Emissions of sulfur trioxide from coal-fired power plants

Emissions of sulfur trioxide (SO3) are a key component of plume opacity and acid deposition. Consequently, these emissions need to be low enough to not cause opacity violations and acid deposition. Generally, a small fraction of sulfur (S) in coal is converted to SO3 in coal-fired combustion devices such as electric utility boilers. The emissions of SO3 from such a boiler depend on coal S content, combustion conditions, flue gas characteristics, and air pollution devices being used. It is well known that the catalyst used in the selective catalytic reduction (SCR) technology for nitrogen oxides control oxidizes a small fraction of sulfur dioxide in the flue gas to SO3. The extent of this oxidation depends on the catalyst formulation and SCR operating conditions. Gas-phase SO3 and sulfuric acid, on being quenched in plant equipment (e.g., air preheater and wet scrubber), result in fine acidic mist, which can cause increased plume opacity and undesirable emissions. Recently, such effects have been observed at plants firing high-S coal and equipped with SCR systems and wet scrubbers. This paper investigates the factors that affect acidic mist production in coal-fired electric utility boilers and discusses approaches for mitigating emission of this mist.     

Emissions of Sulfur Trioxide from Coal-Fired Power Plants

Abstract

Emissions of sulfur trioxide (SO₃) are a key component of plume opacity and acid deposition. Consequently, these emissions need to be low enough to not cause opacity violations and acid deposition. Generally, a small fraction of sulfur (S) in coal is converted to SO₃ in coal-fired combustion devices such as electric utility boilers. The emissions of SO₃ from such a boiler depend on coal S content, combustion conditions, flue gas characteristics, and air pollution devices being used. It is well known that the catalyst used in the selective catalytic reduction (SCR) technology for nitrogen oxides control oxidizes a small fraction of sulfur dioxide in the flue gas to SO₃. The extent of this oxidation depends on the catalyst formulation and SCR operating conditions. Gas-phase SO₃ and sulfuric acid, on being quenched in plant equipment (e.g., air preheater and wet scrubber), result in fine acidic mist, which can cause increased plume opacity and undesirable emissions. Recently, such effects have been observed at plants firing high-S coal and equipped with SCR systems and wet scrubbers. This paper investigates the factors that affect acidic mist production in coal-fired electric utility boilers and discusses approaches for mitigating emission of this mist.     

Emissions and risks associated with oxyfuel combustion: State of the science and critical data gaps

Oxyfuel combustion is a promising technology that may greatly facilitate carbon capture and sequestration by increasing the relative CO₂ content of the combustion emission stream. However, the potential effect of enhanced oxygen combustion conditions on emissions of criteria and hazardous air pollutants (e.g., acid gases, particulates, metals and organics) is not well studied. It is possible that combustion under oxyfuel conditions could produce emissions posing different risks than those currently being managed by the power industry (e.g., by changing the valence state of metals). The data available for addressing these concerns are quite limited and are typically derived from laboratory-scale or pilot-scale tests. A review of the available data does suggest that oxyfuel combustion may decrease the air emissions of some pollutants (e.g., SO₂, NOx, particulates) whereas data for other pollutants are too limited to draw any conclusions. The oxy-combustion systems that have been proposed to date do not have a conventional “stack” and combustion flue gas is treated in such a way that solid or liquid waste streams are the major outputs. Use of this technology will therefore shift emissions from air to solid or liquid waste streams, but the risk management implications of this potential change have yet to be assessed. Truly useful studies of the potential effects of oxyfuel combustion on power plant emissions will require construction of integrated systems containing a combustion system coupled to a CO₂ processing unit. Sampling and analysis to assess potential emission effects should be an essential part of integrated system tests.

Implications: Oxyfuel combustion may facilitate carbon capture and sequestration by increasing the relative CO₂ content of the combustion emission stream. However, the potential effect of enhanced oxygen combustion conditions on emissions of criteria and hazardous air pollutants has not been well studied. Combustion under oxyfuel conditions could produce emissions posing different risks than those currently being managed by the power industry. Therefore, before moving further with oxyfuel combustion as a new technology, it is appropriate to summarize the current understanding of potential emissions risk and to identify data gaps as priorities for future research.     

Evaluating Sources of Indoor Air Pollution

Evaluation of Indoor air pollution problems requires an understanding of the relationship between sources, air movement, and outdoor air exchange. Research is underway to investigate these relationships. A three-phase program is being implemented: 1) Environmental chambers are used to provide source emission factors for specific indoor pollutants; 2) An IAQ (Indoor Air Quality) model has been developed to calculate indoor pollutant concentrations based on chamber emissions data and the air exchange and air movement within the indoor environment; and 3) An IAQ test house is used to conduct experiments to evaluate the model results. Examples are provided to show how this coordinated approach can be used to evaluate specific sources of indoor air pollution. Two sources are examined: 1) para-dichlorobenzene emissions from solid moth repellant; and 2) particle emissions from unvented kerosene heaters.

The evaluation process for both sources followed the three-phase approach discussed above. Para-dichlorobenzene emission factors were determined by small chamber testing at EPA’s Air and Energy Engineering Research Laboratory. Particle emission factors for the kerosene heaters were developed In large chambers at the J. B. Pierce Foundation Laboratory. Both sources were subsequently evaluated in EPA’s IAQ test house. The IAQ model predictions showed good agreement with the test house measurements when appropriate values were provided for source emissions, outside air exchange, in-house air movement, and deposition on “sink” surfaces.     

Evaluating sources of indoor air pollution

Evaluation of indoor air pollution problems requires an understanding of the relationship between sources, air movement, and outdoor air exchange. Research is underway to investigate these relationships. A three-phase program is being implemented: 1) Environmental chambers are used to provide source emission factors for specific indoor pollutants; 2) An IAQ (Indoor Air Quality) model has been developed to calculate indoor pollutant concentrations based on chamber emissions data and the air exchange and air movement within the indoor environment; and 3) An IAQ test house is used to conduct experiments to evaluate the model results. Examples are provided to show how this coordinated approach can be used to evaluate specific sources of indoor air pollution. Two sources are examined: 1) para-dichlorobenzene emissions from solid moth repellant; and 2) particle emissions from unvented kerosene heaters. The evaluation process for both sources followed the three-phase approach discussed above. Para-dichlorobenzene emission factors were determined by small chamber testing at EPA's Air and Energy Engineering Research Laboratory. Particle emission factors for the kerosene heaters were developed in large chambers at the J. B. Pierce Foundation Laboratory. Both sources were subsequently evaluated in EPA's IAQ test house. The IAQ model predictions showed good agreement with the test house measurements when appropriate values were provided for source emissions, outside air exchange, in-house air movement, and deposition on "sink" surfaces.     

Hazardous air pollutant emissions from gas-fired combustion sources: emissions and the effects of design and fuel type

Air emissions from gas-fired combustion devices such as boilers, process heaters, gas turbines and stationary reciprocating engines contain hazardous air pollutants (HAPs) subjected to consideration under the federal clean air act (CAA). This work presents a recently completed major research project to develop an understanding of HAP emissions from gas-fired boilers and process heaters and new HAP emission factors based on field emission tests of gas-fired external combustion devices used in the petroleum industry. The effect of combustion system design and operating parameters on HAP emissions determined by both field and research tests are discussed. Data from field tests of gas-fired petroleum industry boilers and heaters generally show very low emission levels of organic HAPs. A comparison of the emission data for boilers and process heaters, including units with and without various forms of NOx emission controls, showed no significant difference in organic HAP emission characteristics due to process or burner design. This conclusion is also supported by the results of research tests with different burner designs. Based on field tests of units fired with natural gas and various petroleum industry process gases and research tests in which gas composition was intentionally varied, organic HAP emissions were not determined to be significantly affected by the gas composition. Research data indicate that elevated organic HAP emission levels are found only under extreme operating conditions (starved air or high excess air combustion) associated with poor combustion.     

Real-world vehicle emissions: a summary of the twelfth Coordinating Research Council On-Road Vehicle Emissions Workshop

The Coordinating Research Council (CRC) held its 12th workshop in April 2002, with nearly 90 presentations on the most recent on-road vehicle emissions research. This paper summarizes the presentations from researchers who are engaged in improving understanding of the contribution of mobile sources to air quality. Participants in the workshop discussed mobile source emission models and emission inventories, results from gas- and particle-phase emissions studies from spark-ignition and diesel-powered vehicles (with an emphasis in this workshop on particle emissions), effects of fuels on emissions, evaluation of in-use emissions control programs, and efforts to improve our capabilities in performing on-board emissions measurements, as well as topics for future research.     

Trend of vehicle emission levels until 2020 – Prognosis based on current vehicle measurements and future emission legislation

The paper describes the incorporation of actual emission measurements and future emission standards into the emission model ‘NEMO’ (Network Emission Model). This model is then applied to make predictions on vehicle emission levels on basis of the Austrian fleet composition until 2020. The output is compared to the results based on the most common emission tool for the calculation of vehicle emissions in Central Europe – the recent version (2.1) of the ‘Handbook Emission Factors for Road Transport’. The discussion is focused on NO_x and particulate matter (PM), since these pollutants are considered to be the most critical for the local air quality level.The NO_x emission levels of recent modern diesel vehicle generations observed in several real world driving conditions were observed to be clearly higher than demanded in the type approval procedure. Due to the growing number of modern diesel engine concepts equipped with coated catalytic exhaust after treatment, the fraction of NO₂ of the total tailpipe NO_x emissions is predicted to continue to increase in the next few years. Bearing in mind the upcoming tightening of the NO₂ air quality limits and the steady increase of traffic volumes, excesses of the NO₂ air quality limits at roadside locations have to be expected to an increasing extent for the beginning of the next decade. The issue of particle emissions originated from the diesel engine combustion process can be regarded as being technically solved due to the extensive introduction of diesel particle filters in the vehicle fleet if these systems will prove a high efficiency over the entire vehicle life in real world operation conditions. However, PM emissions from road transport will continue to be in the focus of public attention due to particle emissions caused by dust re-suspension and abrasion processes.     

The influence of meteorological conditions and stringent emission control on high TSP episodes in istanbul

Istanbul has faced serious air pollution problems since the mid-80s. This is mainly due to particulate air pollution coming from poor quality lignite in areas, which are heavily populated and industrialized. As a consequence of severe air pollution problems, stringent control on the emissions in the city started in the year of 1994. In this work, in order to study the relationship between emissions and meteorological conditions, an assessment of air pollution episodes and air pollution potential in the city is presented for the terms at the changed emission schedule as the influence of an emission reduction strategy. The influence of meteorological conditions on the TSP (total suspended particulates) levels is considered for two consecutive winter periods. On this occasion, the city has faced different TSP levels and episode characteristics depending on stringent emission reductions covering the banned, poor-quality lignite and fuel switching. For this purpose, climatological conditions and air quality analyses were performed.     

Characterization of In-Use Light-Duty Gasoline Vehicle Emissions by Remote Sensing in Beijing: Impact of Recent Control Measures

Abstract

China’s national government and Beijing city authorities have adopted additional control measures to reduce the negative impact of vehicle emissions on Beijing’s air quality. An evaluation of the effectiveness of these measures may provide guidance for future vehicle emission control strategy development. In-use emissions from light-duty gasoline vehicles (LDGVs) were investigated at five sites in Beijing with remote sensing instrumentation. Distance-based mass emission factors were derived with fuel consumption modeled on real world data. The results show that the recently implemented aggressive control strategies are significantly reducing the emissions of on-road vehicles. Older vehicles are contributing substantially to the total fleet emissions. An earlier program to retrofit pre-Euro cars with three-way catalysts produced little emission reduction. The impact of model year and driving conditions on the average mass emission factors indicates that the durability of vehicles emission controls may be inadequate in Beijing.     

Nitrogen oxides emission control options for coal-fired electric utility boilers

Recent regulations have required reductions in emissions of nitrogen oxides (NOx) from electric utility boilers. To comply with these regulatory requirements, it is increasingly important to implement state-of-the-art NOx control technologies on coal-fired utility boilers. This paper reviews NOx control options for these boilers. It discusses the established commercial primary and secondary control technologies and examines what is being done to use them more effectively. Furthermore, the paper discusses recent developments in NOx controls. The popular primary control technologies in use in the United States are low-NOx burners and overfire air. Data reflect that average NOx reductions for specific primary controls have ranged from 35% to 63% from 1995 emissions levels. The secondary NOx control technologies applied on U.S. coal-fired utility boilers include reburning, selective noncatalytic reduction (SNCR), and selective catalytic reduction (SCR). Thirty-six U.S. coal-fired utility boilers have installed SNCR, and reported NOx reductions achieved at these applications ranged from 15% to 66%. Recently, SCR has been installed at >150 U.S. coal-fired utility boilers. Data on the performance of 20 SCR systems operating in the United States with low-NOx emissions reflect that in 2003, these units achieved NOx emission rates between 0.04 and 0.07 lb/10(6) Btu.     

Black carbon emissions in China

Black carbon (BC) is an important aerosol species because of its global and regional influence on radiative forcing and its local effects on the environment and human health. We have estimated the emissions of BC in China, where roughly one-fourth of global anthropogenic emissions is believed to originate. China's high rates of usage of coal and biofuels are primarily responsible for high BC emissions. This paper pays particular attention to the application of appropriate emission factors for China and the attenuation of these emissions where control devices are used. Nevertheless, because of the high degree of uncertainty associated with BC emission factors, we provide ranges of uncertainty for our emission estimates, which are approximately a factor of eight. In our central case, we calculate that BC emissions in China in 1995 were 1342 Gg, about 83% being generated by the residential combustion of coal and biofuels. We estimate that BC emissions could fall to 1224 Gg by 2020. This 9% decrease in BC emissions can be contrasted with the expected increase of 50% in energy use; the reduction will be obtained because of a transition to more advanced technology, including greater use of coal briquettes in place of raw coal in cities and towns. The increased use of diesel vehicles in the future will result in a greater share of the transport sector in total BC emissions. Spatially, BC emissions are predominantly distributed in an east–west swath across China's heartland, where the rural use of coal and biofuels for cooking and heating is widespread. This is in contrast to the emissions of most other anthropogenically derived air pollutants, which are closely tied to population and industrial centers.     

Real-world vehicle emissions: A summary of the 15th coordinating research council on-road vehicle emissions workshop

The Coordinating Research Council held its 15th workshop in April 2005, with nearly 90 presentations describing the most recent mobile source-related emissions research. In this paper, the authors summarize the presentations from researchers who are engaged in improving our understanding of the contribution of mobile sources to air quality. Participants in the workshop discussed emission models and emission inventories, results from gas- and particle-phase emissions studies from spark-ignition and diesel-powered vehicles (with an emphasis in this workshop on particle emissions), effects of fuels on emissions, evaluation of in-use emissions control programs, and efforts to improve our capabilities in performing on-board emissions measurements, as well as topics for future research.     

The impact of transportation control measures on emission reductions during the 2008 Olympic Games in Beijing,China

Traffic congestion and air pollution were two major challenges for the planners of the 2008 Olympic Games in Beijing. The Beijing municipal government implemented a package of temporary transportation control measures during the event. In this paper, we report the results of a recent research project that investigated the effects of these measures on urban motor vehicle emissions in Beijing. Bottom–up methodology has been used to develop grid-based emission inventories with micro-scale vehicle activities and speed-dependent emission factors. The urban traffic emissions of volatile organic compounds (VOC), carbon monoxide (CO), nitrogen oxides (NO_x) and particulate matter with an aerodynamic diameter of 10 μm or less (PM₁₀) during the 2008 Olympics were reduced by 55.5%, 56.8%, 45.7% and 51.6%, respectively, as compared to the grid-based emission inventory before the Olympics. Emission intensity was derived from curbside air quality monitoring at the North 4th Ring Road site, located about 7 km from the National Stadium. Comparison between the emission intensity before and during the 2008 Olympics shows a reduction of 44.5% and 49.0% in daily CO and NO_x emission from motor vehicles. The results suggest that reasonable traffic system improvement strategies along with vehicle technology improvements can contribute to controlling total motor vehicle emissions in Beijing after the Olympic Games.     

The Impact of Particulate Emissions Control On the Control of Other MWC Air Emissions

On December 20, 1989, the Environmental Protection Agency (EPA) proposed revised new source performance standards for new municipal waste combustion (MWC) units and guidelines for existing sources. The proposed national regulations require tighter particulate matter control and address pre-combustion, combustion, and post-combustion controls, the latter two depending on capacity and age of the facility.

The air pollutants of concern when municipal solid waste (MSW) is burned will be discussed. Generally, particulate control is an inherent part of the systems used to limit the emissions of these air pollutants. The relationships between MWC air emissions (acid gases, trace organics, and trace heavy metals) control and particulate control will be discussed. Test results to quantify air pollutant emissions from MWC units and their control will be presented and compared with the proposed regulations.     

Gas-phase and semivolatile organic emissions from a modern nonroad diesel engine equipped with advanced aftertreatment

ABSTRACT

U.S. Tier 4 Final and Euro Stage IV and V regulations for nonroad compression-ignition engines have led to the development of exhaust aftertreatment technologies optimized for nonroad engines and duty cycles. In this study, several aftertreatment configurations consisting of state-of-the-art diesel oxidation catalysts (DOCs), diesel particulate filters (DPFs), copper (Cu) zeolite– and vanadium-based selective catalytic reduction (SCR) catalysts, and ammonia oxidation (AMOX) catalysts are evaluated using both nonroad transient (NRTC) and steady (8-mode NRSC) cycles in order to understand both component- and system-level effects of diesel aftertreatment on gas-phase, semivolatile, and particle-phase and particle-bound unregulated organic emissions. Organic emissions reported in this work include total hydrocarbon (THC), n-alkanes, branched alkanes, saturated cycloalkanes, aromatics, aldehydes, ketones, hopanes, steranes, and soluble organic fraction (SOF). Brake-specific emissions are reported for four configurations, including engine-out, DOC+CuZ-SCR+AMOX, V-SCR+AMOX, and DOC+DPF+CuZ-SCR+AMOX, and conversion of engine-out emissions is reported for the three aftertreatment configurations. Mechanisms responsible for the reduction of organic species are discussed in detail. This summary of emissions from a current nonroad diesel engine equipped with advanced aftertreatment can be used to more accurately model the impact of anthropogenic emissions on the atmosphere with tools such as the U.S. Environmental Protection Agency’s Motor Vehicle Emissions Simulator (MOVES2014a) model.

Implications: Anthropogenic emissions are a source of significant human health and environmental risk. This study, focused on the treatment of exhaust emissions from a modern nonroad diesel engine with a variety of aftertreatment configurations, examines the impact that human industrial activity can have on air pollution. In particular, we focus on the remediation of gas-phase and semivolatile organic emissions by emission reduction technologies. This detailed summary of emissions from a current nonroad diesel engine equipped with advanced aftertreatment can be used to more accurately model the impact of anthropogenic emissions on the atmosphere with tools such as the U.S. Environmental Protection Agency’s MOVES2014a model.     

Characterization of in-use light-duty gasoline vehicle emissions by remote sensing in Beijing: impact of recent control measures

China's national government and Beijing city authorities have adopted additional control measures to reduce the negative impact of vehicle emissions on Beijing's air quality. An evaluation of the effectiveness of these measures may provide guidance for future vehicle emission control strategy development. In-use emissions from light-duty gasoline vehicles (LDGVs) were investigated at five sites in Beijing with remote sensing instrumentation. Distance-based mass emission factors were derived with fuel consumption modeled on real world data. The results show that the recently implemented aggressive control strategies are significantly reducing the emissions of on-road vehicles. Older vehicles are contributing substantially to the total fleet emissions. An earlier program to retrofit pre-Euro cars with three-way catalysts produced little emission reduction. The impact of model year and driving conditions on the average mass emission factors indicates that the durability of vehicles emission controls may be inadequate in Beijing.     

Emissions profile from new and in-use handheld, 2-stroke engines

The objective of this study was to characterize exhaust emissions from a series of handheld, 2-stroke small engines. A total of 23 new and used engines from model years 1981–2003 were studied; these engines spanned three phases of emission control (pre-control, phase-1, phase-2). Measured emissions included carbon monoxide (CO), carbon dioxide (CO₂), nitrogen oxides (NO_x), hydrocarbons (HC), fine particulate matter (PM_2.5), and sulfur dioxide (SO₂). Emissions reductions in CO (78%) and HC (52%) were significant between pre-control and phase-2 engines. These reductions can be attributed to improvements in engine design, reduced scavenging losses, and implementation of catalytic exhaust control. Total hydrocarbon emissions were strongly correlated with fuel consumption rates, indicating varying degrees of scavenging losses during the intake/exhaust stroke. The use of a reformulated gasoline containing 10% ethanol resulted in a 15% decrease in HC and a 29% decrease in CO emissions, on average. Increasing oil content of 2-stroke engine fuels results in a substantial increase of PM_2.5 emissions as well as smaller increases in HC and CO emissions. Results from this study enhance existing emission inventories and appear to validate predicted improvements to ambient air quality through implementation of new phase-2 handheld emission standards.     

Evaluation of total volatile organic compound emissions from adhesives based on chamber tests

In 1997, Homeswest in western Australia and Murdoch University developed a project to construct low-allergen houses (LAHs) in a newly developed suburb. Before the construction of LAHs, all potential volatile organic compound (VOC) emission materials used in LAHs are required to be measured to ensure that they are low total VOC (TVOC) emission materials. This program was developed based on this purpose. In recent times, the number of complaints about indoor air pollution caused by VOCs has increased. A number of surveys of indoor VOCs have indicated that many indoor materials contribute to indoor air pollution. Although some studies have been conducted on the characteristics of VOC emissions from adhesives, most of them were focused on VOC emissions from floor adhesives. Few measurements of VOC emissions from adhesives used for wood, fabrics, and leather are available. Furthermore, most research on VOC emissions from adhesives has been done in countries with cool climates, where ventilation rates in the indoor environment are lower than those in Mediterranean climates, due to energy conservation. VOCs emitted from adhesives have not been sufficiently researched to prepare an emission inventory to predict indoor air quality and to determine both exposure levels for the Australian population and the most appropriate strategies to reduce exposure. An environmental test chamber with controlled temperature, relative humidity, and airflow rate was used to evaluate emissions of TVOCs from three adhesives used frequently in Australia. The quantity of TVOC emissions was measured by a gas chromatography/flame ionization detector. The primary VOCs emitted from each adhesive were detected by gas chromatography/mass spectrometry. The temporal change of TVOC concentrations emitted from each adhesive was tested. A double-exponential equation was then developed to evaluate the characteristics of TVOC emissions from these three adhesives. With this double-exponential model, the physical processes of TVOC emissions can be explained, and a variety of emission parameters can be calculated. These emission parameters could be used to estimate real indoor TVOC concentrations in Mediterranean climates.     

A Comparison of Organic Emissions from Hazardous Waste Incinerators Versus the 1990 Toxics Release Inventory Air Releases

Incineration is often the preferred technology for disposing of hazardous waste and remediating Superfund sites. The effective implementation of this technology is frequently impeded by strong public opposition to hazardous waste incineration (HWI). One of the reasons cited for this opposition is the perception that the emission of organics pose an unreasonable threat to human health. While numerous risk assessments for these facilities have demonstrated that the risks from the inhalation of HWI emissions are very low, this has not totally allayed some of the concerns. In order to put organic emissions in perspective, the mass of these emissions from the incineration of hazardous waste on a national scale has been estimated using “reasonable worst-case” assumptions and compared to the 1990 Toxics Release Inventory (TRI) air releases. Comparisons were made for 15 carcinogenic organic compounds and 17 non-carcinogenic organic compounds. Ratios for all but one of these compound-specific HWI emissions to their corresponding TRI air releases ranged from 0.0003 to 0.678 percent. The total mass emissions (110.5 tons) of all 32 specific organics from HWIs was less than 0.03 percent of the corresponding 1990 TRI air releases (431,586 tons).