Real-time analysis of soot emissions from bituminous coal pyrolysis and combustion with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer

This paper reports on-line analyses of the soot emissions from the Inner Mongolia bituminous coal combustion and pyrolysis processes with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS). The soot particles are generated by heating a small amount of screened coal powder in synthetic air and nitrogen atmosphere in a tubular oven. The vacuum ultraviolet photoionization time-of-flight (VUV-TOF) mass spectra of the soot particles emitted from combustion and pyrolysis at different oven temperatures and different stages are obtained. The VUV-TOF mass spectra are assigned with the references of the results of the off-line GC/MS analysis.     

Urban environmental mercury in Changchun, a metropolitan city in Northeastern China: source, cycle, and fate

Mercury concentrations in each environmental compartment in Changchun City had obvious spatial and temporal trends. Particulate Hg (HgP) and total gaseous mercury (TGM) concentrations in air, total Hg (HgT) concentrations in precipitation and ratios of HgP to HgT (total Hg in air) in the atmosphere in heating season were higher than those in non-heating season, which resulted from civil heating. In contrast, reactive Hg (HgR) concentrations in precipitation were higher in non-heating season than those in heating season. TGM and SO2 in air had good agreement. HgP concentrations in the atmosphere were correlated with HgT concentrations in precipitation. Based on Hg concentrations in each environmental compartment, Hg exchange fluxes between environmental interfaces were estimated. Only 11.6% of Hg, emitted from coal combustion, deposited into land surface in urban district and the rest part participated in regional or global cycle, so urban district was the source of Hg global and regional cycle. Net fluxes of Hg into land surface and water were 34.26 kg year(-1) and 0.051 kg year(-1), respectively, which were clearly accumulated in the water and soil. Therefore considering urban local Hg cycle, each environmental compartment of urban ecosystem (water, air and soil) was the sink of Hg.     

The distribution, occurrence and environmental effect of mercury in Chinese coals

Mercury (Hg) is a toxic, persistent, and globally distributed pollutant due to its characteristic properties such as low melting and boiling points, conversion between chemical forms and participation in biological cycles. During combustion mercury in coal is almost totally emitted to the atmosphere. With a huge amount of coal consumed, coal combustion is one of the main anthropogenic sources of this element in the environment. In this study, Hg data of 1699 coal samples of China has been compiled, and the concentration, distribution, modes of occurrence, and the impact of Hg emissions on the environment are investigated. Most Chinese coals have Hg content in the range of 0.1 to 0.3 ppm, with an average of 0.19 ppm, which is slightly higher than the average Hg content of world coals and is close to that of the U.S. coals. The Hg content in coals varies in different coal basins, geological ages and coal ranks. The most likely mode of occurrences of Hg in high-sulfur and high Hg content coals is as solid solution in pyrite. But in low-sulfur coals, modes of occurrence of Hg are variable, and the organic-bound and sulfide-bound Hg may dominate. Silicate-bound Hg may be the main form in some coals because of magmatic intrusion. Mercury emissions during coal combustion have resulted in serious environmental contamination in China, particularly in the northeastern and southwestern China, where a high Hg content in the atmosphere occurs.     

冷发生炉煤气作玻璃熔窑气体加热燃料的探讨

从玻璃熔窑加热燃料现状、气体燃料选择方案、理论燃烧温度、清洁生产分析等方面论述了用脱硫后的冷发生炉煤气增热和预热助燃空气替代重油作为玻璃熔窑加热燃料的可行性.     

Atmospheric mercury near a chlor-alkali plant in Sweden

Atmospheric mercury species/fractions were measured near a chlor-alkali plant in Sweden during August 28 to September 4, 2001. The concentration of total gaseous mercury in the plume from the plant was measured using TEKRAN and GARDIS instruments. Gaseous elemental mercury was measured using a light detection and ranging (LIDAR) technique. From vertical LIDAR sweeps through the plume from the chlor-alkali plant mercury emission rates could be calculated. The concentrations of reactive gaseous mercury (RGM) in the plume and also inside the cell house were measured using annular KCl coated denuders. The RGM emission constitutes 0.5-1.0% of the total mercury emitted from the plant. The mercury concentration adsorbed on particles was measured as well as the mercury flux from soil. The data presented also include an intercomparison showing an excellent agreement between TEKRAN/GARDIS and LIDAR gaseous mercury measurements.     

Estimation of mercury emission from different sources to atmosphere in Chongqing, China

This investigation presents a first assessment of the contribution to the regional mercury budget from anthropogenic and natural sources in Chongqing, an important industrial region in southwest China. The emissions of mercury to atmosphere from anthropogenic sources in the region were estimated through indirect approaches, i.e. using commonly acceptable emission factors method, which based on annual process throughputs or consumption for these sources. The natural mercury emissions were estimated from selected natural sources by the dynamic flux chamber technique. The results indicated that the anthropogenic mercury emissions totaled approximately 8.85 tons (t), more than 50% of this total originated in coal combustion and 23.7% of this total emission in the industrial process (include cement production, metal smelting and chemical industry). The natural emissions represented approximately 17% of total emissions (1.78 t yr(-1)). The total mercury emission to atmosphere in Chongqing in 2001 was 10.63 t.     

Preliminary investigation of the mercury saturation in the Baltic Sea winter surface water

A new experimental measuring system for the total gaseous mercury saturation in the sea surface water has been developed. The technique applied to the system is based on equilibrating water-air mercury partial pressures at the air-sea interface. First data using this system were collected in the Baltic Sea on 13-22 January 2000. Measurements were completed from the research vessel 'Alexander von Humboldt' on the way from the Gotland Sea to the Mecklenburg Bight. In general the results showed domination of supersaturated winter sea surface waters with respect to gaseous mercury. Two areas with distinctly elevated mercury saturation were found: one in the east-west shipping route, south of Bornholm, where the equilibrated gaseous Hg content of water was approximately 9.2-fold higher, and another over the ammunition disposal region south-east of Hoburgs Bank, where the Hg content of water was approximately 3.8-fold higher than that in air. In general, the data indicate that the south-western Baltic Sea, and in particular both maritime areas identified with elevated mercury saturation, can emit gaseous mercury from surface waters into the atmosphere and contribute to long-range atmospheric transport.     

Mercury emissions to the atmosphere from anthropogenic sources in Europe in 2000 and their scenarios until 2020

The paper reviews the current state of knowledge regarding European emissions of mercury and presents estimates of European emissions of mercury to the atmosphere from anthropogenic sources for the year 2000. This information was then used as a basis for Hg emission scenario development until the year 2020. Combustion of coal in power plants and residential heat furnaces generates about half of the European emissions being 239 tonnes. The coal combustion is followed by the production of caustic soda with the use of the Hg cell process (17%). Major points of mercury emission generation in the mercury cell process include: by-product hydrogen stream, end box ventilation air, and cell room ventilation air. This technology is now being changed to other caustic soda production technologies and further reduction of Hg emissions is expected in this connection. The third category on the list of the largest Hg emitters in Europe is cement production (about 13%). The largest emissions were estimated for Russia (the European part of the country), contributing with about 27% to the European emissions, followed by Poland, Germany, Spain, Ukraine, France, Italy and the United Kingdom. Most of these countries use coal as a major source of energy in order to meet the electricity and heat demands. In general, countries in the Central and Eastern Europe generated the main part of the European emissions in 2000. Emission reductions between 20% and 80% of the 2000 emission amounts can be obtained by the year 2020, as estimated by various scenarios.     

Mercury emissions from a coal-fired power plant in Japan

The emissions study for mercury was conducted at a 700 MW coal-fired plant for the combustion of three types of coal with mercury concentrations of 0.0063, 0.0367 and 0.065 mg/kg. The power plant is equipped with a cold-side electrostatic precipitator and wet type flue gas desulfurization system. During full load operation of the boilers, samples of the input and output streams such as coal, coal ash, ESP ash and post-ESP particulates and flue gas were collected. The Hg concentrations in solid were measured by cold-vapor atomic absorption spectrometry (AAS) after appropriate preparation and acid digestion. Gaseous Hg was collected using a mixed solution of potassium permanganate and sulfuric acid and the Hg concentrations in the samples were measured using cold-vapor AAS. The results were used to examine: (1) overall mass balances; (2) relative distribution in the power plant; (3) equilibrium of Hg species using MALT-2 calculation program; and (4) Hg concentrations in stack emissions. The mass balances estimated in this study were 100, 138 and 89%, respectively, for the coals. Total Hg concentrations in stack gas were 1.113, 0.422 and 0.712 microg(m3N), respectively, for the coals. More than 99.5% of the Hg in the stack emissions were in gaseous form and the proportion in particulate form was extremely low. The relative distribution of Hg in ESP, FGD and Stack ranged from 8.3 to 55.2%, 13.3 to 69.2% and 12.2% to 44.4%, respectively. The results indicated that factors other than the Hg concentration of coals and efficiency of pollution control devices might affect Hg emissions from coal-fired plant. The calculated equilibrium of the distribution of Hg species using the MALT2 program suggest that it is necessary to consider condensation mechanism to interpret the affect of Hg species on the variations of the removal efficiencies of Hg in the ESP.     

Mercury emissions from selected stationary combustion sources in Korea

Mercury emissions from various stationary combustion sources such as coal-fired power plants, oil-fired power plants, industrial utility oil boilers, iron manufacturing plants, and industrial waste incinerators, were measured. The US EPA (Environmental protection agency) method 101A and the Ontario hydro method were used to sample the mercury containing combustion flue gases, at the inlet of the air pollution control devices (APCDs) and at the stack. Collected samples of both gaseous and particulate forms were then analyzed using CVAA (cold vapor atomic absorption) type analyzer. Measurement results from the coal-fired power plant showed percentages of elemental mercury (Hg0) as high as 31.4% and as low as 9.5%. However, the content of Hg0 was in the range of 1.3-3.7% from the industrial waste incinerator. Differences in mercury speciation from various stationary combustion sources are believed to be coming from: (1) difference in the fuel types; (2) difference in the major flue gas compositions (ex. HCl and SOx); and (3) difference in the types of air pollution control devices (APCDs). When the measurement results obtained using different sampling methods were compared, the Ontario Hydro Method gave a slightly higher mercury concentration measurement than that of the US EPA Method 101A.     

Piloted ignition times,critical heat fluxes and mass loss rates at reduced oxygen atmospheres

Ignition, pyrolysis and burning of materials in reduced oxygen atmospheres occur when recirculating combustion gases are mixed with the air flowing into an enclosure. Still the incoming air can be sufficient for the complete combustion of the pyrolysis gases. Thus, for the prediction of fires in enclosures it is essential to understand the ignition and burning of materials in a reduced oxygen atmosphere even when plenty of oxidizer is available for complete combustion. Previous work employing gaseous fuels has shown that under these conditions, but before extinction, burning of gaseous fuels issuing from a nozzle is complete but radiation from the flames decreases owing to the reduction of their temperature. Complementary to that work, piloted ignition of solids is investigated here at reduced oxygen concentrations by measuring the ignition times and mass loss rates of the solid at ignition.These results were obtained in a cone calorimeter modified to supply air at reduced oxygen concentrations. Two types of plywood, normal and fire retardant 4 mm thick were examined at three imposed heat fluxes 25, 35 and 50 kW/m² and at oxygen concentrations of 21%, 18% and 15% by volume. Because heating at these heat fluxes and material thickness corresponds to intermediate thermal conditions (i.e. neither thin nor thick), novel analytical solutions are developed to analyze the data and extract the thermal and ignition properties of the material. The same novel solutions can be applied to modeling concurrent or countercurrent flame spread. Moreover, a theory for piloted ignition explains why the ignition times and mass pyrolysis rates are weakly dependent on reduced oxygen concentrations.     

A prospective atmospheric emission inventory for cadmium--the European community as a study area

The quantities of cadmium emitted to the atmosphere from natural and human sources have been estimated for the member states of the European Community, allowing the construction of an atmospheric emission inventory for cadmium at the regional level. A survey of the available emission data was used to calculate an emission factor (g cadmium emitted tonne -1 material consumed or produced) for each source. This value was applied to the most recent consumption or production data for the region to obtain an annual discharge estimate. Predictions of future trends in cadmium emissions from human sources over the next two decades were based on economic forecasts for the process in question. The iron and steel industries and refuse incineration are the two largest sources of airborne cadmium in the region, followed by volcanic action and zinc production. It is forecast that there will be an increase in cadmium emissions over the next two decades due mainly to the iron and steel industries and zinc production. A comparison of the emission estimates obtained in this study with those given in previously published inventories reveal disparities in the source strengths for some processes. In particular, it would appear that cadmium emissions from coal combustion and non-ferrous metal production have been overestimated in some past studies.     

A preliminary study on mercury contamination to the environment from artisanal zinc smelting using indigenous methods in Hezhang County, Guizhou, China: Part 2. Mercury contaminations to soil and crop

Artisanal zinc smelting using indigenous method in Hezhang County, Guizhou, China has posed seriously environmental pollution to the local environment. Within less than 150 km2 area in Hezhang, a few metric tons of mercury were released into the atmosphere each year since 1989 due to artisanal zinc smelting, and the surface waters were seriously contaminated with mercury. For the first time, we investigated the mercury contamination to the local soil and crop compartments due to mercury emissions from artisanal zinc smelting activities in this area. Mercury distribution patterns in 5 soil profiles collected in artisanal zinc smelting area showed that the top soils were seriously contaminated with mercury. The soils from agriculture land close to the zinc smelting areas were also contaminated with mercury due to the deposition of mercury species that emitted from artisanal zinc smelting processes. Total mercury concentrations in top soils decrease exponentially with distance from the zinc smelting area. Corn plants that were cultivated in agriculture land close to the zinc smelting area were also contaminated with mercury. Mercury concentration in corn plant tissue increased in the order of grains相似文献   

Heavy coal combustion as the dominant source of particulate pollution in Taiyuan, China, corroborated by high concentrations of arsenic and selenium in PM10

Coal burning generates toxic elements, some of which are characteristic of coal combustion such as arsenic and selenium, besides conventional coal combustion products. Airborne particulate samples with aerodynamic diameter less than 10 microm (PM(10)) were collected in Taiyuan, China, and multi-element analyses were performed by inductively coupled plasma atomic emission spectrometry (ICP-AES) and inductively coupled plasma mass spectrometry (ICP-MS). Concentrations of arsenic and selenium from ambient air in Taiyuan (average 43 and 58 ng m(-3), respectively) were relatively high compared to what is reported elsewhere. Arsenic and selenium were found to be highly correlated (r=0.997), indicating an overwhelmingly dominant source. Correlation between these two chalcophile elements and the lithophile element Al is high (r is 0.75 and 0.72 for As and Se, respectively). This prompted the hypothesis that the particles were from coal combustion. The enrichment of the trace elements could be explained by the volatilization-condensation mechanism during coal combustion process. Even higher correlations of arsenic and selenium with PM(10) (r=0.90 and 0.88) give further support that airborne particulate pollution in Taiyuan is mainly a direct result of heavy coal consumption. This conclusion agrees with the results from our previous study of individual airborne particles in Taiyuan.     

Elemental gaseous mercury flux at the water/air interface over the Negro River basin, Amazon, Brazil

The amount of dissolved gaseous mercury (DGM) released annually into the atmosphere by water bodies in each of the 18 major sub-basins of the Negro River tributaries has been estimated for the wet season and adopted for the entire year. Using Remote Sensors (RS) and the Geographic Information System (GIS), an estimate was made for the total flooded area during the period of the wet season (May-July), which corresponds to around 10% of the total basin area. The estimates of DGM evasive flux values were made during four scientific campaigns and ranged from 0.09 to 14 mug m(-2) y(-1). Mercury wet deposition to the same area was estimated using average values of the metal concentration in the rainwater (9.8 ng L(-1)), which varies from 17 to 27 microg m(-2) year(-1). Considering the flooded area of the Negro River Basin as 69,000 km(2), the total amount of mercury emitted by all bodies of water reaches nearly 0.26 ton year(-1), which represents not more than 2% of the total mercury found in wet deposition in this same area.     

Seasonal pollution characteristics of organic compounds in atmospheric fine particles in Beijing

Beijing is a rapidly developing city with severe and unique air pollution problems. Organic matter is the most abundant fraction in fine particles in Beijing, occupying 30-50% of the total mass, indicating its key role in air pollution control. However, detailed chemical characterization of particulate organic matter in Beijing has never been reported. In this study, fine particles in the urban atmosphere in Beijing were investigated for its organic components by GC/MS technique. Over 100 individual organic compounds were identified and quantified in 25 PM2.5 samples from the summer, autumn and winter of 2002-2003. Alkanes, fatty acids, dicarboxylic acids, polycyclic aromatic hydrocarbons and some important tracer compounds (hopanes, levoglucosan and steroids) were the major constituents with the sum of their concentrations of 502, 1471 and 1403 ng m(-3) in summer, autumn and winter, respectively. Different organic compounds presented apparently different seasonal characteristics, reflecting their different dominant emission sources, such as coal combustion, biomass burning and cooking emission. The abundance and origin of these organic compounds are discussed to reveal seasonal air pollution characteristics of Beijing.     

聚丙烯腈织物热稳定性与燃烧特性研究

对聚丙烯腈(PAN)织物在空气气氛下的热稳定性和3种热辐射强度下的燃烧特性进行研究。结果表明,PAN织物在空气气氛中的热分解过程主要包括3个失重阶段;随着热辐射强度的增大,PAN织物点燃时间有所提前,热释放速率和产烟率的峰值均得到了一定程度的提高,到达峰值的时间均有不同程度的提前,质量损失率增加,且初始热分解时间提前;当热辐射强度为25 kW/m2时,PAN织物的燃烧不充分,烟密度最大;热辐射强度越大,烟气扩散越快,且PAN织物的火灾性能指数值减小,火灾增长指数值增大;PAN织物具有较高的火灾危险性。     

The sulphuric acid content of soot

The sulphuric acid content of soot, originating from the combustion of fuel oil, has been determined by a specific method; 171 samples were studied. Of these samples, 89 were collected in a pilot plant boiler, fueled by residual fuel oil containing 2 to 5% sulphur. The remaining 72 samples were taken from 6 different locations from the firebox to the chimney of domestic heating furnaces burning light fuel oil. The results obtained suggest that most of the sulphuric acid found in urban air is emitted as such into the atmosphere, instead of being produced by the oxidation of SO₂ to SO₃, with subsequent hydration with H₂O.     

Accumulation and transformation of atmospheric mercury in soil

Field investigation and simulating experiments were carried out for understanding the accumulation and transformation of mercury in soil in relation to the deposition of atmospheric mercury. A positive correlation between the atmospheric mercury concentration and the content of mercury in soil was observed in the field investigation, with the correlation coefficient being 0.741** (n=52). The mercury content in soil decreased with the increasing distance from the mercury emission source. Simulated experiment demonstrated that the higher the mercury content in air was, the higher was the amount of mercury accumulated in soil, which was in accordance with the results found from the field investigation. Transformation process occurred once mercury deposited into the soil. Analyses of soil samples exposed to air with mercury contents of 796.4+/-186.3 ng/m(3) for 2 months indicated that 24.58-26.86% of total mercury deposited into the soil existed in Hg(0) form, 0.10-0.12% in active form, 14.56-18.75% in HCl-dissoluble form, 0.86-5.84% in organic-bound form and 52.64-55.29% in residual form.     

Simulation and health risk assessment of residential particle pollution by coal combustion in China

In China, residential coal combustion has resulted in serious indoor air pollution, and the emitted particulate matters and associated toxic organic compounds are greatly harmful to human health. For example, the high lung cancer mortality in Xuanwei County, Yunnan Province was attributed to inhalation of polycyclic aromatic hydrocarbons (PAHs)-coated particles within the houses. Based on previous investigations, this paper simulated the indoor particle pollution from coal combustion for a typical home in Xuanwei by computational fluid dynamics (CFD) method. Benzo[a]pyrene (BaP), one of the important pollutants from incomplete combustion, was used as a criterion for its strong carcinogenicity in risk assessment. Mechanical exhaust fan was installed in order to reduce the concentration of suspended particles indoors. Based on the simulated results, an engineering-oriented method was demonstrated to be effective in assessing indoor particle pollution by coal combustion and its health effect. Results indicated that the indoor particle pollution was rather serious due to the poor ventilation. Women, who spent more time indoors than men, had higher risk for lung cancer, and the predicted incidence for local people accorded well with previous surveys [Chapman RS, Mumford JL, Harris DB. The epidemiology of lung cancer in Xuanwei, China: current process, issues and research strategies. Archives of Environmental Health 1988;43(2):180–5]. The installation of the exhaust fan turned out to be effective in removing indoor particles since it greatly strengthened airflows and the contaminant removal is significantly improved.