This thesis focused on the fate of nitrogen and trace metals species from combustion and gasification of biomass. The effect of process parameters on the release of these species during pilot-scale combustion and gasification of biomass was investigated and the information used to identify methods for the reduction of these species. The investigation focused on Miscanthus and Dried distillers’ grains with solubles (DDGS). The pilot-scale test rigs used were a fluidised-bed combustor and a fixed-bed downdraft gasifier. The two fuels were analysed by means of proximate, ultimate and ash analysis. The process parameters monitored were temperatures, gas flow, gas composition and ash composition and the process parameters studied are bed temperature and equivalence ratio. The different nitrogen content of the two fuels plays an important role in the emission. Both bed temperature and air to fuel ratio have demonstrated to have an important influence in the release of nitrogen oxides in combustion and ammonia in gasification, therefore they can be used to mitigate the emission of these species in the flue gas. Both processes are affected by the high alkali metals content of the fuels for the tendency to form low melting composites. Differences have been highlighted in the metal distribution between combustion and gasification. The different nitrogen and ash content of the two fuels make the results of the present thesis applicable to predict the behaviour of other biomass fuels according to the fuel characteristics. The scale of the tests performed allowed highlighting which methods can be used to control the emission of nitrogen and trace metal species. Moreover, the investigation highlighted major drawbacks in the use of biomass fuels in both fluidised bed and fixed bed technology due to ash properties.

Interest in biodiesel has piqued with advent of stringent emissions regulations. Biodiesel is a viable substitute for petroleum diesel because biodiesel produces significantly lower particulate and soot emissions relative to petroleum diesel. Higher nitric oxide (NO) emissions for biodiesel, however, are of primary concern in biodiesel-fueled engines. Search for an in-cylinder technique to reduce NO emissions for biodiesel has motivated studies to gain an improved understanding of fundamental factors that drive increase in NO emissions with biodiesel. Potential factors include fuel-bound oxygen, fuel-bound nitrogen and post-flame gas temperature. The role of fuel-bound oxygen however is debated in the literature. The research objective of this study is to computationally determine if biodiesel and petroleum diesel yield equivalent concentrations of NO with the same oxygen equivalence ratio in a 0-D homogeneous reactor, to explain the role of fuel-bound oxygen in biodiesel on increases in NO emissions with biodiesel. The results from this study indicate that the biodiesel surrogate yields higher NO emissions than the n-heptane because of its lower oxygen consumption efficiency. The lower oxygen consumption efficiency for biodiesel is likely because of the slower decomposition of the individual components and the blending ratios of the biodiesel surrogate blend. The relative differences in combustion efficiency of individual components of the biodiesel blend suggest this conclusion. The more efficient burning of the methyl esters relative to the n-heptane in biodiesel surrogate perhaps indicates the favorable role of fuel-bound oxygen in the fuel’s combustion. The low utilization of oxygen by the biodiesel surrogate could not be explained in this study. The dominance of NO2 H ↔ NO OH and N NO ↔ N2 O mechanisms during biodiesel combustion however explain the high NO emissions for the biodiesel surrogate relative to the n-heptane. The biodiesel may yield lower NO emissions than the petroleum diesel if the blending ratios for the biodiesel are adjusted such that combustion efficiency of biodiesel and petroleum diesel is same or the NO2 H ↔ NO OH and N NO ↔ N2 O mechanisms are suppressed during biodiesel combustion.

In recent years, the development and use of biofuels have received considerable attention due to the high demand for environmentally acceptable (green) fuels. Most of the recent studies have looked at the processes of converting vegetable oils into biodiesel. It is well known vegetable oil to biodiesel conversion involves many processes including transesterification, which makes biodiesel costly and time-consuming to produce. In this study, the effects of blending high-viscosity fresh and used corn oils with low-viscosity diesel and jet fuel mixed with butanol and ethanol were studied. Several corn oil-based blends were formulated and characterized to understand the effect of composition on viscosity, fuel stability and energy content. The formulated corn oil blends were combusted in a 30 kW modified combustion chamber to determine the corresponding NOx and CO emission levels, along with CO₂ levels. Used corn oil was made by simply heating fresh corn oil for a fixed period of time (about 44 hours), and was characterized by quantifying its total polar material (TPM), iodine value, free fatty acid content, and peroxide value. The combustion experiments were conducted at a constant heat output of 68,620 kJ/hr (19 kW), to observe and study the effects of equivalence ratio, swirl number, and fuel composition on emissions. Used corn oil blends exhibited better combustion performance than fresh corn oil blends, due in part to the higher unsaturation levels in fresh corn oil. NOx emissions for used corn oil increased with swirl number. Among all the blends, the one with the higher amount of diesel (lower amount of corn oil) showed higher NOx emissions. The blend with fresh corn oil showed decreasing NOx with increasing equivalence ratio at swirl number 1.4. All blends showed generally decreasing CO trends at both swirl numbers at very lean conditions. The diesel fuel component as well as the alcohols in the blends were also important in the production of pollutants. Compared to the diesel-based blends mixed with used corn oil, butanol, and ethanol, the jet fuel-based blends showed higher NOx levels and lower CO levels at both swirl numbers.

The safe and efficient propagation of the Deflagration to Detonation Transition (DDT) is a topic that has been researched for many years due to its applications in Aerospace and Mechanical Engineering. DDT is when fire caused by the burning of fuel is accelerated to the upper CJ point on the Rankine Hugoniot curve due to instabilities in the flame and the turbulence caused by these instabilities. The complex flame dynamics that go along with DDT have ensured that the process is yet to be fully understood and defined. This research will work towards observing the early stages of burning hydrogen-air mixtures in DDT conditions in order to better understand the processes that cause DDT. The research will also involve the testing of multiple different equivalence ratios of hydrogen known to undergo DDT. This research will assist in making places that store reactive gasses such as hydrogen safer by searching for the method of DDT formation and ways to prevent it. This research will also allow for safer commercial use of DDT in Detonation Based Engines. The research was tested in a secure facility and observed the first four inches of ignition and deflagration using schlieren and chemiluminescence imaging techniques. Through the research, it was found that flames at higher equivalence ratios tend to be longer, more top-biased, and have more instabilities than flames of lower equivalence ratios, better preparing them for DDT. This study will be elaborated on in future research using a variety of different fuels to solidify the findings of the research performed and to assist in the ability to innovate using DDT.

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Plasma gasification experiments were conducted on sucrose and crushed macadamia nutshells. The pilot-scale plasma gasification system used comprises a 15 kW DC plasma torch fitted to a 5 L gasification reactor. The DC plasma torch has an efficiency of ~30 % with most of the energy lost in the torch anode. For the macadamia nutshells, the plasma input-power was set at 9, 11 and 14 kW. At each power input setting, four different feed rates were investigated, namely 0.5, 0.7, 1.04 and 1.14 kg/h. It was observed that as the power increases, conversion increases from 48 % at 9 kW to higher than 80 % at 14 kW. It was also observed that higher mass feed rates increase the conversion. The lower heating values of the syngas produced during gasification increased with higher power inputs and higher feed rates. At a feed rate of 1 kg/h, the maximum calorific power value was 3.45 kW, at a torch setting of 14 kW. The highest power values obtained was slightly more than 4 kW. The effect of equivalence ratio (ER) was evaluated on the plasma gasification of sucrose. ER values of 1 and 2 were investigated. With an ER of 1, the CO/H2 ratio was 1.8 and the CO/CO2 ratio was 109. With an ER of 2, the CO/H2 ratio was 1.73, and the CO/CO2 ratio 18. As expected, an increase in ER enhances the formation of CO2. A low ER thus results in higher syngas quality. At equivalent conditions the homogenous, crystalline sucrose yielded a CO/CO2 ratio of 109, significantly higher than the 29 for plasma gasification of the macadamia nut shells. A contributing factor to having better quality syngas, was the smaller the average particle diameter of the sucrose, 0.4 mm, compared to the 10 mm of the crushed macadamia nut shells was. Another contributing factor could be that the available carbon in the macadamia nut shells structure are more strongly bonded than in sucrose. For additional insight, kinetic data for the pyrolysis of sucrose, fructose and glucose were obtained using a TGA-FTIR hyphenated system, at much lower heating rates than anticipated in plasma system, and TGA-DTG experiments on macadamia nut shells. Dynamic studies were performed on sucrose, fructose and glucose at heating rates of 5, 10, 15, 20 and 50 °C/min in an atmosphere of nitrogen flowing at 50 mL/min, and for the macadamia shell at heating rates of 5, 10 and 20 °C/min in an atmosphere of nitrogen flowing at 50 mL/min. The sugars yielded 80 % to 85 % conversion into gaseous products, while the conversion of the shells approached 90 %; the residue was biochar. The FTIR spectra showed the major products that form from the pyrolysis of sugars to be CO2, H2O, along with large quantities C-H-O-containing compounds, amongst them C5H4O2 and C6H6O3. The latter two compounds are probably condensible. / Dissertation (MEng)--University of Pretoria, 2020. / Chemical Engineering / MEng / Unrestricted

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Les variations de la composition des gaz naturels nécessitent un system de réglage automatique de la richesse de flamme pour des chaudières domestiques à gaz. Dans ce travail,deux solutions potentielles sont étudiées, à savoir la chimiluminescence de flamme et le courant d’ionisation. Des indicateurs de richesse sont déduits des signaux de chimiluminescence obtenus expérimentalement. L’impact de l’échange de chaleur entre la flamme et le brûleur sur des signaux de chimiluminescence est ensuite étudié. Une analyse est également faite des principaux facteurs pouvant perturber la caractérisation du signal de chimiluminescence. Le courant d’ionisation est ensuite étudié sur une flamme conique pour comprendre l’évolution de son intensité avec la position de sonde et avec les conditions de flamme. Il est montré ensuite que ces évolutions sont corrélées avec le changement de la distance entre la flamme et le brûleur. Enfin, une boucle de contrôle est développée pour démontrer la faisabilité d’un réglage automatique de richesse en exploitant le signal de chimiluminescence. / The variations of natural gas composition call for an automatic equivalence ratio regulation system for domestic gas boilers. Two potential techniques for this purpose are investigated, i.e. the flame chemiluminescence and ionization current. Equivalence ratio indicators are inferred from the chemiluminescence signal based on the experiments. The investigation proceeds by examining effects of the flameburner heat exchange on the chemiluminescence signal. The interference of several disturbing factors for the chemiluminescence signal characterization is also analyzed. The flame ionization current is investigated on a conical flame to understand the evolution of its intensity with the probe position and flame conditions. These changes are then attributed to modifications of the distance between the flame base and the burner rim. Finally a control loop is developed to demonstrate the feasibility of equivalence ratio self-regulation with the chemiluminescence signal.

Flame chemiluminescence has received increasing attention for its potential sensor and diagnostic applications in combustors. A number of studies have used flame chemiluminescence to monitor flame status, and combustor performance. While most of these studies have been empirical in nature, chemiluminescence modeling has the potential to provide a better understanding of the chemiluminescence processes and their dependence on various combustion operating conditions. The primary objective of this research was to identify and validate the important chemiluminescence reaction mechanisms for OH*, CH* and CO2*. To this end, measurements were performed at various operating conditions, primarily in laminar, premixed flames, fueled with methane, syngas (H2/CO) and Jet-A. The results are compared to 1-d laminar flame simulations employing the chemiluminescence mechanisms. The secondary objective was to use the experiments and validated chemiluminescence reaction mechanisms to evaluate the usefulness of flame chemiluminescence as a combustion diagnostic, particularly for heat release rate and equivalence ratio. The validation studies were able to identify specific mechanisms for OH*, CH* and CO2* that produced excellent agreement with the experimental data in most cases. The mechanisms were able to predict the variation of the chemiluminescence signals with equivalence ratio but not with pressure and reactant preheat. The possible reasons causing this disagreement could be due to the inaccuracies in the basic chemical mechanism used in the simulations, lack of accurate quenching data (for CH*), thermal excitation (for OH*) and radiative trapping (for OH* and CO2*) and interference from the emissions of other species (such as HCO and H2O), for CO2*. Regarding the utility of chemiluminescence for sensing, a number of observations can be made. In syngas-air flames, CO2* is a reasonable heat release rate marker, at least for very lean conditions. OH* shows some advantage in atmospheric-pressure methane and Jet-A flames in general, while CH* is advantageous at high pressure and very lean conditions at atmospheric pressure. The CO2*/OH* intensity ratio is not useful for sensing equivalence ratio in syngas flames, except maybe at very lean conditions. However, the CH*/OH* signal ratio is a promising approach for sensing equivalence ratio at low or very high pressure conditions in hydrocarbon flames. Thermal excitation and self-absorption processes for OH* chemiluminescence can become important for combustors operating at high pressure, high preheat and near stoichiometric conditions. Background subtracted chemiluminescence signals are recommended for sensing purposes.

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