Formation of fine particles enriched by V and Ni from heavy oil combustion: Anthropogenic sources and drop-tube furnace experiments

The present study attempts to investigate the emission characteristics of fine particles with special emphasis on nickel and vanadium metal elements emitted from the heavy oil combustion in industrial boilers and power plant, which are typical anthropogenic sources in Korea. A series of combustion experiments were performed to investigate the emission characteristics of particles in the size range of submicron by means of drop-tube furnace with three major domestic heavy oils. Cascade impactors were utilized to determine the size distribution of particulates as well as to analyze the partitioning enrichment of vanadium and nickel in various size ranges. Experimental results were compared with field data of particle size distribution and metal partitioning at commercial utility boilers with heavy oil combustion. Such data were interpreted by chemical equilibrium and particle growth mechanism by means of computational models. In general, fine particles were the major portion of PM₁₀ emitted from the heavy oil combustion, with significant fraction of ultra-fine particles. The formation of ultra-fine particles through nucleation/condensation/coagulation from heavy oil combustion was confirmed by field and experimental data. Vanadium and nickel were more enriched in fine particles, particularly in ultra-fine particles. The conventional air pollution devices showed inefficient capability to remove ultra-fine particles enriched with hazardous transition metal elements such as vanadium and nickel.     

Source identification of nickel in TSP and PM2.5 in Tokyo,Japan

This study investigates the source identification of nickel in the aerosol of the Tokyo metropolitan area. TSP and PM_2.5 samples were collected daily from August to November 2004. The samples were examined by means of the water-extraction method, followed by elemental analysis and SEM/EDX analysis. We distinguished two types of atmospheric nickel sources in the studied area: (1) particles derived from heavy oil combustion, distributed mostly in fine particles such as PM_2.5, relatively water-soluble, and containing vanadium and (2) particles derived from mechanical abrasion/erosion of metallic surfaces, distributed in coarse particles such as TSP, relatively water-insoluble, and containing chromium.     

Comparison of particle size distributions and elemental partitioning from the combustion of pulverized coal and residual fuel oil

U.S. Environmental Protection Agency (EPA) research examining the characteristics of primary PM generated by the combustion of fossil fuels is being conducted in efforts to help determine mechanisms controlling associated adverse health effects. Transition metals are of particular interest, due to the results of studies that have shown cardiopulmonary damage associated with exposure to these elements and their presence in coal and residual fuel oils. Further, elemental speciation may influence this toxicity, as some species are significantly more water-soluble, and potentially more bio-available, than others. This paper presents results of experimental efforts in which three coals and a residual fuel oil were combusted in three different systems simulating process and utility boilers. Particle size distributions (PSDs) were determined using atmospheric and low-pressure impaction as well as electrical mobility, time-of-flight, and light-scattering techniques. Size-classified PM samples from this study are also being utilized by colleagues for animal instillation experiments. Experimental results on the mass and compositions of particles between 0.03 and > 20 microns in aerodynamic diameter show that PM from the combustion of these fuels produces distinctive bimodal and trimodal PSDs, with a fine mode dominated by vaporization, nucleation, and growth processes. Depending on the fuel and combustion equipment, the coarse mode is composed primarily of unburned carbon char and associated inherent trace elements (fuel oil) and fragments of inorganic (largely calcium-alumino-silicate) fly ash including trace elements (coal). The three coals also produced a central mode between 0.8- and 2.0-micron aerodynamic diameter. However, the origins of these particles are less clear because vapor-to-particle growth processes are unlikely to produce particles this large. Possible mechanisms include the liberation of micron-scale mineral inclusions during char fragmentation and burnout and indicates that refractory transition metals can contribute to PM < 2.5 microns without passing through a vapor phase. When burned most efficiently, the residual fuel oil produces a PSD composed almost exclusively of an ultrafine mode (approximately 0.1 micron). The transition metals associated with these emissions are composed of water-soluble metal sulfates. In contrast, the transition metals associated with coal combustion are not significantly enriched in PM < 2.5 microns and are significantly less soluble, likely because of their association with the mineral constituents. These results may have implications regarding health effects associated with exposure to these particles.     

Comparison of Particle Size Distributions and Elemental Partitioning from the Combustion of Pulverized Coal and Residual Fuel Oil

ABSTRACT

U.S. Environmental Protection Agency (EPA) research examining the characteristics of primary PM generated by the combustion of fossil fuels is being conducted in efforts to help determine mechanisms controlling associated adverse health effects. Transition metals are of particular interest, due to the results of studies that have shown cardiopulmonary damage associated with exposure to these elements and their presence in coal and residual fuel oils. Further, elemental speciation may influence this toxicity, as some species are significantly more water-soluble, and potentially more bio-available, than others. This paper presents results of experimental efforts in which three coals and a residual fuel oil were combusted in three different systems simulating process and utility boilers. Particle size distributions (PSDs) were determined using atmospheric and low-pressure impac-tion as well as electrical mobility, time-of-flight, and light-scattering techniques. Size-classified PM samples from this study are also being utilized by colleagues for animal instillation experiments.

Experimental results on the mass and compositions of particles between 0.03 and >20 μm in aerodynamic diameter show that PM from the combustion of these fuels produces distinctive bimodal and trimodal PSDs, with a fine mode dominated by vaporization, nucleation, and growth processes. Depending on the fuel and combustion equipment, the coarse mode is composed primarily of unburned carbon char and associated inherent trace elements (fuel oil) and fragments of inorganic (largely calcium-alumino-silicate) fly ash including trace elements (coal). The three coals also produced a central mode between 0.8- and 2.0-μm aerodynamic diameter. However, the origins of these particles are less clear because vapor-to-particle growth processes are unlikely to produce particles this large.

Possible mechanisms include the liberation of micron-scale mineral inclusions during char fragmentation and burnout and indicates that refractory transition metals can contribute to PM <2.5 μm without passing through a vapor phase. When burned most efficiently, the residual fuel oil produces a PSD composed almost exclusively of an ultrafine mode (~0.1 μm). The transition metals associated with these emissions are composed of water-soluble metal sulfates. In contrast, the transition metals associated with coal combustion are not significantly enriched in PM <2.5 μm and are significantly less soluble, likely because of their association with the mineral constituents. These results may have implications regarding health effects associated with exposure to these particles.     

Determination of cadmium, zinc, copper, chromium and arsenic in crude oil cargoes

One of the sources of trace heavy metal elements in air is emission by the oil industry, either directly through stack emissions from refineries or indirectly from emissions of combustion of hydrocarbons. Emission estimates are based mainly on the trace metal content of the crude oil processed. From a literature study carried out at the beginning of the 1990s it became clear that data on the trace metal content of crudes were scarce and showed a very large scatter. For this reason a measurement programme to assess the occurrence and concentrations of a number of trace metals, i.e. Cadmium (Cd), Zinc (Zn), Copper (Cu), Chromium (Cr), and arsenic (As), in crudes which are regularly processed in the Netherlands, was set up. By drafting strict sampling protocols and by constructing a special sampling device, as many as possible of the additional contamination sources were avoided. The study suggests that sample contamination may explain a significant amount of the scatter and some of the high concentrations reported in the literature for certain metals. The measured variation in the concentrations of Cd, Zn, and Cu is thought to be due to associated water and/or sediment particles from the producing wells or that picked up during transport. The greater consistency in our measurements for Cr and As suggests that these metals are predominantly associated with the hydrocarbon matrix. Based on the results of this work, it can be concluded that emissions of Cd, Zn, Cu, Cr, and As by the oil industry in the Netherlands are most probably significantly lower than hitherto assumed.     

Size-resolved trace metal characterization of aerosols emitted by four important source types in Switzerland

In central Switzerland five types of emission sources are mainly responsible for airborne trace metals: traffic, industrial plants burning heavy oil, resuspension of soil particles, residential heatings and refuse incineration plants. The particulate emissions of each of these source types except refuse incineration were sampled using Berner impactors and the mass and elemental size distributions of Cd, Cu, Mn, Pb, Zn, As and Na determined.Cd, Na and Zn are not characteristic for any of these source types. As and Cu, occurring in the fine particle fractions are characteristic for heavy oil combustion, Mn for soil dust and sometimes for heavy and fuel oil combustion and Pb for traffic aerosols. The mass size distributions of aerosols originating from erosion and abrasion processes show a maximum mass fraction in the coarse particle range larger than about 1 μm aerodynamic equivalent diameters (A.E.D.). Aerosols originating from combustion processes show a second maximum mass fraction in the fine particle range below about 0.5μm A.E.D.Scanning electron microscopy combined with an EDS analyzer was used for the morphological characterization of emission and ambient aerosols.     

Dissolution and solubility of trace metals from natural and anthropogenic aerosol particulate matter

An open flow reactor is used to simulate the dissolution process of mineral aerosol particles in atmospheric water droplets. Data on dissolution kinetic and solubility are provided for the major trace metals from two kinds of matrix: alumino-silicated and carbonaceous sample. The results emphasise that the metals contained in the carbonaceous aerosols are easier dissolved than in the alumino-silicated particles. The released concentrations are not related to the total metal composition or the origin of particles, but are directly associated with the type of liaisons whereby the metals are bound in the solid matrix. Thus, the metals coming from carbonaceous particles are adsorbed impurities or salts and hence are very soluble and with a dissolution hardly dependent on pH, whereas the metals dissolved from alumino-silicated particles are less soluble, notably the ones constitutive of the matrix network (Fe, Mn), and with a dissolution highly influenced by pH. Consequently, in the regions with an anthropogenic influence, the dissolved concentrations of metals found in the atmospheric waters are mainly governed by the elemental carbon content. Moreover, it appears that the dissolution kinetic of metals is not constant as a function of time. The dissolution rates are very rapid in the first 20 min of leaching and then they are stabilised to lower values in comparison to initial rates. By consequence, the total dissolved metal content is provided after the first 20 min of the droplet lifetime. For this reason, the effects of trace metals on the atmospheric aqueous chemistry and as atmospheric wet input to the marine biota are maximal for "aged" droplets.     

Nondestructive characterization of municipal-solid-waste-contaminated surface soil by energy-dispersive X-ray fluorescence and low-Z (atomic number) particle electron probe X-ray microanalysis

The long-term environmental impact of municipal solid waste (MSW) landfilling is still under investigation due to the lack of detailed characterization studies. A MSW landfill site, popularly known as Dhapa, in the eastern fringe of the metropolis of Kolkata, India, is the subject of present study. A vast area of Dhapa, adjoining the current core MSW dump site and evolving from the raw MSW dumping in the past, is presently used for the cultivation of vegetables. The inorganic chemical characteristics of the MSW-contaminated Dhapa surface soil (covering a 2-km stretch of the area) along with a natural composite (geogenic) soil sample (from a small countryside farm), for comparison, were investigated using two complementary nondestructive analytical techniques, energy-dispersive X-ray fluorescence (EDXRF) for bulk analysis and low-Z (atomic number) particle electron probe X-ray microanalysis (low-Z particle EPMA) for single-particle analysis. The bulk concentrations of K, Rb, and Zr remain almost unchanged in all the soil samples. The Dhapa soil is found to be polluted with heavy metals such as Cu, Zn, and Pb (highly elevated) and Ti, Cr, Mn, Fe, Ni, and Sr (moderately elevated), compared to the natural countryside soil. These high bulk concentration levels of heavy metals were compared with the Ecological Soil Screening Levels for these elements (U.S. Environment Protection Agency) to assess the potential risk on the immediate biotic environment. Low-Z particle EPMA results showed that the aluminosilicate-containing particles were the most abundant, followed by SiO2, CaCO3-containing, and carbonaceous particles in the Dhapa samples, whereas in the countryside sample only aluminosilicate-containing and SiO2 particles were observed. The mineral particles encountered in the countryside sample are solely of geogenic origin, whereas those from the Dhapa samples seem to have evolved from a mixture of raw dumped MSW, urban dust, and other contributing factors such as wind, precipitation, weather patterns, farming, and water logging, resulting in their diverse chemical compositions and the abundant observation of carbonaceous species. Particles containing C and P were more abundant in the Dhapa samples than in the countryside soil sample, suggesting that MSW-contaminated soils are more fertile. However, the levels of particles containing potentially toxic heavy metals such as Cr, Mn, Ni, Cu, Zn, and/or Pb in the Dhapa samples were significant, corroborated by their high bulk concentration levels (EDXRF), causing deep concern for the immediate environment and contamination of the food chain through food crops.     

粉煤燃烧过程中细粒子形成机理的研究

煤是一种有机沉淀岩 ,主要包括有机碳化合物和无机矿物。在燃烧的高温条件下 ,煤中的矿物质首先经历热分解和气化 ,当烟气冷却时 ,它们经过冷凝成核、凝结和团聚等作用 ,形成大量细粒子。这些细粒子的排放会对大气环境和人类健康造成严重的影响。研究燃烧过程中细粒子的形成机理将为其污染防治提供理论基础和科学依据。本文系统地综述了煤燃烧过程中矿物质和痕量元素的气化、冷凝成核、表面凝结、团聚的机理、模拟和预测方法以及细粒子形成机理的研究进展。     

Characterisation of particulate matter and gaseous emissions from a large ship diesel engine

Composition of exhaust from a ship diesel engine using heavy fuel oil (HFO) was investigated onboard a large cargo vessel. The emitted particulate matter (PM) properties related to environmental and health impacts were investigated along with composition of the gas-phase emissions. Mass, size distribution, chemical composition and microphysical structure of the PM were investigated. The emission factor for PM was 5.3 g (kg fuel)^?1. The mass size distribution showed a bimodal shape with two maxima: one in the accumulation mode with mean particle diameter D_P around 0.5 μm and one in the coarse mode at D_P around 7 μm. The PM composition was dominated by organic carbon (OC), ash and sulphate while the elemental carbon (EC) composed only a few percent of the total PM. Increase of the PM in exhaust upon cooling was associated with increase of OC and sulphate. Laser analysis of the adsorbed phase in the cooled exhaust showed presence of a rich mixture of polycyclic aromatic hydrocarbon (PAH) species with molecular mass 178–300 amu while PM collected in the hot exhaust showed only four PAH masses.Microstructure and elemental analysis of ship combustion residuals indicate three distinct morphological structures with different chemical composition: soot aggregates, significantly metal polluted; char particles, clean or containing minerals; mineral and/or ash particles. Additionally, organic carbon particles of unburned fuel or/and lubricating oil origin were observed. Hazardous constituents from the combustion of heavy fuel oil such as transitional and alkali earth metals (V, Ni, Ca, Fe) were observed in the PM samples.Measurements of gaseous composition in the exhaust of this particular ship showed emission factors that are on the low side of the interval of global emission factors published in literature for NO_x, hydrocarbons (HC) and CO.     

Size distribution and anthropogenic sources apportionment of airborne trace metals in Kanazawa, Japan

Aerosol samples were collected from Kanazawa, Japan to examine the size distribution of 12 elements and to identify the major sources of anthropogenic elements. Key emission sources were identified and, concentrations contributed from individual sources were estimated as well. Concentrations of elements V, Ca, Cd, Fe, Ba, Mg, Mn, Pb, Sr, Zn, Co and Cu in aerosols were determined with ICP-MS. The results showed that Ca, Mg, Sr, Mn, Co and Fe were mainly associated with coarse particles (>2.1 μm), primarily from natural sources. In contrast, the elements Zn, Ba, Cd, V, Pb and Cu dominated in fine aerosol particles (<2.1 μm), implying that the anthropogenic origin is the dominant source. Results of the factor analysis on elements with high EF_Crust values (>10) showed that emissions from waste combustion in incinerators, oil combustion (involving waste oil burning and oil combustion in both incinerators and electricity generation plants), as well as coal combustion in electricity generation plants were major contributors of anthropogenic metals in the ambient atmosphere in Kanazawa. Quantitatively estimated sum of mean concentrations of anthropogenic elements from the key sources were in good agreement with the observed values. Results of this study elucidate the need for making pollution control strategy in this area.     

Comparative analysis of the structure of carbon materials relevant in combustion

The determination of the structure of carbon materials is an analytical problem that join the research scientific communities involved in the chemical characterization of heavy fuel-derived products (heavy fuel oils, coal-derived fuels, shale oil, etc.) and of carbon materials (polycyclic aromatic compounds, tar, soot) produced in many combustion processes.

The knowledge of the structure of these “difficult” fuels and of the carbon materials produced by incomplete combustion is relevant to research for the best low-environmental impact operation of combustion systems; but an array of many analytical and spectroscopic tools are necessary, and often not sufficient, to attempt the characterization of such complex products and in particular to determine the distribution of molecular masses.

In this paper the size exclusion chromatography using N-methyl-pyrrolidinone as eluent has been applied for the characterization of different carbon materials starting from typical carbon species, commercially available like polyacenaphthylene, carbon black, naphthalene pitch up to combustion products like soot and soot extract collected in fuel-rich combustion systems. Two main fractions were detected, separated and molecular weights (MWs) determined by comparison with polystyrene standards: a first fraction consisted of particles with very large molecular masses (>100 000 u); a second fraction consisted of species in a relatively small MW range (200–600 u). The distribution of these fractions changes in dependence on the carbon sample characteristics.

Fluorescence spectroscopy applied on the fractions separated by size-exclusion chromatography has been used and comparatively interpreted giving indications on the differences and similarities in chemical structure of such different materials.     

Application of spectrometric analysis to the identification of pollution sources causing cultural heritage damage

Black crusts are recognized to have been, up to now, one of the major deterioration forms affecting the built heritage in urban areas. Their formation is demonstrated to occur mainly on carbonate building materials, whose interaction with an SO₂-loaded atmosphere leads to the transformation of calcium carbonate (calcite) into calcium sulfate dihydrate (gypsum) which, together with embedded carbonaceous particles, consequently forms the black crusts on the stone surface. An analytical study was carried out on black crust samples collected from limestone monumental buildings and churches belonging to the European built Heritage, i.e., the Corner Palace in Venice (Italy), the Cathedral of St. Rombouts in Mechelen (Belgium), and the Church of St. Eustache in Paris (France). For a complete characterization of the black crusts, an approach integrating different and complementary techniques was used, including laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS), Fourier transform infrared spectroscopy, optical and scanning electron microscopy. In particular, the application of LA-ICP-MS permitted to obtain a complete geochemical characterization in terms of trace elements of the black crusts from the inner parts to the external layers contributing to the identification of the major combustion sources responsible for the deterioration over time of the monuments under study. In addition, the obtained results revealed a relation between the height of sampling and the concentration of heavy metals and proved that the crust composition can be a marker to evaluate the variation of the fuels used over time.     

Size distribution and anthropogenic sources apportionment of airborne trace metals in Kanazawa,Japan

Aerosol samples were collected from Kanazawa, Japan to examine the size distribution of 12 elements and to identify the major sources of anthropogenic elements. Key emission sources were identified and, concentrations contributed from individual sources were estimated as well. Concentrations of elements V, Ca, Cd, Fe, Ba, Mg, Mn, Pb, Sr, Zn, Co and Cu in aerosols were determined with ICP-MS. The results showed that Ca, Mg, Sr, Mn, Co and Fe were mainly associated with coarse particles (>2.1 μm), primarily from natural sources. In contrast, the elements Zn, Ba, Cd, V, Pb and Cu dominated in fine aerosol particles (<2.1 μm), implying that the anthropogenic origin is the dominant source. Results of the factor analysis on elements with high EF_Crust values (>10) showed that emissions from waste combustion in incinerators, oil combustion (involving waste oil burning and oil combustion in both incinerators and electricity generation plants), as well as coal combustion in electricity generation plants were major contributors of anthropogenic metals in the ambient atmosphere in Kanazawa. Quantitatively estimated sum of mean concentrations of anthropogenic elements from the key sources were in good agreement with the observed values. Results of this study elucidate the need for making pollution control strategy in this area.     

Chemical and mineralogical forms of Cu and Ni in contaminated soils from the Sudbury mining and smelting region, Canada

Available information on soil contamination by trace elements in the Sudbury Cu/Ni mining and smelting region consists largely of total elemental concentration data. Little is known about the mode of occurrence and behaviour of Cu and Ni (the main metallic contaminants) in the soils of the region. In this study, sequential extraction and Scanning Electron Microscopy and Energy Dispersive X-ray Analysis (SEM/EDX) observations were complementarily used to define Cu and Ni forms in the Sudbury soils, so as to assess metal mobility. Most Cu (on average 75%) was associated with 'non-residual' soil forms, whereas Ni was mainly (on average 60%) associated with inorganic 'residual' forms of a sulphide and oxide nature. Therefore, Cu occurs in the soils in more mobile forms than Ni. Consequently, Cu should be removed from these soils at a faster rate than Ni. This is an unusual finding, because generally Ni is known to be more mobile in soils than Cu. SEM/EDX analysis confirmed the greater Cu mobility by showing that the metal was strongly associated with organic matter and was homogeneously distributed on the clay fraction surfaces. Nickel occurred alone or was associated with Fe oxides in various size fractions. Both elements were found as sulphides but Ni was often included in the silicate matrices of spherical particles in associations with Fe. SEM/EDX observations have shown that Cu and Ni are associated with soil forms which would not have been predicted by the sequential extraction alone, such as carbonaceous material, silicate spheres and carbonate particles, supporting complementary use of the two techniques.     

Dynamic studies on the mobility of trace elements in soil and sediment samples influenced by dumping of residues of the flood in the Mulde River region in 2002

In the analysis of soil samples, batch sequential extraction procedures are traditionally used for the fractionation of trace elements to access their mobility and potential risk for the contamination of groundwater. In the present work a continuous-flow technique has been used that enables not only the fast and efficient leaching of trace elements but as well as time-resolved studies on the mobilization of arsenic and selected heavy metals in different forms to be made. Rotating coiled columns (RCC) earlier used mainly in countercurrent chromatography have been successfully applied to the dynamic leaching of heavy metals from soils contaminated by flooding sludge's. The sample was retained in a PTFE rotating column as the stationary phase whereas aqueous solutions were continuously pumped through. The contents of elements were determined by on-line coupling of RCC and inductively coupled plasma atomic emission spectrometry (ICP-AES). This enables real-time data on the leaching process to be obtained. Dynamic and traditional batch procedures were compared. It has been shown that the aqueous elution under centrifugal forced conditions is much more effective for the mobilization of heavy metals. Hence, the dynamic leaching is characterized by a substantially more intensive interaction between solid and water and is besides substantially more time-saving than the conventional batch procedure. The RCC procedure was also employed for preliminary leaching studies with a simulated "acid rain". In comparison with the water leaching, the mobilization of heavy metals and arsenic from soil samples with employment of simulated acid rain as eluent was less effective.     

Reconstructed mass-spectrometric pattern for characterization of carbon compounds in smoker's lung in situ

BACKGROUND: Cigarette smoke is a major anthropogenic pollutant and contributes to the permanent load of ambient particulate matter in the air, particularly indoors. It is the leading risk factor for premature loss of life due to chronic bronchitis, emphysema and lung cancer. Smoker's lung and graphite pneumoconiosis are pathological states characterized by the deposition of carbonaceous particles. METHODS: Mass spectrometry was used to evaluate unstained lung sections obtained in vivo from a heavy smoker and a patient with occupationally acquired graphite pneumoconiosis. RESULTS AND DISCUSSION: The composition of carbon compounds deposited in lung tissue samples is demonstrated here for the first time. Thirty carbonaceous-containing microareas from ten biopsies (three areas per biopsy) of lung tissues were analyzed mass-spectrometrically. In each case, the samples were taken from a smoker's lung or those demonstrating a graphite pneumoconiosis. The lung-tissue samples were selected by light microscopy before they were evaporated for mass spectrometry. First-order criteria were anionic and cationic mass peaks which occur within the mass patterns in lung tissues of smoker's lung, although not in graphite pneumoconiosis. Second-order criteria were mass peaks from smoker's lung with standard deviations SD < or = 14% of the mean value. First and second-order mass peaks matched the mass peaks of experimental cigarette-smoke condensate in 9 out of 11 peaks. A software program was developed that enabled fast, automated recognition of the typical mass peaks, and thereby confirmed the histological diagnosis of smoker's lung. CONCLUSIONS: The analysis of carbonaceous particles within lung biopsies from a heavy smoker corresponded to the spectra of tobacco condensate and not to the investigated biopsies of graphite peneumoconiosis. RECOMMENDATION AND OUTLOOK: The analyses were performed in order to find out whether mass-spectrometric criteria exist for the differentiation of carbonaceous lung-tissue deposits. Mass spectrometry may be a valuable tool in determining the composition of carbon compounds deposited in human lung tissue. So far, qualitative assessment of the composition of deposits in lung tissue is only possible after the patient is deceased (autopsy).     

Evaluating the size distribution characteristics and sources of atmospheric trace elements at two mountain sites: comparison of the clean and polluted regions in China

Size-resolved trace metal concentrations at two background sites were assessed during a 1-year observation campaign, with the measurements performed in parallel at two mountain sites, where Mt. Dinghu (DHS) located in the rural region of Pearl River Delta (PRD) and Mt. Gongga (GGS) located in the Tibetan Plateau region. In total, 15 selected trace elements (Mg, Al, K, V, Mn, Fe, Cu, Zn, As, Mo, Ag, Cd, Ba, Tl, and Pb) in aerosol samples were determined using inductively coupled plasma mass spectrometry (ICPMS). The major metals in these two mountain sites were Fe, K, Mg, and Ca with concentrations ranging between 241 and 1452 ng/m³, 428 and 1351 ng/m³, 334 and 875 ng/m³, and 376 and 870 ng/m³, respectively, while the trace metals with the lowest concentrations were Mo, Ag, Cd, and Tl with concentrations lower than 4 ng/m³ in DHS and 2 ng/m³ in GGS. The pronounced seasonal variability in the trace elements was observed in DHS, with lower concentrations in spring and summer and relatively high in winter and autumn, whereas seasonal variance of trace elements is hardly observed in Mt. Gongga. The size distribution pattern of crustal elements of Al, Mg, K, Ba, and Fe was quite similar in DHS and GGS, which were mainly found in coarse particles peaked at 4.7–5.8 μm. In addition, V, Mo, Ag, and Tl were also concentrated in coarse particles, although the high enrichment factor (EF?>?100) of which suggested anthropogenic origin, whereas trace metals of Cd, Mn, Zn, As, Cu, and Pb concentrated in fine mode particles. Specifically, these trace metals peak at approximately 1.5 μm in DHS, while those in GGS peaked at diameter smaller than 0.3 μm, indicating the responsible for long-range transport from the far urban and industrialized areas. Multivariate receptor model combined with the enrichment factor results demonstrated that the trace elemental components at these two background sites were largely contributed from the fossil fuel combustion (55.4% in DHS and 44.0% in GGS) and industrial emissions factors (20.1% vs. 26.5%), which are associated with long distance transport from the coastal area of Southeast China and the Northwestern India, respectively, as suggested by the backward air mass trajectory analysis. Local sources from soil dust contributed a minor variance for trace elements in DHS (9.7%) and GGS (13.8%), respectively.

     

高速公路路面沉积物的污染特性

对湖南省长潭西高速公路不同采样点的路面沉积物进行取样分析,并检测了样品的颗粒级配、COD、重金属(Cu、Zn、Pb和Cd)和有机质。结果表明,路面沉积物主要以粒径<0.15 mm的颗粒为主;较小颗粒物中的COD含量高于较大颗粒中的COD含量;粒径在0.15 mm以下的颗粒物所含重金属Cu、Zn、Pb和Cd的浓度普遍高于所选的土壤标准值,降雨一旦形成径流将会产生严重的污染危害;沉积物中的有机质含量对重金属的吸附有一定的影响,有机质含量越高,沉积物中重金属含量相对也高。     

Distribution behavior of heavy metals investigated in a laboratory-scale incinerator

The distribution behavior of Pb, Cd, Fe, Cu, Mo and Zn was determined in a laboratory-scale incinerator. Points of interest were the influence of the temperature and combustion atmosphere on the emission rates of those metals, orientating at frequent combustion conditions of accidental fires. The experiments were carried out at 600 degrees C and 800 degrees C in N2, air, N2 + HCl and air + HCl atmospheres. Furthermore, the influence of the matrix (quartz, polyethylene and cellulose powder) on the distribution behavior of the heavy metals was investigated as well. It was determined whether the distribution behavior of Cu, Pb and Cd were affected by the other heavy metals. In conclusion, it was found that in air and N2 atmosphere a temperature increase from 600 degrees C to 800 degrees C and the addition of the matrix had no effect on the evaporation rates of the heavy metals, except for Cd. Addition of gaseous HCl led to increased evaporation of the heavy metals. The increase of the evaporation rates during the experiments with matrix was higher for Fe, remained the same for Pb, Cd, Zn, and lower for Mo and Cu compared to the experiments without matrix.