emission rates is not very sensitive to relative humidity. MicroFacCO can also be applied to examine the contribution of emission rates per vehicle class and model year. The model evaluation is presented for tunnel studies at five locations. In general, this evaluation study found good agreement between the measured and the modeled emissions. These analyses and evaluations have identified the need for additional studies to update the high-speed (>35 mph) air conditioning (A/C) correction factor and to add effects due to road grades. MicroFacCO emission estimates are very sensitive to the emission standard failure rate. Therefore, the model performance can be greatly improved by using a local emission standard failure rate.  相似文献   

13.
A microscale emission factor model (MicroFacPM) for predicting real-time site-specific motor vehicle particulate matter emissions was presented in the companion paper titled "Development of a Microscale Emission Factor Model for Particulate Matter (MicroFacPM) for Predicting Real-Time Motor Vehicle Emissions". The emission rates discussed are in mass per unit distance with the model providing estimates of fine particulate matter (PM2.5) and coarse particulate matter. This paper complements the companion paper by presenting a sensitivity analysis of the model to input variables and evaluation model outputs using data from limited field studies. The sensitivity analysis has shown that MicroFacPM emission estimates are very sensitive to vehicle fleet composition, speed, and the percentage of high-emitting vehicles. The vehicle fleet composition can affect fleet emission rates from 8 mg/mi to 1215 mg/mi; an increase of 5% in the smoking (high-emitting) current average U.S. light-duty vehicle fleet (compared with 0%) increased PM2.5 emission rates by -272% for 2000; and for the current U.S. fleet, PM2.5 emission rates are reduced by a factor of -0.64 for speeds >50 miles per hour (mph) relative to a speed of 10 mph. MicroFacPM can also be applied to examine the contribution of emission rates per vehicle class, model year, and sources of PM. The model evaluation is presented for the Tuscarora Mountain Tunnel, Pennsylvania Turnpike, PA, and some limited evaluations at two locations: Sepulveda Tunnel, Los Angeles, CA, and Van Nuys Tunnel, Van Nuys, CA. In general, the performance of MicroFacPM has shown very encouraging results.  相似文献   

14.
This technical note describes a United States Environmental Protection Agency (U.S. EPA) measurement project to determine elemental mercury (Hg0) emissions from a mercury cell chlor-alkali (MCCA) facility in the southeastern U.S. during a 53-day monitoring campaign in the fall of 2006. The optical remote sensing (ORS) area source measurement method EPA OTM 10 was used to provide Hg0 flux data for the site. These results are reported and compared with cell room roof-vent monitoring data acquired by the facility for similar time periods. The 24-h extrapolated mercury emission rate estimates determined by the two monitoring approaches are shown to be similar with overall averages in the 400 g day?1 range with maximum values around 1200 g day?1. Results from the OTM 10 measurements, which include both cell room emissions and potential fugitive sources outside the cell room, are shown to be approximately 10% higher than cell room monitoring results indicating that fugitive emissions from outside the cell room produce a small but measurable effect for this site.  相似文献   

15.
GOAL, SCOPE AND BACKGROUND: Malodorous volatiles derived from the decomposition of biowaste within the process of composting might pose a risk to human health. Different techniques of process engineering have been developed to minimise the burden of malodorous compounds in air possibly affecting compost workers and residents in the vicinity. METHODS: In the present study, three different composting facilities were examined for the emission of volatiles to estimate the impact of process engineering on the dispersal of odorous compounds and to discuss its relevance for human health. RESULTS AND DISCUSSION: Concentrations of single compounds belonging to alcohols, ketones, furanes, sulfur-containing compounds and especially terpenes ranged from 10(2) up to nearly 10(6) ng/m3 depending on the sampling sites and the process engineering. The ratio of MVOC and total VOC measured changed throughout the process of biodegradation. A certain combination of volatile compounds coincided with the occurrence of typical compost odour. CONCLUSION: The type of process engineering seemed to have a major impact on the emission of volatiles, as amounts of (microbial) volatiles emitted were characteristic for the different techniques used. Thus, the MVOC emission basically depends on the degree of biodegradation. It is likely that the concentrations workers are exposed to can have an impact on human health. RECOMMENDATIONS AND OUTLOOK: It is obvious that less sophisticated types of process engineering give rise to greater amounts of bioaerosols and volatiles and, therefore, technical devices have to be improved and controlled regularly to minimise adverse health effects on workers.  相似文献   

16.
Aguilar L  Thibodeaux LJ 《Chemosphere》2005,58(10):1309-1318
Temporary water reservoirs built upon peat soil may exhibit water quality impairment from elevated dissolved organic carbon (DOC). Microbiological decay of the organic carbon in the bed with subsequent release produces "tea" colored water which may require treatment prior to use. This paper describes laboratory experiments designed to obtain data on the release process of DOC from soils containing 0.65%, 10% and 19% carbon. Parallel experiments with and without sodium azide treatment clearly distinguished the initial release of a porewater residual fraction and the microbial produced fraction. A one to two day quick-release DOC fraction, which ranges from 28% to 50%, first emerged from the bed, Step-1. This was followed by a constant rate of DOC production over four weeks, Step-2. The Step-2 average production rates were 3.4, 12, and 31 mg DOC/kg(dry)/day for the respective soils and increased as soil carbon content increased. The inorganic carbon (IC) behaved oppositely; its rate of production decreased with increasing soil carbon. A consistent and simple rate equation described the Step-2 DOC production process. This and other evidence obtained provided the basis for developing a mathematical model that couples both steps of the bed-to-water DOC release chemodynamics. The model is presented in a companion paper (Part-2).  相似文献   

17.
This paper describes the development of a detailed dry deposition model for routine computation of dry deposition velocities of SO2, O3, HNO3 and fine particle SO42− across much of North America. Four different dry deposition/surface exchange sub-models have been combined with the current Canadian weather forecast model (Global Environmental Multiscale model) with a 3 h time resolution and a horizontal spatial resolution of 35 km. The present model uses the US Geological Survey North American Land Cover Characteristics data to obtain fourteen different land use and five seasonal categories. The four sub-models used are a multi-layer model for gaseous species over taller canopy land-use types, a big-leaf model for gaseous species over lower canopies (including bare soil and water) and for HNO3 under all surface types and, two different models for SO42−, one for tall canopies and the other for short canopies. All necessary parameters for each sub-model, chemical species, land-use and seasonal categories have been selected from available data libraries or from the values reported in the literature. The purpose for developing this model (referred to as the Routine Deposition Model (RDM)), when coupled with air concentration data, is to provide estimates of seasonal dry deposition, which can be combined with wet deposition to produce total deposition estimates. Model theory is discussed in this paper and model sensitivity tests and results will be presented in a companion paper.  相似文献   

18.
The objectives of this study were to assess the potential for using Thlaspi caerulescens as a phytoextraction plant and develop a user-advice model, which can predict the frequency of phytoextraction operation required under prescribed conditions. Pot and field trials were conducted using soil collected from a dedicated sewage sludge disposal facility. Soil amendments (sulphuric acid, potassium chloride and EDTA) intended to increase Cd solubility were also tested. Predictive models of Cd and Zn uptake were developed which were able to reproduce the observed pH-dependence of Cd uptake with an apparent maximum around pH 6. Chemical treatments did not significantly increase the uptake of Cd. The periodic use of phytoextraction with T. caerulescens to maintain soils below statutory metal concentration limits, when modern sewage sludges are repeatedly applied, seems very attractive given the non-intrusive and cost-effective nature of the process. The major limitations lie with the large-scale husbandry of T. caerulescens.  相似文献   

19.
The process of electrochemical treatment of a solution after strong basic anion exchanger regeneration was studied. The goal of the study was to reduce the nitrate content in the solution to allow its use in a closed loop. Diaphragmless, flow-through cells in a recirculation mode with and without a fluidizing bed of inert particles in the interelectrode space equipped with copper (Cu) cathodes and activated titanium anodes were used. The temperature was maintained at 20 degrees C. To assess the influence of recirculation of the regenerant solution on the quality of the treated water, the effect of the addition of copper ions to the solution, postelectrolysis cathode treatment, and enhanced mass transfer on the electrolysis results with respect to current efficiency and residual nitrate and nitrite concentration were investigated using an artificial solution. On the basis of the experimental results, a laboratory-scale unit for selective nitrate removal was designed and constructed that integrated ion exchange and electrochemical cell to one assembly. The process of recirculation of regenerant solution was tested using groundwater.  相似文献   

20.
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   

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