Evaluation of mercury emissions to the atmosphere from coal combustion,China

Mercury emissions from the coal smoke is the main source of anthropogenic discharge and mercury pollution in atmosphere. The calculated total amount of mercury emissions of China in 1995 is approximately 213.8 tonnes, which accounts for c. 5% of estimated total global discharge of 4000 tonnes in the same period. From 1978 to 1995, total coal consumption increased fourfold. Based on these data it is estimated that the mercury emissions will increase at a rate of 5% a year, and the predicted emissions will be 273 tonnes in China in 2000. Controlling and solving mercury emissions from coal combustion are among the most important environmental tasks facing China.     

The history of mercury emissions from fuel combustion in Maritime Canada

In this study, we present an inventory of historical emissions of mercury resulting from combustion of wood, coal and refined petroleum products in Maritime Canada. The pattern of emissions illustrates the strong influences of population growth, industrial development and prevailing fuel preferences in the region. According to our calculations, anthropogenic mercury releases from fuel combustion in Maritime Canada have cumulatively totaled more than 50 tonnes since 1800. We have compiled both high and low estimates of annual mercury releases in this region. Mercury emissions from fuel combustion in Maritime Canada reached a maximum level in the 1940s. At this time, emissions were between 778 (low) and 1494 (high) kg per year, coinciding with the period of most intensive coal use in Maritime Canada. In 1995, emissions were approximately 54% of the level reached in 1940, at 427 (low)-800 (high) kg per year. In presenting this emissions inventory, we hope to refine past estimates with current information on the mercury content of different fuel types, and create a comprehensive database on how mercury emissions from various sources have changed over time.     

A new method to assess mercury emissions: a study of three coal-fired electric-generating power station configurations

U.S. Environmental Protection Agency (EPA) Method 7473 for the analysis of mercury (Hg) by thermal decomposition, amalgamation, and atomic absorption spectroscopy has proved successful for use in Hg assessment at coal-fired power stations. In an analysis time of approximately 5 min per sample, this instrumental methodology can directly analyze total Hg--with no discrete sample preparation--in the solid matrices associated with a coal-fired power plant, including coal, fly ash, bottom ash, and flue gas desulfurization (FGD) material. This analysis technique was used to investigate Hg capture by coal combustion byproducts (CCBs) in three different coal-fired power plant configurations. Hg capture and associated emissions were estimated by partial mass balance. The station equipped with an FGD system demonstrated 68% capture on FGD material and an emissions estimate of 18% (11 kg/yr) of total Hg input. The power plant equipped with low oxides of nitrogen burners and an electrostatic precipitator (ESP) retained 43% on the fly ash and emitted 57% (51 kg/yr). The station equipped with conventional burners and an ESP retained less than 1% on the fly ash, emitting an estimated 99% (88 kg/yr) of Hg. Estimated Hg emissions demonstrate good agreement with EPA data for the power stations investigated.     

A New Method to Assess Mercury Emissions: A Study of Three Coal-Fired Electric-Generating Power Station Configurations

Abstract

U.S. Environmental Protection Agency (EPA) Method 7473 for the analysis of mercury (Hg) by thermal decomposition, amalgamation, and atomic absorption spectroscopy has proved successful for use in Hg assessment at coal-fired power stations. In an analysis time of ～5 min per sample, this instrumental methodology can directly analyze total Hg—with no discrete sample preparation—in the solid matrices associated with a coal-fired power plant, including coal, fly ash, bottom ash, and flue gas desulfurization (FGD) material. This analysis technique was used to investigate Hg capture by coal combustion byproducts (CCBs) in three different coal-fired power plant configurations. Hg capture and associated emissions were estimated by partial mass balance. The station equipped with an FGD system demonstrated 68% capture on FGD material and an emissions estimate of 18% (11 kg/yr) of total Hg input. The power plant equipped with low oxides of nitrogen burners and an electrostatic precipitator (ESP) retained 43% on the fly ash and emitted 57% (51 kg/yr). The station equipped with conventional burners and an ESP retained less than 1% on the fly ash, emitting an estimated 99% (88 kg/yr) of Hg. Estimated Hg emissions demonstrate good agreement with EPA data for the power stations investigated.     

Anthropogenic mercury emissions in China

An inventory of mercury emissions from anthropogenic activities in China is compiled for the year 1999 from official statistical data. We estimate that China's emissions were 536 (±236) t of total mercury. This value includes open biomass burning, but does not include natural sources or re-emission of previously deposited mercury. Approximately 45% of the Hg comes from non-ferrous metals smelting, 38% from coal combustion, and 17% from miscellaneous activities, of which battery and fluorescent lamp production and cement production are the largest. Emissions are heaviest in Liaoning and Guangdong Provinces, where extensive smelting occurs, and in Guizhou Province, where there is much small-scale combustion of high-Hg coal without emission control devices. Emissions are gridded at 30×30 min spatial resolution. We estimate that 56% of the Hg in China is released as Hg⁰, 32% as Hg²⁺, and 12% as Hg^p. Particulate mercury emissions are high in China due to heavy burning of coal in residential and small industrial settings without PM controls. Emissions of Hg²⁺ from coal-fired power plants are high due to the absence of flue-gas desulfurization units, which tend to dissolve the soluble divalent mercury. Metals smelting operations favor the production of elemental mercury. Much of the Hg is released from small-scale activities in rather remote areas, and therefore the activity levels are quite uncertain. Also, emissions test data for Chinese sources are lacking, causing uncertainties in Hg emission factors and removal efficiencies. Overall, we calculate an uncertainty level of ±44% (95% confidence interval) in the estimate of total emissions. We recommend field testing of coal combustors and smelters in China to improve the accuracy of these estimates.     

The application of regenerable sorbents for mercury capture in gas phase

Mercury is a well-known toxic element, and flue gas streams emitted from coal-fired utilities are one of the largest anthropogenic sources of this element. This study briefly reviews the proposed technologies for reducing mercury emissions from coal combustion, focusing on an emerging process which involves the use of regenerable sorbents and especially those loaded with noble metals. Among the mercury species formed during coal combustion, elemental mercury is the most difficult to remove from the flue gases due to its low reactivity and insolubility in water. The widespread interest in using regenerable sorbents with metals is due to their ability to retain elemental mercury. With this technology, not only can efficiencies of 100 % be reached in the retention of elemental mercury but also a way to avoid the generation of new wastes loaded with mercury. This study considers the main aspects that must be taken into account when developing effective regenerable sorbents for mercury capture, with special attention to sorbents containing noble metals. The characteristics of this process are compared with those of other processes in a more advanced state of development.     

Mercury emission from coal-fired power plants in Poland

The paper reviews the current state of knowledge regarding sources of mercury emission in Poland. Due to the large quantities of coal burned at present, as well as taking into account existing reserves, coal remains the main energy source of energy in Poland. The data on coal consumption in Poland in the past, at present and in the future are discussed in the paper. Information on the content of mercury in Polish coals is presented.Coal combustion processes for electricity and heat production are the main source of anthropogenic mercury emission in Poland. It is expected that the current emissions will decrease in the future due to implementation of efficient control measures. These measures for emission reduction are described in the paper. Results of estimated mercury emission from coal-fired power station situated in the Upper Silesia Region, Poland are investigated. A relationship between mercury emission to the air and the mercury content in the consumed coal in power station equipped with the electrostatic precipitators (ESPs) is discussed.     

我国氮氧化物排放因子的修正和排放量计算:2000年

根据我国城市的发展状况 ,采用城市分类的方法 ,将我国 2 6 1个地级市按照人口数量分为 5个类别。每类城市选取一个典型城市进行实地调查 ,对我国燃烧锅炉和机动车的NOx 的排放因子进行了修正 ,提出了适合我国目前排放水平的各类城市的固定源和移动源的排放因子。并依据 2 0 0 0年中国大陆地区的电站锅炉、工业锅炉和民用炉具的燃料消耗量和机动车保有量 ,以地级市为基本单位 ,估算了 2 0 0 0年我国各地区的NOx 排放量 ,分析了分地区、分行业、分燃料类型的NOx 排放特征。 2 0 0 0年我国NOx 排放总量为 11.12Mt,其中固定源占 6 0 .8% ;移动源占 39.2 %。NOx 排放在地域、行业和燃料类型上分布均不平衡。NOx 的排放主要集中在华东和华北地区 ,其排放量占全国排放量的一半以上。燃煤为最重要的NOx 排放源 ,其排放量占燃料型NOx 排放量的 72 .3%左右。     

Active methods of mercury removal from flue gases

Due to its adverse impact on health, as well as its global distribution, long atmospheric lifetime and propensity for deposition in the aquatic environment and in living tissue, the US Environmental Protection Agency (US EPA) has classified mercury and its compounds as a severe air quality threat. Such widespread presence of mercury in the environment originates from both natural and anthropogenic sources. Global anthropogenic emission of mercury is evaluated at 2000 Mg year⁻¹. According to the National Centre for Emissions Management (Pol. KOBiZE) report for 2014, Polish annual mercury emissions amount to approximately 10 Mg. Over 90% of mercury emissions in Poland originate from combustion of coal.

The purpose of this paper was to understand mercury behaviour during sub-bituminous coal and lignite combustion for flue gas purification in terms of reduction of emissions by active methods. The average mercury content in Polish sub-bituminous coal and lignite was 103.7 and 443.5 μg kg⁻¹. The concentration of mercury in flue gases emitted into the atmosphere was 5.3 μg m⁻³ for sub-bituminous coal and 17.5 μg m⁻³ for lignite. The study analysed six low-cost sorbents with the average achieved efficiency of mercury removal from 30.6 to 92.9% for sub-bituminous coal and 22.8 to 80.3% for lignite combustion. Also, the effect of coke dust grain size was examined for mercury sorptive properties. The fine fraction of coke dust (CD) adsorbed within 243–277 μg Hg kg⁻¹, while the largest fraction at only 95 μg Hg kg⁻¹. The CD fraction < 0.063 mm removed almost 92% of mercury during coal combustion, so the concentration of mercury in flue gas decreased from 5.3 to 0.4 μg Hg m⁻³. The same fraction of CD had removed 93% of mercury from lignite flue gas by reducing the concentration of mercury in the flow from 17.6 to 1.2 μg Hg m⁻³. The publication also presents the impact of photochemical oxidation of mercury on the effectiveness of Hg vapour removal during combustion of lignite. After physical oxidation of Hg in the flue gas, its effectiveness has increased twofold.

     

Anthropogenic mercury emission inventory with emission factors and total emission in Korea

Mercury emissions concentrations, emission factors, and the total national emission from major anthropogenic sources in Korea for the year 2007 were estimated. Uncontrolled and controlled mercury emission factors and the total emission from each source types are presented. The annual national mercury emission from major anthropogenic sources for the year 2007, on average was 12.8 ton which ranged from 6.5 to 20.2 ton. Averaged emissions of elemental, oxidized, and particulate mercury were estimated at 8.25 ton, 3.69 ton, and 0.87 ton, respectively. Due to the removal of a major portion of particulate and oxidized mercury species, elemental mercury was dominant in stack emission. About 54.8% of mercury emission was contributed by industrial sources, 45.0% by stationary combustion sources and 0.02% by mobile sources. Thermal power plants, oil refineries, cement kilns and incinerators (municipal, industrial, medical, sewage sludge) were the major mercury emitters, contributing about 26%, 25%, 21% and 20%, respectively to the total mercury emission. Other sources (crematory, pulp and paper manufacturing, nonferrous metals manufacturing, glass manufacturing) contributed about 8% of the total emission. Priority should be given in controlling mercury emissions from coal-fired power plants, oil refineries, cement kilns and waste incinerators. More measurements including natural and re-emission sources are to be carried out in the future in order to have a clear scenario of mercury emission from the country and to apply effective control measures.     

Estimates of global anthropogenic methane emissions 1860–1993

This paper provides the first time series estimates of global anthropogenic methane emissions from the mid-19th century to the present. Our purpose is to provide time series estimates of anthropogenic methane emissions for global climate models estimated or calibrated using historical time series data. Previous estimates of methane emissions include “top-down” (deconvolution) estimates of total emissions, estimates of global anthropogenic emissions for the 16th century, and various estimates of anthropogenic and natural emissions in the 1980s and 1990s. This study uses previously published point estimates for the 16th century and the 1980s and early 1990s and a variety of historical time series of proxy variables to estimate a time series of global anthropogenic methane emissions. We find that anthropogenic methane emissions have increased from about 80 million tonnes per annum in 1860 to about 380 million tonnes in 1990. The relative importance of various emission sources changes over time. The rate of increase now may be slowing. A comparison with the estimates generated by Khalil and Rasmussen suggests that natural sources of methane have declined over the period. There are, however, great uncertainties in these estimates which future research may be able to reduce.     

Trends in anthropogenic mercury emissions estimated for South Africa during 2000–2006

Recent studies suggest an increase in mercury (Hg) emissions to the global environment, particularly as a result of anthropogenic activities. This has prompted many countries to complete Hg emission inventories, based on country-specific Hg sources. In this study, information on annual coal consumption and Hg-containing commodities produced in South Africa, was used to estimate Hg emissions during 2000–2006. Based on the information, the UNEP toolkit was used to estimate the amount of Hg released to air and general waste from each activity; using South Africa specific and toolkit based emission factors. In both atmospheric and solid waste releases, coal-fired power plants were estimated to be the largest contributors of Hg emissions, viz. 27.1 to 38.9 tonnes y^?1 in air, and 5.8 to 7.4 tonnes y^?1 in waste. Cement production was estimated to be the second largest atmospheric Hg emission contributor (2.2–3.9 tonnes y^?1), while coal gasification was estimated to be the second largest Hg contributor in terms of general waste releases (2.9–4.2 tonnes y^?1). Overall, there was an increase in total atmospheric Hg emissions from all activities, estimated at ca. 34 tonnes in 2000, to 50 tonnes in 2006, with some fluctuations between the years. Similarly, the total Hg emissions released to general waste was estimated to be 9 tonnes in 2000, with an increase to 12 tonnes in 2006.     

Fine Particulate Matter Emissions Inventories: Comparisons of Emissions Estimates with Observations from Recent Field Programs

Abstract

Emissions inventories of fine particulate matter (PM_2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM_2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM_2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5–20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM_2.5 are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM_2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.     

Fine particulate matter emissions inventories: comparisons of emissions estimates with observations from recent field programs

Emissions inventories of fine particulate matter (PM2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5-20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM2.s are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.     

Modeling of mercury emission,transport and deposition in North America

Most studies on the atmospheric behaviour of mercury in North America have excluded a detailed treatment of natural mercury emissions. The objective of this work is to report a detailed simulation of the atmospheric mercury in a domain that covers a significant part of North America and includes not only anthropogenic mercury emissions but also those from natural sources including vegetation, soil and water.The simulations were done using a natural mercury emission model coupled with the US EPA's SMOKE/CMAQ modelling system. The domain contained 132×90 grid cells at a resolution of 36 km, covering the continental United States, and major parts of Canada and Mexico. The simulation was carried out for 2002, using boundary conditions from a global mercury model. Estimated total natural mercury emission in the domain was 230 tonnes (1 tonne=1000 kg) and the ratio of natural to anthropogenic emissions varied from 0.7 in January to 3.2 in July. Average total gaseous mercury (TGM) concentration ranged between 1 and 4 ng m⁻³. Good agreement was found between the modelled results and measurements at three Ontario sites for ambient mercury concentrations, and at 72 mercury deposition network sites in the domain for wet deposition. The correlation coefficient between the simulated and the measured values of the daily average TGM at three monitoring sites varied between 0.48 and 0.64. When natural emissions were omitted, the correlation coefficients dropped to between 0.15 and 0.40. About 335 tonnes of mercury were deposited in the domain during the simulation period but overall, it acted as a net source of mercury and contributed about 21 tonnes to the global pool. The net deposition of mercury to the Great Lakes was estimated to be about 2.4 tonnes. The estimated deposition values were similar to those reported by other researchers.     

Studies of potential sources that contributed to atmospheric mercury in Toronto,Canada

This study identified sources of mercury (Hg) in downtown Toronto, Canada by analyzing gaseous elemental mercury (GEM), mercury associated with particles with sizes less than 2.5 microns (PHg < 2.5), and gaseous oxidized inorganic mercury (GOIM), commonly referred to as reactive gaseous mercury (RGM), and air pollutants (CO, NO_x, O₃, PM_2.5, SO₂) concentrations between Dec 2003 and Nov 2004. The data were analyzed using Positive Matrix Factorization (PMF) model, Principal Components Analysis (PCA), ratio analysis, back trajectories, and correlation analyses. The analyses suggest industrial sources (chemical production, metal production, sewage treatment), rather than coal combustion, were the major contributors to measured Hg levels. Overlap in source profiles for the Hg sources listed in the Canadian National Pollutant Release Inventory (NPRI) and lack of source profiles for urban sources were the major limitations to positively identifying sources from the PMF and PCA factors. Correlation analyses revealed direct emissions were the sources of GOIM in spring, summer, and fall, and the occurrence of GEM oxidation by ozone in the summer. Elevated Hg events are attributed to emissions from urban sources near the sampling site, regional point sources, and photochemical processes involving ozone.     

Uncertainties in current estimates of emissions of ammonia in the United Kingdom

Estimates of the emissions of ammonia have previously concentrated on animal husbandry sources from agricultural systems. Animal husbandry sources still constitute the major fraction of emissions of ammonia, but we have also considered the potential magnitude of other 'minor' sources, which may include coal combustion, waste incineration, road vehicles, sewage treatment plants, fertiliser manufacture and application, vegetation senescence and crop emissions, domestic pets, and human sources. Where possible, a provisional estimate of UK emissions from each of these sources is given. It is concluded that the potential magnitude of emissions from these 'minor' sources may make a significant contribution to the total emissions of ammonia to the atmosphere. On the basis of the available data, and the application of a range of emission factors to the UK situation, an additional annual emission potential lying in the range of approximately 80-140 ktonne year(-1) over and above that from animal husbandry has been calculated. The uncertainties in the emission estimates and instances in which a better resolution of sources is required are discussed. The emission factors used for animals in various inventories are reviewed and applied to the main UK agricultural animal populations. By using this approach, estimates of emissions from these sources range between 113 and 647 ktonne year(-1), which illustrates the uncertainties involved. It is suggested that our knowledge of the sources of ammonia, and their distribution, is far from complete.     

The emissions of heavy metals and persistent organic pollutants from modern coal-fired power stations

Extensive research for establishing the emissions of heavy metals from coal-fired power stations is performed in the Netherlands for the past 25 years. In the Netherlands coal is fired from all over the world. This means that the emissions are established for coal of various origins. In the eighties, the emissions of installations equipped with ESPs (electrostatic precipitators) were measured. In the nineties, the influence of wet FGD (flue gas desulphurisation) on the emissions was studied. The effect of co-combustion of biomass and other secondary fuels is the main item for the last 10 years.Fifty-five elements were measured in the solid state and eight elements in the gaseous phase. It appeared that at low particulate concentration the influence of calcium containing evaporated water droplets downstream the wet FGD on the emissions of heavy metals is bigger than the composition of the coal. Also it appeared that at modern coal-fired power stations the emissions are hardly influenced by co-combustion of biomass. All the results are used for modelling, resulting in the KEMA TRACE MODEL^®, by which the emissions can be predicted. The established emission factors are for most elements in good agreement with literature values for comparable modern installations.Persistence organic pollutants (POPs) that were detected in the flue gases of coal-fired power stations are polycyclic aromatic hydrocarbons (PAH) and dioxins/furans. Measurements during full coal-firing and during co-firing of biomass have indicated that these emissions are negligible.     

Estimation of heavy metal emission fluxes on the territory of the NIS

As the result of our research, the specific procedures to use emission factor methodology were developed and applied for trace metal emission evaluation into the atmosphere over the territory of the former Soviet Union. The existing data on heavy metal emissions were revised as background information from official sources and expert estimations. Source categories and different initial information as well as the concept of spatial emission distribution were defined and observed. The calculated atmospheric emissions of lead, cadmium and mercury were produced among the main source categories of 12 NIS countries for 1990, 1995 and 1997, using modified emission coefficients.Total cadmium emissions into the atmosphere from determined source categories were estimated as 388.4 tonnes in 1990 for the whole domain with reduction by up to 207.0 tonnes per year for 1997. Mercury emissions were estimated as equal to 303.2 tonnes in 1990 and 159.8 tonnes in 1997. Lead emission amounted to 24903.0 tonnes in 1990, and 9652.5 tonnes in 1997.The results of the evaluation demonstrated the general trends of atmospheric heavy metal emissions with a greater decrease during the first half of the 1990s followed later by the rather stable level to be explained by recession in industrial activity and fuel consumption in NIS in that period. The significant spatial variations of atmospheric emissions over vast territories are described based on the results of their distribution according to 1×1 degree grid with remarkably higher values in the location of industrial cities.     

Remote SO2 Mass Flux Measurements Using COSPEC

During the intensive Nanticoke Environmental Field Study of May/June 1978, three Barringer Correlation Spectrometers (COSPEC) were employed to obtain remote sensing estimates of sulfur dioxide emissions from a coal fired hydroelectric generating station. The results from about one hundred half-hourly sampling periods shows that the COSPEC derived estimate is within 7% of those computed by the utility. The sources of the variance in the COSPEC flux estimate are examined and sampling recommendations regarding the use of COSPEC for this purpose are made.