The need to limit sulphur dioxide, nitrous oxides and particulate matter emissions from fossil fuel combustion processes is now a major factor in the design, construction and operation of plants. Over the past 5 to 10 years, most developed countries have introduced legislations to control these. emissions. This report was done to investigate emissions of sulphur dioxide (S02), nitrogen oxides (NOx) and particulate matter from coal fired power plants. S02 emissions contribute to an air pollution load that has been found to be linked to respiratory and heart problems. It increases the formation of acid precipitation, called acid rain. NOx oxides to nitrogen dioxide (N02). N02 acts as an irritant to the respiratory tract, alveoli of the lungs and causes chest pains. Toxic elements concentrate on fine particulate matter because of their high surface-area to volume ratio. These particles penetrate and settle onto the lung wall, leading to respiratory disorders and lung diseases. Due to the strict legislative requirements, flue gas detoxification processes were investigated. They include: • Wet scrubbing • Spray dry scrubbing • Dual-alkali • Well man-Lord • Activated carbon • Magnesium oxides • Selective catalytic recovery • Circulating fluidised bed combustion • Electromembrane desulphurisation A study was done to show the possible cost implications associated with the wet scrubbing, spray dry scrubbing, selective catalytic recovery, circulating fluidised bed and electromembrane desulphurisation process. A variety of methods were used to calculate cost, due to costs being difficult to obtain. Most of the information was based on European, Asian and American installations. The objective of this economic analysis was to compare the different technologies. Because of the assumptions used, costs were always "order of magnitude" estimates. Capital and operating costs were calculated for these technologies, but they can only be used as an indication of costs and to allow for comparisons between the technologies. The costs were converted using the January 2000 exchange rates. Due to this, costs may be more inflated than what would normally be expected due to equipment being purchased earlier than January 2000. Of the processes investigated, the circulating fluidised bed process was found to be the most economical. There is no inexpensive route for the removal of sulphur dioxide, nitrous oxides and particulate matter. The most suitable detoxification process will depend on the legislative requirements per country. South Africa is a signatory of the Montreal Protocol and the Framework for Climatic Change. Legislations for gaseous emissions were not considered a priority. Currently, Eskom's drive is to electrify townships rather than spend money on detoxification processes. However, future legislations may require more stringent control measures. / Thesis (M.Sc.Eng.)-University of Durban-Westville, 2000.

Soot formation from complex solid fuels, such as coal or biomass, is an under-studied and little understood phenomena which has profound physical effects. Any time a solid fuel is combusted, from coal-burning power plants to wildland fires, soot formation within the flame can have a significant influence on combustion characteristics such as temperature, heat flux, and chemical profiles. If emitted from the flame, soot particles have long-last effects on human health and the environment. The work in this dissertation focuses on creating and implementing computational models to be used for predicting soot mechanisms in a combustion environment. Three models are discussed in this work; the first is a previously developed model designed to predict soot yield in coal systems. This model was implemented into a computational fluid dynamic software and results are presented. The second model is a detailed-physics based model developed here. Validation for this model is presented along with some results of its implementation into the same software. The third model is a simplified version of the detailed model and is presented with some comparison case studies implemented on a variety of platforms and scenarios. While the main focus of this work is the presentation of the three computational models and their implementations, a considerable bulk of this work will discuss some of the technical tools used to accomplish this work. Some of these tools include an introduction to Bayesian statistics used in parameter inference and the method of moments with methods to resolve the 'closure' problem.

Direct fuel injection technology is increasingly being applied to the spark ignition internal combustion engine as one of the many actions required to reduce the CO2 emissions from road transport. Whilst the potential for CO2 reductions is compelling, the technology is not without disadvantages. Early examples typically emitted over an order of magnitude more Particulate Matter (PM) than vehicles with conventional spark ignition engines. Consequently, future revisions to European and North American exhaust emissions legislation are likely to regulate the particulate emissions from vehicles with direct injection gasoline engines. This thesis undertakes to investigate a) instrumentation capable of simultaneously resolving the number concentration and size distribution of particles in the 5-1000 nm size range and b) the factors affecting the PM emissions from spark ignition engines with direct fuel injection. The first objective is achieved by evaluation and comparison of a differential mobility spectrometer; photo-acoustic soot sensor; condensation particle counter and electrical low pressure impactor. To address the second question, a differential mobility spectrometer is applied to quantify the PM emissions from a number of direct injection gasoline engines, together with investigation of their dependence on various calibratable parameters, operating temperature and fuel composition. The differential mobility spectrometer showed good agreement with the other more established instruments tested. Moreover, it exhibited a faster time response and finer resolution in particle size. The number weighted size distribution of the PM emitted was typically lognormal with either one or two modes located between 20 and 100 nm. Chemical analysis of PM samples showed the presence of elemental carbon, volatile organic material and sulphates. Transient PM measurements enabled short time-scale events such as mode switching between homogeneous and stratified mixture preparation to be identified. PM number concentrations in stratified mode exceeded those in homogeneous mode by a factor of 10-100. Dynamometer based experiments showed that PM emissions increase for rich air fuel ratios, retarded fuel injection and advanced ignition events. They also demonstrated a strong dependence on fuel composition: the highest PM emissions were measured with an aromatic fuel, whereas blending alcohols such as methanol or ethanol tended to suppress PM emissions, particularly in the accumulation mode size range. These measurements are amongst the first of their kind and demonstrate the applicability of the differential mobility spectrometer to the measurement of ultra-fine particulate emissions from engines with direct fuel injection systems. Numerous explanations are put forward to describe the data obtained, together with suggestions for future work on PM control and abatement.

Biomass fast pyrolysis liquid (bio-oil) is a cellulose based alternative fuel with the potential to displace fossil fuels in stationary heat and power applications. To better understand the combustion behavior and emissions of bio-oil, a 10 kW spray burner was designed and constructed. The effect of swirl, atomization quality, ignition source (pilot) energy, air/fuel preheat and equivalence ratio on the stability and emissions of bio-oil spray flames was investigated. A blend of 80% pyrolysis liquid and 20% ethanol by volume was used during the tests and the results were compared to burner operation with diesel. It is important to have good atomization, thorough mixing and high swirl in order to stabilize ignition, promote the burnout of bio-oil and decrease CO, hydrocarbon and particulate matter emissions. The total amount of primary air and atomizing air that can be used to improve turbulence, mixing, droplet burnout and overall combustion quality is limited by the distillable fraction and narrow lean blow-out limit associated with pyrolysis liquid. Air and fuel preheat are important for reducing hydrocarbon and CO emissions, although subsequent fuel boiling should be avoided in order to maintain flame stability. The NOx produced in bio-oil flames is dominated by the conversion of fuel bound nitrogen. The particulate matter collected during bio-oil combustion is composed of both carbonaceous cenosphere residues and ash. Under good burning conditions, the majority consists of ash. Pilot flame energy and air/fuel preheat have a weak effect on the total particulate matter in the exhaust. Generally, these results suggest that available burner parameters can be adjusted in order to achieve low hydrocarbon, CO and carbonaceous particulate matter emissions when using pyrolysis liquid. Total particulates can be further mitigated by reducing the inherent ash content in bio-oil. Comparative burner tests with diesel reveal much lower emissions for this fuel at most of the operating points considered. This is due to the fully distillable nature, better atomization and improved spray ignition characteristics associated with diesel. Because of its superior volatility, diesel can also operate over a much wider range of primary air and atomizing air flow rates compared to bio-oil.

Biomass fast pyrolysis liquid (bio-oil) is a cellulose based alternative fuel with the potential to displace fossil fuels in stationary heat and power applications. To better understand the combustion behavior and emissions of bio-oil, a 10 kW spray burner was designed and constructed. The effect of swirl, atomization quality, ignition source (pilot) energy, air/fuel preheat and equivalence ratio on the stability and emissions of bio-oil spray flames was investigated. A blend of 80% pyrolysis liquid and 20% ethanol by volume was used during the tests and the results were compared to burner operation with diesel. It is important to have good atomization, thorough mixing and high swirl in order to stabilize ignition, promote the burnout of bio-oil and decrease CO, hydrocarbon and particulate matter emissions. The total amount of primary air and atomizing air that can be used to improve turbulence, mixing, droplet burnout and overall combustion quality is limited by the distillable fraction and narrow lean blow-out limit associated with pyrolysis liquid. Air and fuel preheat are important for reducing hydrocarbon and CO emissions, although subsequent fuel boiling should be avoided in order to maintain flame stability. The NOx produced in bio-oil flames is dominated by the conversion of fuel bound nitrogen. The particulate matter collected during bio-oil combustion is composed of both carbonaceous cenosphere residues and ash. Under good burning conditions, the majority consists of ash. Pilot flame energy and air/fuel preheat have a weak effect on the total particulate matter in the exhaust. Generally, these results suggest that available burner parameters can be adjusted in order to achieve low hydrocarbon, CO and carbonaceous particulate matter emissions when using pyrolysis liquid. Total particulates can be further mitigated by reducing the inherent ash content in bio-oil. Comparative burner tests with diesel reveal much lower emissions for this fuel at most of the operating points considered. This is due to the fully distillable nature, better atomization and improved spray ignition characteristics associated with diesel. Because of its superior volatility, diesel can also operate over a much wider range of primary air and atomizing air flow rates compared to bio-oil.

Doctor of Philosophy / Department of Biological and Agricultural Engineering / Ronaldo G. Maghirang / Emission of particulate matter (PM) and various gases from open-lot beef cattle feedlots is becoming a concern because of the adverse effects on human health and the environment; however, scientific information on feedlot emissions is limited. This research was conducted to estimate emission rates of PM[subscript]10 from large cattle feedlots. Specific objectives were to: (1) determine feedlot PM[subscript]10 emission rates by reverse dispersion modeling using AERMOD; (2) compare AERMOD and WindTrax in terms of their predicted concentrations and back-calculated PM[subscript]10 emission rates; (3) examine the sensitivity of both AERMOD and WindTrax to changes in meteorological parameters, source location, and receptor location; (4) determine feedlot PM[subscript]10 emission rates using the flux-gradient technique; and (5) compare AERMOD and computational fluid dynamics (CFD) in simulating particulate dispersion from an area source. PM[subscript]10 emission rates from two cattle feedlots in Kansas were determined by reverse dispersion modeling with AERMOD using PM[subscript]10 concentration and meteorological measurements over a 2-yr period. PM[subscript]10 emission rates for these feedlots varied seasonally, with overall medians of 1.60 and 1.10 g /m[superscript]2 -day. Warm and prolonged dry periods had significantly higher PM emissions compared to cold periods. Results also showed that the PM[subscript]10 emissions had a diurnal trend; highest PM[subscript]10 emission rates were observed during the afternoon and early evening periods. Using particulate concentration and meteorological measurements from a third cattle feedlot, PM[subscript]10 emission rates were back-calculated with AERMOD and WindTrax. Higher PM[subscript]10 emission rates were calculated by AERMOD, but their resulting PM[subscript]10 emission rates were highly linear (R[superscript]2 > 0.88). As such, development of conversion factors between these two models is feasible. AERMOD and WindTrax were also compared based on their sensitivity to changes in meteorological parameters and source locations. In general, AERMOD calculated lower concentrations than WindTrax; however, the two models responded similarly to changes in wind speed, surface roughness, atmospheric stability, and source and receptor locations. The flux-gradient technique also estimated PM[subscript]10 emission rates at the third cattle feedlot. Analyses of PM[subscript]10 emission rates and meteorological parameters indicated that PM[subscript]10 emissions at the feedlot were influenced by friction velocity, sensible heat flux, temperature, and surface roughness. Based on pen surface water content measurements, a water content of at least 20% (wet basis) significantly lowered PM[subscript]10 emissions at the feedlot. The dispersion of particulate from a simulated feedlot pen was predicted using CFD turbulence model ([kappa]-[epsilon] model) and AERMOD. Compared to CFD, AERMOD responded differently to wind speed setting, and was not able to provide detailed vertical concentration profiles such that the vertical concentration gradients at the first few meters from the ground were negligible. This demonstrates some limitations of AERMOD in simulating dispersion for area sources such as cattle feedlots and suggests the need to further evaluate its performance for area source modeling.

The control of particle emissions from an oil refinery is often difficult, due to changing operational conditions and the limited range of available treatment options. Excessive particle emissions have often been attributed start up problems with Fluidized Catalytic Cracker Units (FCCU) and little information is available regarding the exact composition and nature of these excessive emissions. Due to the complex nature of a FCCU, it has in the past been difficult to identify and control emissions, without the use of expensive end of pipe technologies. An Australian Oil Refinery, concerned with their catalyst emissions, sponsored this study of FCCU particle emissions. Due to the industrial nature of the project, a holistic approach to the management of emissions was taken, instead of a detailed investigation of a single issue. By looking at the broader range of issues, practical and useful outcomes can be achieved for the refinery. Initially, detailed emissions samplings were conducted to investigate the degree of particle emissions under start up conditions. Stack emissions were collected during a standard start up, and analysed to determine the particle size distribution and metal concentration of the emitted material. Three distinct stages of emissions were discovered, initially a high concentration of larger particles, followed by a peak in the very fine particles and finally a reduction of particle emissions to a more steady or normal operational state. The variation in particle emissions was caused by operational conditions, hardware design and catalyst characteristics. Fluctuations in the gas velocity through the system altered the ability of the cyclones to collect catalyst material. Also, the low bed level allowed air bypass to occur more readily, contributing to the increased emissions levels seen during the initial stage of the start up. Reduced fluidity characteristics of the circulating catalyst also affected the diplegs operations, altering the collection efficiency of the cyclone. During the loading of catalyst into the system, abraded material was quickly lost due to its particle size, contributing to fine particle emissions levels. More importantly, thermal fracturing of catalyst particles occurred when the cold catalyst was fed into the hot regenerator. Catalyst particles split causing the generation of large amounts of fine particle material, which is easily lost from the system. This loading of catalyst directly linked to the period of high concentration of fine particles in the emissions stream. It was found that metals, and in particular iron, calcium and silicon form a thick layer on the outside of the catalyst, with large irregular shaped metal ridges, forming along the surface of the particle. These ridges reduce the fluidity of the catalyst, leading to potential disruptions in the regenerator. In addition to this, the metal rich ridges are preferentially removed via attrition, causing metal rich material to be emitted into the atmosphere. To overcome these high particle emissions rates from the FCCU the refinery should only use calcinated catalyst to reduce the influence of thermal process and particle fracture and generation. Although the calcinated catalyst can fracture when added to the system, it is far less than that obtained with uncalicinated catalyst. To further reduce the risk of particle fracture due to thermal stresses the refinery should consider reducing the temperature gradients between the hot and cold catalyst. Due to the economics involved with the regenerator, possible pre-warming of catalyst before addition into system is the preferred option. This pre-heating of catalyst should also incorporate a controlled attrition stage to help remove the build up of metals on the surface of the particles whilst allowing this material to be collected before it can be released into the atmosphere. The remove of the metal crust will also improve the fluidity of the system and reduce the chance of catalyst blockages occurring. Finally, modelling of the system has shown that control of key parameters such as particle size and gas velocity are essential to the management of air emissions. The refinery should look at adjusting start up procedures to remove fluctuations in these key parameters. Also the refinery should be careful in using correlation found in the literature to predicted operational conditions in the system as these correlations are misleading when used under industrial situations.