Application of the tracer-aerosol gradient interpretive technique to sulfur attribution for the big bend regional aerosol and visibility observational study

A simple data analysis method called the Tracer-Aerosol Gradient Interpretive Technique (TAGIT) is used to attribute particulate S and SO2 at Big Bend National Park in Texas and nearby areas to local and regional sources. Particulate S at Big Bend is of concern because of its effects on atmospheric visibility. The analysis used particulate S, SO2, and perfluorocarbon tracer data from six 6-hr sampling sites in and near Big Bend National Park. The data were collected in support of the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study; the field portion was conducted from July through October 1999. Perfluorocarbon tracer was released continuously from a tower at Eagle Pass, TX, approximately 25 km northeast of two large coal-fired power plants (Carbon I and II) in Coahuila, Mexico, and approximately 270 km east-southeast of Big Bend National Park. The perfluorocarbon tracer did not properly represent the location of the emissions from the Carbon power plants for individual 6-hr sampling periods and attributed only 3% of the particulate S and 27% of the SO2 at the 6-hr sites in and near Big Bend to sources represented by the tracer. An alternative approach using SO2 to tag "local" sources such as the Carbon plants attributed 10% of the particulate S and 75% of the SO2 at the 6-hr sites to local sources. Based on these two approaches, most of the regional (65-86%) and a small fraction (19-31%) of the local SO2 was converted to particulate S. The analysis implies that substantial reductions in particulate S at Big Bend National Park cannot be achieved by only reducing emissions from the Carbon power plants; reduction of emissions from many sources over a regional area would be necessary.     

Application of the Tracer-Aerosol Gradient Interpretive Technique to Sulfur Attribution for the Big Bend Regional Aerosol and Visibility Observational Study

Abstract

A simple data analysis method called the Tracer-Aerosol Gradient Interpretive Technique (TAGIT) is used to attribute particulate S and SO₂ at Big Bend National Park in Texas and nearby areas to local and regional sources. Particulate S at Big Bend is of concern because of its effects on atmospheric visibility. The analysis used particulate S, SO₂ , and perfluorocarbon tracer data from six 6-hr sampling sites in and near Big Bend National Park. The data were collected in support of the Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study; the field portion was conducted from July through October 1999. Perfluorocarbon tracer was released continuously from a tower at Eagle Pass, TX, approximately 25 km northeast of two large coal-fired power plants (Carbon I and II) in Coahuila, Mexico, and approximately 270 km east-southeast of Big Bend National Park.

The perfluorocarbon tracer did not properly represent the location of the emissions from the Carbon power plants for individual 6-hr sampling periods and attributed only 3% of the particulate S and 27% of the SO₂ at the 6-hr sites in and near Big Bend to sources represented by the tracer. An alternative approach using SO₂ to tag “local” sources such as the Carbon plants attributed 10% of the particulate S and 75% of the SO2 at the 6-hr sites to local sources. Based on these two approaches, most of the regional (65–86%) and a small fraction (19–31%) of the local SO₂ was converted to particulate S. The analysis implies that substantial reductions in particulate S at Big Bend National Park cannot be achieved by only reducing emissions from the Carbon power plants; reduction of emissions from many sources over a regional area would be necessary.     

Emissions from Burning Grass Stubble and Straw

The emissions from burning the residue following grass-seed harvest were determined by means of a combined laboratory-field study. Samples of the straw and stubble residue were burned in the laboratory burning tower at the University of California at Riverside. Complete analyses were determined for gaseous and particulate emissions for the important grass species from the Willamette Valley of Oregon. Particulate emissions averaged 15.6 lb/ton of fuel burned. Carbon monoxide averaged 101 lb/ton of fuel burned. Hydrocarbon emission averages, in pounds per ton of fuel burned, were 1.74 for saturates plus acetylene, 2.80 for defines, and 1.68 for ethylene. The NO_x emission, at the temperature peak during the burn, averaged 29.3 ppm. Field studies, conducted by personnel from Oregon State University, measured only particulate emissions, carbon dioxide, and temperature over the burn. The carbon dioxide values were found to be similar to those obtained on the burning table at UCR and it was therefore concluded that the other gaseous emissions were similar and could be used as reasonably accurate for emission inventories. The temperature values obtained in the laboratory and field were also similar and further justifies extrapolating the burning table data to field situations. The particulate matter collected in the field studies averaged 15.55 lb of particulate per ton of fuel burned. This is the same average obtained for the burning table data which again serves to validate the emissions reported from Riverside. Much more variability was found in the particulate emissions obtained in the field which reflects the wider range of environmental conditions encountered in the field.     

Combustion Mechanisms in Wood Fired Boilers

The emissions from combustion of wood residue fuel in an experimental spreader-stoker boiler were measured at the Fairplay Test Facility at Oregon State University. Stack gases were monitored to determine levels of excess air, opacity, and particulate loading. Particulate emissions were measured to determine the effects of underfire air flow rate and fuel bed depth on particulate carry over rate. An experiment conducted at four energy release rates and two fuel bed depths indicated that increased bed depth has the effect of reducing particulate emissions and that the effect increases as energy release rate increases. The experiment also showed increased energy release rate has the effect of increasing particulate emissions. The effects were found to be statistically significant.     

Current Technology for Continuous Monitoring of Particulate Emissions

Particulate matter is characterized by its physical and chemical properties. Federal and state emission standards identify two important physical properties, opacity (visible emissions) and particulate mass concentration. In addition, particle size and particle composition are characteristics that play a significant role in the assessment of health effects, visibility, and control strategy. Systems to monitor these particle characteristics are in various stages of development. Opacity monitors have the longest history of commercial availability and of applicability to various source emissions. Particulate mass monitors have a short history as commercially available systems and are under evaluation in various source applications. Particle size monitors are mainly in the advanced prototype development stage undergoing evaluation. Particle composition monitors are in the early stages of development as research prototypes. Real time size monitoring systems will eventually be wedded to real time particle composition analyzers to give a monitoring system for particle size distributions of chemical constituents.     

Reduction of Open Hearth Furnace Particulate Emissions via a Parametric Study

A linear relationship has been found between oxygen usage and particulate mass emission rate for a basic open hearth furnace. Particulate emissions were found to pass through a minimum at 50% hot metal addition to the furnace which also corresponded to minimum oxygen consumption. Number 2 dealer scrap and hot metal addition were found to have a secondary effect on the particulate emissions. Variation of number 2 dealer scrap from 0 to 15% of the charge and hot metal from 10 to 70% resulted in a maximum 44% increase in particulate emissions. Aerodynamic particle size distributions for all heats and within heats were relatively invariant with an average mass median diameter of 1.4µ     

Heavy Duty Diesel Particulate Emission Factors

For the past several years, EPA has been measuring particulate emissions from a variety of heavy-duty diesel engines through contracts with Southwest Research Institute. Particulate emissions samples have been collected using an exhaust splitter to divert a fraction of the engine exhaust into a standard dilution tunnel. A small fraction of the diluted exhaust from the tunnel is pulled through a filter from which particulate mass and, in some cases, organic content of the particulate is determined. This paper discusses the sampling system and gives particulate emission factors that have been computed from truck and bus fuel consumption data as well as average truck and bus speed data from New York and Los Angeles (freeway and nonfreeway usage). Average particulate emission test results (steady state tests) for 2-stroke engines were 4.74 g/kg fuel and for 4-stroke engines were 2.64 g/kg fuel. Using average particulate emissions results, a particulate emission factor range of 0.8 to 1.3 g/km was computed. Nationwide diesel particulate emissions were calculated to be 88,000 metric tons per year.     

A study of emissions from a Euro 4 light duty diesel vehicle with the European particulate measurement programme

The California Air Resources Board, CARB, has participated in a program to quantify particulate matter (PM) emissions with a European methodology, which is known as the Particulate Measurement Programme (PMP). The essence of the PMP methodology is that the diesel PM from a Euro 4 vehicle equipped with a Diesel Particulate Filter (DPF) consists primarily of solid particles with a size range greater than 23 nm. The PMP testing and the enhanced testing performed by CARB have enabled an increased understanding of both the progress that has been made in PM reduction, and the future remaining challenges for new and improved DPF-equipped diesel vehicles. A comparison of measured regulated emissions and solid particle number emissions with the results obtained by the PMP participating international laboratories was a success, and CARB’s measurements and standard deviations compared well with the other laboratories. Enhanced measurements of the influence of vehicle conditioning prior to testing on PM mass and solid particle number results were performed, and some significant influences were discovered. For example, the influence of vehicle preconditioning on particle number results was significant for both the European and USA test driving cycles. However, the trends for the cycles were opposite with one cycle showing an increase and the other cycle showing a decrease in particle number emissions. If solid particle size distribution and total particle numbers are to be used as proposed in PMP, then a greater understanding of the quality and errors associated with measurement technologies is advisable.In general, particle counting instruments gave results with similar trends, but cycle-to-cycle testing variation was observed. Continuous measurements of particle number concentrations during test cycles have given detailed insight into PM generation. At the present time there is significant variation in the capabilities of the particle counting instruments in terms of particle size and concentration.Current measurements show the existence of a large number of volatile and semi-volatile particles of yet-to-be-resolved chemical composition in diesel exhaust, especially during DPF regeneration, and these particles are not included in the PMP methodology because they are smaller than 20 nm. It will be very challenging to improve our understanding of this class of diesel particulate matter.     

Bioethanol-gasoline fuel blends: exhaust emissions and morphological characterization of particulate from a moped engine

This study was aimed at evaluating the effects of gasoline-ethanol blends on the exhaust emissions in a catalyst-equipped four-stroke moped engine. The ethanol was blended with unleaded gasoline in at percentages (10, 15, and 20% v/v). The regulated pollutants and the particulate matter emissions were evaluated over the European ECE R47 driving cycle on the chassis dynamometer bench. Particulate matter was characterized in terms of total mass collected on filters and total number ofparticles in the range 7 nm-10 microm measured by electrical low-pressure impactor (ELPI). In addition, particle-phase polycyclic aromatic hydrocarbons (PAHs) emissions were evaluated to assess the health impact of the emitted particulate. Finally, an accurate morphological analysis was performed on the particulate by high-resolution transmission electron microscope (TEM) equipped with a digital image-processing/data-acquisition system. In general, CO emission reductions of 60-70% were obtained with 15 and 20% v/v ethanol blends, while the ethanol use did not reduce hydrocarbon (HC) and NOx emissions. No evident effect of ethanol on the particulate mass emissions and associated PAHs emissions was observed. Twenty-one PAHs were quantified in the particulate phase with emissions ranging from 26 to 35 microg/km and benzo[a]pyrene equivalent (BaPeq) emission factors from 2.2 to 4.1 microg/km. Both particulate matter and associated PAHs with higher carcinogenic risk were mainly emitted in the submicrometer size range (<0.1 microm). On the basis of the TEM observations, no relevant effect of the ethanol use on the particulate morphology was evidenced, showing aggregates composed ofprimary particles with mean diameters in the range 17.5-32.5 nm.     

Informative Report

Abstract

Chemical composition and particle size data for particulate emissions from stationary sources are required for environmental health effect assessments, air chemistry studies and for air quality modeling investigations such as source apportionment. The Information presented In this paper is directed to those individuals concerned with these environmental Investigations. In this study, particulate emissions from a group of non-ferrous smelters have been physically and chemically characterized. Emission samples were collected at the baghouse outlets from smelter furnaces and at smelter acid plant stacks at three locations; a zinc, a lead, and a copper smelter.

Mass emission rate determinations were made by EPA reference methods. Cascade impactors were used to collect in-stack samples for particle size distribution measurements. Particulate samples for chemical characterization were collected on membrane filters for analysis by X-ray fluorescence spectroscopy. Development of measurement techniques required to determine the elemental composition of the total mass and sized fractions of the emission are discussed. Results of the tests at the three smelters include total mass and elemental emission rates, particle size distribution, and the elemental composition of the total particulate mass and of sized fractions from both the smelter furnaces and acid plants. The results obtained at the copper smelter may not be representative of the emissions at the many copper smelters where reverbatory furnaces have been replaced.     

Air Quality Effects from Quenching Coke with Fresh versus Process Water

Because of the extreme difficulties in sampling the discharge from coke-quench towers, only limited data have been available on the magnitude and effect of the emissions from this source. To evaluate this process better, U.S. Steel retained TRC Environmental Consultants, Inc., to undertake a test program at Gary Works (1) to conduct the necessary sampling tests to develop particulate emission factors for the coke-quenching operation during quenching with fresh water and with waste process water makeup to the quench system and (2) to estimate the impact of the emissions on ambient air quality for both conditions by means of dispersion modeling.

The test results for a new offset quench tower provided with impingement baffles show particulate emissions of 0.35 pound per ton of coal (Ib/ton) for fresh water and 0.45 Ib/ton for process water quenching. The results for an older, straight-through, low-velocity quench tower, also provided with baffles, show 0.32 and 0.64 Ib/ton for fresh and process water quenching, respectively. The results of the dispersion model studies indicate a minimal effect on ambient air concentration of particulates due to coke quenching with either fresh or process water.     

Woodstove smoke and CO emissions: comparison of reference methods with the VIP sampler

A new field sampler has been developed for measuring the particulate matter (PM) and carbon monoxide emissions of woodburning stoves. Particulate matter is determined by carbon balance and the workup of a sample train which is similar to a room-temperature EPA Method 5G train. A steel tank, initially evacuated, serves as the motive force for sampling and also accumulates a gas sample for post-test analysis of time-averaged stack CO and CO2 concentrations. Workup procedures can be completed within 72 hours of sampler retrieval. The system has been compared to reference methods in two laboratory test series involving six different woodburning appliances and two independent laboratories. The correlation of field sampler emission rates and reference method rates is strong.     

Hot Filter/Impinger and Dilution Sampling for Fine Particulate Matter Characterization from Ferrous Metal Casting Processes

Abstract

A study using two stack-sampling methodologies for collecting particulate matter (PM) emissions was conducted using a hot filter followed by a cold impinger sampling train and a dilution sampler. Samples were collected from ferrous iron metal casting processes that included pouring molten iron into a sand mold containing an organic binder, metal cooling, removal of the sand from the cooled casting (shakeout), and postshakeout cooling. The shakeout process contributed more to PM emissions than the metal pouring and cooling processes. Particulate matter less than 2.5 μm in aerodynamic diameter (PM_2.5) mass emissions for the entire casting cycle ranged from 3.4 to 4.7 lb/t of metal for the hot filter/impinger method and from 0.8 to 1.8 lb/t of metal for the dilution method. Most of the difference was due to PM captured by the impingers, much of which was probably dissolved gases rather than condensable vapors. Of the PM fraction captured by the impingers, 96–98% was organic in nature. The impinger PM fraction contributed 32–38% to the total suspended particle mass and caused a factor of 2–4 positive bias for PM_2.5 emissions. For the pouring and cooling processes only, the factor increased to over seven times.     

Woodstove Smoke and CO Emissions: Comparison of Reference Methods with the VPI Sampler

A new field sampler has been developed for measuring the particulate matter (PM) and carbon monoxide emissions of woodburning stoves. Particulate matter is determined by carbon balance and the workup of a sample train which is similar to a room-temperature EPA Method 5G train. A steel tank, initially evacuated, serves as the motive force for sampling and also accumulates a gas sample for post-test analysis of time-averaged stack CO and CO₂ concentrations. Workup procedures can be completed, within 72 hours of sampler retrieval. The system has been compared to reference methods in two laboratory test series involving six different woodburning appliances and two independent laboratories. The correlation of field sampler emission rates and reference method rates is strong.     

Blast Furnace Casthouse Control Technology and Recent Emissions Test Data

By the fall of 1980, three new and seven retrofit casthouse emission control systems had been installed in North America. A number of prototype systems are being evaluated by steel companies and regulatory agencies. By 1981, the U.S. steel industry had made commitments to install controls on at least 58 additional casthouses in the U.S.

This paper describes the current status of casthouse control technology in the U.S. and Canada as of the spring of 1981, addresses future trends, and presents emissions test data collected in 1980 and 1981. Mass emissions and inhalable particulate test results from sampling at DOFASCO’s No. 3 blast furnace casthouse are presented. Roof monitor visible emissions data are also provided to describe performance of installed and demonstration systems including three J&L plants, Wheeling-Pittsburgh and Bethlehem Steel, and Inland’s new furnace.     

Impacts of biodiesel on pollutant emissions of a JP-8-fueled turbine engine

The impacts of biodiesel on gaseous and particulate matter (PM) emissions of a JP-8-fueled T63 engine were investigated. Jet fuel was blended with the soybean oil-derived methyl ester biofuel at various concentrations and combusted in the turbine engine. The engine was operated at three power settings, namely ground idle, cruise, and takeoff power, to study the impact of the biodiesel at significantly different pressure and temperature conditions. Particulate emissions were characterized by measuring the particle number density (PND; particulate concentration), the particle size distribution, and the total particulate mass. PM samples were collected for offline analysis to obtain information about the effect of the biodiesel on the polycyclic aromatic hydrocarbon (PAH) content. In addition, temperature-programmed oxidation was performed on the collected soot samples to obtain information about the carbonaceous content (elemental or organic). Major and minor gaseous emissions were quantified using a total hydrocarbon analyzer, an oxygen analyzer, and a Fourier Transform IR analyzer. Test results showed the potential of biodiesel to reduce soot emissions in the jet-fueled turbine engine without negatively impacting the engine performance. These reductions, however, were observed only at the higher power settings with relatively high concentrations of biodiesel. Specifically, reductions of approximately 15% in the PND were observed at cruise and takeoff conditions with 20% biodiesel in the jet fuel. At the idle condition, slight increases in PND were observed; however, evidence shows this increase to be the result of condensed uncombusted biodiesel. Most of the gaseous emissions were unaffected under all of the conditions. The biodiesel was observed to have minimal effect on the formation of polycyclic aromatic hydrocarbons during this study. In addition to the combustion results, discussion of the physical and chemical characteristics of the blended fuels obtained using standard American Society for Testing and Materials (ASTM) fuel specifications methods are presented.     

Impacts of Biodiesel on Pollutant Emissions of a JP-8–Fueled Turbine Engine

Abstract

The impacts of biodiesel on gaseous and particulate matter (PM) emissions of a JP-8–fueled T63 engine were investigated. Jet fuel was blended with the soybean oil-derived methyl ester biofuel at various concentrations and combusted in the turbine engine. The engine was operated at three power settings, namely ground idle, cruise, and takeoff power, to study the impact of the biodiesel at significantly different pressure and temperature conditions. Particulate emissions were characterized by measuring the particle number density (PND; particulate concentration), the particle size distribution, and the total particulate mass. PM samples were collected for off-line analysis to obtain information about the effect of the biodiesel on the polycyclic aromatic hydrocarbon (PAH) content. In addition, temperature-programmed oxidation was performed on the collected soot samples to obtain information about the carbonaceous content (elemental or organic). Major and minor gaseous emissions were quantified using a total hydrocarbon analyzer, an oxygen analyzer, and a Fourier Transform IR analyzer. Test results showed the potential of biodiesel to reduce soot emissions in the jet-fueled turbine engine without negatively impacting the engine performance. These reductions, however, were observed only at the higher power settings with relatively high concentrations of biodiesel. Specifically, reductions of ～15% in the PND were observed at cruise and takeoff conditions with 20% biodiesel in the jet fuel. At the idle condition, slight increases in PND were observed; however, evidence shows this increase to be the result of condensed uncombusted biodiesel. Most of the gaseous emissions were unaffected under all of the conditions. The biodiesel was observed to have minimal effect on the formation of polycyclic aromatic hydrocarbons during this study. In addition to the combustion results, discussion of the physical and chemical characteristics of the blended fuels obtained using standard American Society for Testing and Materials (ASTM) fuel specifications methods are presented.     

Hot filter/impinger and dilution sampling for fine particulate matter characterization from ferrous metal casting processes

A study using two stack-sampling methodologies for collecting particulate matter (PM) emissions was conducted using a hot filter followed by a cold impinger sampling train and a dilution sampler. Samples were collected from ferrous iron metal casting processes that included pouring molten iron into a sand mold containing an organic binder, metal cooling, removal of the sand from the cooled casting (shakeout), and postshakeout cooling. The shakeout process contributed more to PM emissions than the metal pouring and cooling processes. Particulate matter less than 2.5 microm in aerodynamic diameter (PM2.5) mass emissions for the entire casting cycle ranged from 3.4 to 4.7 lb/t of metal for the hot filter/impinger method and from 0.8 to 1.8 lb/t of metal for the dilution method. Most of the difference was due to PM captured by the impingers, much of which was probably dissolved gases rather than condensable vapors. Of the PM fraction captured by the impingers, 96-98% was organic in nature. The impinger PM fraction contributed 32-38% to the total suspended particle mass and caused a factor of 2-4 positive bias for PM2.5 emissions. For the pouring and cooling processes only, the factor increased to over seven times.     

An Emission Sampling Probe Installed,Operated, and Retrieved from Ground Level

The “Teepee” type wood residue incinerator, similar to many other sources, requires sampling at the point where the emissions enter the atmosphere. Because the location of the emission point is hazardous and unpleasant for the operation of a sampling probe, a portable, tilt-up column was developed which permitted installation, operation, and retrieval of the sampling train from ground level. The sampling train developed permitted determination of the size distribution and weight of the particulate emitted by this highly variable source.