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1.
Dust particles affect the budgets of important traces gases by providing a surface on which heterogeneous reactions can occur. The uptake of soluble species on dust alters the physical, chemical, and optical properties and the overall ability of dust to act as cloud condensation and ice nuclei. It is commonly assumed that all measured chloride in particulate filter samples is associated with sea-salt particles and any chloride in dust occurs as the result of internal mixtures of sea-salt and dust particles, formed by cloud processing. Here we show high temporal resolution data demonstrating the direct uptake of chlorine by dust via heterogeneous reaction with HCl(g). This reaction added significant amounts of chlorine to the dust particles during a major dust storm, representing 4–9% of the individual dust particle mass. Up to 65±4% of the dust particles contained chlorine due to this heterogeneous reaction during the dust front. Ignoring this process leads to an overestimation of sea-salt concentrations from bulk measurements, and an underestimation of the degree of sea-salt aging. The uptake of chloride will change the pH and hygroscopic properties of the dust and thus can influence the budgets of other reactive gases. Including this heterogeneous process in atmospheric measurements and chemical transport models will improve our ability to predict the atmosphere's composition and radiation budget with greater accuracy.  相似文献   

2.
For a number of phthalates and especially for di(2-ethylhexyl)phthalate (DEHP), surprisingly high house dust concentrations are reported in the literature. Therefore, the uptake of the most prominent compounds DEHP and di-n-butylphthalate (DnBP) from plasticized indoor materials into house dust samples of different organic content has been experimentally determined. The experiments have been performed within 45 days which is sufficient for the more volatile phthalate (DnBP) to reach equilibrium conditions. DnBP reaches considerably higher concentrations in the chamber air compared to real room measurements and, thus, also elevated dust concentrations. In contrast, the mass transfer of DEHP in the dust via the gas phase was significantly lower. However, small chamber experiments showed elevated mass transfer of DEHP in case of direct contact between emission source and sink. This aspect is experimentally determined using an plasticized PVC polymer with and without direct contact to house dust. A transfer into the dust could be observed in dependence of the initial concentration in the material. However, the results do not allow the differentiation between the two uptake mechanisms via capillary forces and contact to the material’s boundary layer. The results illustrate that the reasons for elevated DEHP concentrations in dust indoors can be traced back to direct contact of source and sink, abrasion from the source, and transport via airborne particles.  相似文献   

3.
4.

A comprehensive approach has been developed to the assessment of composition and properties of atmospherically deposited dust in the area affected by a copper smelter. The approach is based on the analysis of initial dust samples, dynamic leaching of water soluble fractions in a rotating coiled column (RCC) followed by the determination of recovered elements and characterization of size, morphology and elemental composition of nano-, submicron, and micron par ticles of dust separated using field-flow fractionation in a RCC. Three separated size fractions of dust (<0.2, 0.2–2, and >2 μm) were characterized by static light scattering and scanning electron microscopy, whereupon the fractions were analyzed by ICP-AES and ICP-MS (after digestion). It has been evaluated that toxic elements, which are characteristics for copper smelter emissions (As, Cu, Zn), are accumulated in fraction >2 μm. At the same time, up to 2.4, 3.1, 8.2, 6.7 g/kg of As, Cu, Zn, Pb, correspondently, were found in nanoparticles (<0.2 μm). It has been also shown that some trace elements (Sn, Sb, Ag, Bi, and Tl) are accumulated in fraction <0.2, and their content in this fraction may be one order of magnitude higher than that in the fraction >2 μm, or the bulk sample. It may be assumed that Sn, Sb, Ag, Bi, Tl compounds are adsorbed onto the finest dust particles as compared to As, Cu, Zn compounds, which are directly emitted from the copper smelter as microparticles.

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5.
This study presents and develops a controlled and characterized method to explore the influence of specific occupant activity on the aerosolization of allergen-containing particles. Indoor allergen-related diseases are primarily inhalation sensitized and developed, suggesting an aerobiological pathway of allergen-containing carrier particles from dust reservoir to occupant respiration. But the pathways are not well understood or quantified. The influence of occupant walking on particle aerosolization is simulated by a system in which complex floor disturbances are deconvoluted into aerodynamic and mechanical components. Time resolved particle size distributions are measured for particles resuspended from representative samples of flooring materials and different types of floor disturbances in an environmentally controlled experimental chamber. Results indicate aerodynamic disturbances, relative to mechanical, dominate the particle resuspension behavior. Dust type, dust load and floor type showed marginal influences on a normalized surface loading basis. Humidity effects were not clear since during experiments the floor samples may not have reached moisture partitioning equilibrium with the controlled air humidity. Average resuspension rates ranged from 10−7 to 10−3 min−1, having phenomenological consistency with previous, large room or chamber investigations, suggesting the method can be utilized to develop a database for particle resuspension rates.  相似文献   

6.
Road dust contributes a large percentage of the atmosphere's suspended particles in Taiwan. Three road dust samples were collected from downtown, electrical park, and freeway tunnel areas. A mechanical sieve separated the road dust in the initial stage. Particles > 100 microm were 75%, 70%, and 60% (wt/wt), respectively, of the samples. Those particles < 37 microm were resuspended in another mixing chamber and then collected by a Moudi particle sampler. The largest mass fraction of resuspended road dust was in the range of 1-10 microm. Ultrafine particles (< 1 microm) composed 33.7, 17, and 7.4% of the particle samples (downtown, electrical park, and freeway tunnel, respectively). The road dust compositions were analyzed by inductively coupled plasma (ICP)-atomic emissions spectroscopy and ICP-mass spectrometry. The highest concentration fraction contained more aluminum (Al), iron (Fe), calcium (Ca), and potassium than other elements in the road dust particle samples. Additionally, the sulfur (S) content in the road dust from the electrical park and freeway tunnel areas was 2.1 and 3.4 times the downtown area sample, respectively. The sulfur originated from the vehicle and boiler oil combustion and industrial manufacturing processes. Furthermore, zinc (Zn) concentration in the tunnel dust was 2.6 times that of the downtown and electrical park samples, which can be attributed to vehicle tire wear and tear. Resuspended road dusts (< 10 microm) from the downtown and freeway tunnel areas were principally 2.5-10 microm Al, barium (Ba), Ca, copper (Cu), Fe, magnesium (Mg), sodium (Na), antimony (Sb), and Zn, whereas arsenic (As), chromium (Cr), and nickel (Ni) were predominant in the ultrafine particle samples (< 1 microm). Al, Ba, and Ca are the typical soil elements in coarse particles; and As, and Cr and Ni are the typical fingerprint of oil combustion and vehicle engine abrasion in ultrafine particles. There was a special characteristic of resuspension road dust at electrical park, that is, many elements, including As, Ba, Ca, cadmium, Cr, Cu, Fe, manganese (Mn), Ni, lead (Pb), S, vanadium (V), and Zn, were major in ultrafine particles. These elements should be attributed to the special manufacturing processes of electric products.  相似文献   

7.
This is an experimental study on the characterization of particulate (soot) emissions from burning polymers. Emissions of polystyrene (PS), polyethylene (PE), polypropylene (PP), polymethyl methacrylate (PMMA), and polyvinyl chloride (PVC) plastics were studied. Combustion took place in a laboratory-scale, electrically heated, drop-tube furnace at temperatures of 1300 and 1500 K, in air. The nominal bulk (global) equivalence ratio, phi, was varied in the range of 0.5-1.5, and the gas residence time in the nearly isothermal radiation zone of the furnace was approximately 1 sec. The particulate emissions were size-classified at the exit of the furnace, using a multi-stage inertial particle impactor. Results showed that both the yields and the size distributions of the emitted soot were remarkably different for the five plastics burned. Soot yields increased with an increasing bulk equivalence ratio. Combustion of PS yielded the highest amounts of soot (most highly agglomerated), several times more than the rest of the polymers. More soot was emitted from PS at 1500 than at 1300 K. Substantial amounts of soot agglomerates were larger than 9 microns. At 1500 and 1300 K, 35 and 29% of the soot mass, respectively, was PM2 (2 microns or smaller). Emissions from PE and PP were remarkably similar to each other. These polymers produced very low emissions at phi < or = 0.5, but emissions increased drastically with phi, and most of the soot was very fine (70-97% of the mass was PM2, depending on phi). Emissions from the combustion of PMMA were comparatively low and were the least influenced by the bulk phi, and 79-95% of the emissions were PM2. Combustion of PVC yielded the lowest amounts of soot; moreover, only 13-34% of the mass was PM2. On a comparative basis, at 1500 K, the following ranges of particulate yields were PM2: 19-75 mg/g of PS, 8-36 mg/g of PE, 1.5-47 mg/g of PP, 11-20 mg/g of PMMA, and 2-8 mg/g of PVC, depending on phi. These comparative results demonstrate that PS produces the highest amounts of fine particulates, followed by PP, PE, and PMMA, and then PVC. Burning these materials with excess oxygen drastically reduces the particulate emissions of PE and PP, substantially reduces those of PS, and mildly reduces those of PMMA and PVC.  相似文献   

8.
A novel process for degradation of toluene in the gas-phase using heterogeneous gas-liquid photocatalytic oxidation has been developed. The degradation of toluene gas by photo-Fenton reaction in the liquid-phase has experimentally examined. The photo-Fenton reaction in the liquid-phase could improve the overall toluene absorption rate by increasing the driving force for mass transfer and as a result enhance the removal of toluene in the exhaust gas. The toluene concentrations in the inlet gas were varied in the range from 0.0968 to 8.69gm(-3) with initial hydrogen peroxide concentration of 400mgl(-1) and Fe dose of 5.0mgl(-1). It was found that toluene in the inlet gas was almost completely dissolved into water and degraded in the liquid-phase for the inlet toluene gas concentration of less than 0.42gm(-3). The dynamic process of toluene gas degradation by the photo-Fenton reaction providing information for reaction kinetics and mass transfer rate was examined. Toluene removal kinetic analysis indicated that photo-Fenton degradation was significantly affected by H(2)O(2) concentration. The experimental results were satisfactorily described by the predictions simulated using the simplified tanks-in-series model combined with toluene removal kinetic analysis. The present results showed that the proposed chemical absorption process using the photo-Fenton heterogeneous gas-liquid photocatalytic oxidation is very effective for degradation of volatile organic gases.  相似文献   

9.
The body of information presented in this paper is directed to those individuals concerned with the catalytic NOx removal reactor for a dirty (containing dust) flue gas. In the case of treating a dirty flue gas, the concentration of dust is the most important factor. While the dirty gas passes through the catalytic reactor, dust particles deposit and plug up the catalyst causing the reactor pressure loss to rise. As a result, the NOx reduction efficiency decreases more and more, and continuous operation becomes impossible. A new type of NOx removal reactor for dirty flue gas, the intermittent moving bed reactor, has been developed. The following characteristics have been evaluated: (1) method of calculating reactor pressure loss caused by dust particles, (2) static pressure distribution across the catalyst bed in the reactor, (3) method of evaluating uniform movement of catalyst and (4) reentrainment pattern of dust by catalyst movement. After carrying out various successful pilot plant tests, the information needed for construction and operation of a commercial plant has been developed.  相似文献   

10.
Abstract

Road dust contributes a large percentage of the atmosphere’s suspended particles in Taiwan. Three road dust samples were collected from downtown, electrical park, and freeway tunnel areas. A mechanical sieve separated the road dust in the initial stage. Particles >100 μm were 75%, 70%, and 60% (wt/wt), respectively, of the samples. Those particles <37 μm were resuspended in another mixing chamber and then collected by a Moudi particle sampler. The largest mass fraction of resuspended road dust was in the range of 1–10 μm. Ultrafine particles (<1 μm) composed 33.7, 17, and 7.4% of the particle samples (downtown, electrical park, and freeway tunnel, respectively). The road dust compositions were analyzed by inductively coupled plasma (ICP)-atomic emissions spectroscopy and ICP-mass spectrometry. The highest concentration fraction contained more aluminum (Al), iron (Fe), calcium (Ca), and potassium than other elements in the road dust particle samples. Additionally, the sulfur (S) content in the road dust from the electrical park and freeway tunnel areas was 2.1 and 3.4 times the downtown area sample, respectively. The sulfur originated from the vehicle and boiler oil combustion and industrial manufacturing processes. Furthermore, zinc (Zn) concentration in the tunnel dust was 2.6 times that of the downtown and electrical park samples, which can be attributed to vehicle tire wear and tear. Resuspended road dusts (<10 μm) from the downtown and freeway tunnel areas were principally 2.5–10 μm Al, barium (Ba), Ca, copper (Cu), Fe, magnesium (Mg), sodium (Na), antimony (Sb), and Zn, whereas arsenic (As), chromium (Cr), and nickel (Ni) were predominant in the ultrafine particle samples (<1 μm). Al, Ba, and Ca are the typical soil elements in coarse particles; and As, and Cr and Ni are the typical fingerprint of oil combustion and vehicle engine abrasion in ultrafine particles. There was a special characteristic of resuspension road dust at electrical park, that is, many elements, including As, Ba, Ca, cadmium, Cr, Cu, Fe, manganese (Mn), Ni, lead (Pb), S, vanadium (V), and Zn, were major in ultrafine particles. These elements should be attributed to the special manufacturing processes of electric products.  相似文献   

11.
烟气和粉尘性质对除尘效率影响的仿真研究   总被引:1,自引:0,他引:1  
应用欧拉-拉格朗日多相流模型对影响电除尘器内部气流分布的烟气含尘浓度、烟气湿度、粉尘粒径及真密度等因素进行了数值仿真。分析了烟气和粉尘性质对除尘效率的影响。由于在仿真过程中考虑了烟气特性和粉尘性质等因素,不仅可获得各因素对气流分布均匀性的影响,而且仿真结果更能反映电除尘器气流分布的实际情况。提出的烟气和粉尘性质仿真方法可以为电除尘器除尘效率分析提供新的途径。  相似文献   

12.
Aerosol particles were collected for 1 year, starting in April 2003, in rural areas of Kanazawa, Ishikawa, Japan to understand the role of Asian dust as a long-range transporter of polycyclic aromatic hydrocarbons (PAHs). Three sampling intervals were designated in this study, namely: (1) Dust period 1 (March 11–19, 2003); (2) Dust period 2 (March 28, 2003–April 9, 2003); and (3) Dust period 3 (April 9, 2004–April 25, 2004). The Asian dust particles are predominantly in the coarse particle size range (2.1–11 μm). PAH analyses were performed separately on both the coarse and fine (<1.1 μm) particle ranges. Seasonal trends in PAH concentrations for coarse and fine particles showed that the Asian dust particles in Dust period 3 contained significant amounts of less-volatile PAHs such as benzo[a]pyrene (BaP) and benzo[g,h,i]perylene (BghiP). A kinetic model developed in this study shows that almost none of these PAHs would be accumulated on Asian dust particles in the atmosphere, due to their extremely slow adsorption rates. These PAHs would have to originate from PAH-polluted soil particles around industrialized areas. Back trajectory analyses suggest that the Asian dust in Dust period 3 came from loess regions around industrialized areas. This indicates that geologic materials play a significant role in the atmospheric circulation of PAHs.  相似文献   

13.
The mass transfer rate of pure ammonium nitrate between the aerosol and gas phases was quantified experimentally by the use of the tandem differential mobility analyzer/scanning mobility particle sizer (TDMA/SMPS) technique. Ammonium nitrate particles 80–220 nm in diameter evaporated in purified air in a laminar flow reactor under temperatures of 20–27°C and relative humidities in the vicinity of 10%. The evaporation rates were calculated by comparing the initial and final size distributions. A theoretical expression of the evaporation rate incorporating the Kelvin effect and the effect of relative humidity on the equilibrium constant is developed. The measurements were consistent with the theoretical predictions but there was evidence of a small kinetic resistance to the mass transfer rate. The discrepancy can be explained by a mass accommodation coefficient ranging from 0.8 to 0.5 as temperature increases from 20–27°C. The corresponding timescale of evaporation for submicron NH4NO3 particles in the atmosphere is of the order of a few seconds to 20 min.  相似文献   

14.
The humic colloid borne Am(III) transport was investigated in column experiments for Gorleben groundwater/sand systems. It was found that the interaction of Am with humic colloids is kinetically controlled, which strongly influences the migration behavior of Am(III). These kinetic effects have to be taken into account for transport/speciation modeling. The kinetically controlled availability model (KICAM) was developed to describe actinide sorption and transport in laboratory batch and column experiments. Application of the KICAM requires a chemical transport/speciation code, which simultaneously models both kinetically controlled processes and equilibrium reactions. Therefore, the code K1D was developed as a flexible research code that allows the inclusion of kinetic data in addition to transport features and chemical equilibrium. This paper presents the verification of K1D and its application to model column experiments investigating unimpeded humic colloid borne Am migration. Parmeters for reactive transport simulations were determined for a Gorleben groundwater system of high humic colloid concentration (GoHy 2227). A single set of parameters was used to model a series of column experiments. Model results correspond well to experimental data for the unretarded humic borne Am breakthrough.  相似文献   

15.
磺胺类抗生素的活性炭吸附过程研究   总被引:2,自引:1,他引:1  
采用煤质活性炭对3种磺胺类抗生素(浓度在1~2 mg/L之间)的吸附处理过程做了深入研究。结果表明,3种磺胺类抗生素在2~3 h之内可以达到吸附平衡;准一级动力学对其吸附动力学的模拟结果良好,且SMZ、SM1和SM2的一级吸附动力学常数k1分别为0.029、0.024和0.017 min-1,3种抗生素的平衡吸附容量分别为3.75、3.23和2.95 mg/g,SMZ的平衡吸附容量最大,最先达到吸附平衡,且平衡浓度也最低。3种磺胺类抗生素的吸附过程中,吸附前期的阻力主要是内扩散,而吸附后期较低浓度的抗生素吸附过程的阻力主要来自于膜扩散;采用Freundlich等温线方程描述3种磺胺类抗生素的吸附过程更为合理。  相似文献   

16.
Semivolatile organic compounds (SVOCs) are a major class of indoor pollutants. Understanding SVOC partitioning between the gas phase and settled dust is important for characterizing the fate of these species indoors and the pathways by which humans are exposed to them. Such knowledge also helps in crafting measurement programs for epidemiological studies designed to probe potential associations between exposure to these compounds and adverse health effects. In this paper, we analyze published data from nineteen studies that cumulatively report measurements of dustborne and airborne SVOCs in more than a thousand buildings, mostly residences, in seven countries. In aggregate, measured median data are reported in these studies for 66 different SVOCs whose octanol-air partition coefficients (Koa) span more than five orders of magnitude. We use these data to test a simple equilibrium model for estimating the partitioning of an SVOC between the gas phase and settled dust indoors. The results demonstrate, in central tendency, that a compound’s octanol-air partition coefficient is a strong predictor of its abundance in settled dust relative to its gas phase concentration. Using median measured results for each SVOC in each study, dustborne mass fractions predicted using Koa and gas-phase concentrations correlate reasonably well with measured dustborne mass fractions (R2 = 0.76). Combined with theoretical understanding of SVOC partitioning kinetics, the empirical evidence also suggests that for SVOCs with high Koa values, the mass fraction in settled dust may not have sufficient time to equilibrate with the gas phase concentration.  相似文献   

17.
Suspended atmospheric particles were collected in Israel in order to identify their nature and relationships with the major synoptic-scale circulation patterns. The particles were analyzed for their major and trace element concentrations and mineralogical composition. Samples were collected during three synoptic systems associated with desert dust storms: Red Sea trough, Sharav cyclone and cold depression, and during deep and shallow modes of Persian Gulf trough, which prevails in the summer months and is not associated with dust storms.All samples mostly contain particles smaller than 2 μm. The suspended desert dust is composed primarily of illite–smectite and calcite. Some indicative secondary minerals were found for each of the dust transporting synoptic systems (e.g., palygorskite for Red Sea trough). The bulk chemistry data support the mineralogical observations and reveal additional chemical signatures of each dust transporting system. For instance, Red Sea trough samples have significantly higher Ca/Al and Ca/Mg in the carbonate and Mg/Al in Al-silicate fraction than cold depression samples. Nevertheless, Sharav cyclone samples have intermediate values in spite of the fact that the source of the dust during these conditions is similar to cold depression (i.e., North Africa). Even though differences in the chemical and the mineralogical composition of desert dust do exist, this study reveals their overall chemical and mineralogical similarities.In contrast to the synoptic systems that carry desert dust, the inorganic fraction of the Persian Gulf trough samples contains significant amount (up to 50%) of non-mineral material that has a pronounced chemical signature in terms of major element concentrations (e.g., Al, Ca, Mg, Na, S) implying their anthropogenic nature, probably from countries around the Black Sea. This striking finding is indicative for atmospheric pollution in the Eastern Mediterranean region during the summer.  相似文献   

18.
A three dimensional chemical transport model (PMCAMx) is applied to the Mexico City Metropolitan Area (MCMA) in order to simulate the chemical composition and mass of the major PM1 (fine) and PM1–10 (coarse) inorganic components and determine the effect of mineral dust on their formation. The aerosol thermodynamic model ISORROPIA-II is used to explicitly simulate the effect of Ca, Mg, and K from dust on semi-volatile partitioning and water uptake. The hybrid approach is applied to simulate the inorganic components, assuming that the smallest particles are in thermodynamic equilibrium, while describing the mass transfer to and from the larger ones. The official MCMA 2004 emissions inventory with improved dust and NaCl emissions is used. The comparison between the model predictions and measurements during a week of April of 2003 at Centro Nacional de Investigacion y Capacitacion Ambiental (CENICA) “Supersite” shows that the model reproduces reasonably well the fine mode composition and its diurnal variation. Sulfate predicted levels are relatively uniform in the area (approximately 3 μg m?3), while ammonium nitrate peaks in Mexico City (approximately 7 μg m?3) and its concentration rapidly decreases due to dilution and evaporation away from the urban area. In areas of high dust concentrations, the associated alkalinity is predicted to increase the concentration of nitrate, chloride and ammonium in the coarse mode by up to 2 μg m?3 (a factor of 10), 0.4 μg m?3, and 0.6 μg m?3 (75%), respectively. The predicted ammonium nitrate levels inside Mexico City for this period are sensitive to the physical state (solid versus liquid) of the particles during periods with RH less than 50%.  相似文献   

19.
An activated carbon bed adsorption process is influenced by the adsorbents' characteristics, volatile organic compound (VOC) characteristics, and process conditions. In the literatures, the adsorption processes of the adsorbents and VOCs were usually considered to be in equilibrium. In this study, the VOC adsorption processes by activated carbon were considered to be a kinetic process, i.e. they are not in equilibrium. Then, isothermal adsorption curves and a small column experiment were simulated.  相似文献   

20.
Atmospheric dust deposition is a major external iron source for remote surface ocean waters. Organic complexation is known to play a role in the dissolution of iron-containing minerals. In this paper, we present our study on the effect of oxalate on dust iron solubility in simulated rainwater. Our results reveal that the solubility of iron carried by analogs of different African dusts varies with the dust source. Our experiments indicate a positive linear correlation between iron solubility and oxalate concentration. Soluble iron (SFe) increases from 0.0025(±0.0005)% to 0.26(±0.01)% of total iron, considering all dust sources and with oxalate concentrations ranging from 0 to 8 μM. These results show that the observed variability of iron solubility in aerosols collected over the Atlantic Ocean is, at least partly, due to an increase in dust iron solubility, with the presence of oxalate complexation, rather than to the presence of more soluble anthropogenic iron. Considering the mineralogical composition of those particles, experiments with pure minerals (hematite, goethite and illite) were performed to study the dissolution process. We found that oxalate promotes the solubility of iron contained in clay and hence confirmed that more than 95% of SFe from soil dust is provided by clay (illite). This experimental work enables us to establish a parameterization of iron solubility in dust as a function of oxalate concentration and based on the individual iron solubility of pure iron-bearing minerals usually present in dust particles. Finally, our results emphasize that oxalate contributes to iron solubility on the same order of magnitude as the acid processes. Organic complexation appears to be a process that increases iron solubility and likely enhances the bioavailability of iron from dust.  相似文献   

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