The gasification of carbonaceous fuel materials offers significant potential for the production of both energy and chemical products. Advancement of gasification technologies may be expedited through the use of computational fluid dynamics, as virtual reactor design offers a low cost method for system prototyping. To that end, a series of numerical studies were conducted to identify a computational modeling strategy for the simulation of coal gasification in fluidized bed reactors. The efforts set forth by this work first involved the development of a validatable hydrodynamic modeling strategy for the simulation of sand and coal fluidization. Those fluidization models were then applied to systems at elevated temperatures and polydisperse systems that featured a complex material injection geometry, for which no experimental data exists. A method for establishing similitude between 2-D and 3-D multiphase systems that feature non-symmetric material injection were then delineated and numerically tested. Following the development of the hydrodynamic modeling strategy, simulations of coal gasification were conducted using three different chemistry models. Simulated results were compared to experimental outcomes in an effort to assess the validity of each gasification chemistry model. The chemistry model that exhibited the highest degree of agreement with the experimental findings was then further analyzed identify areas of potential improvement. / Ph. D.

No

Fluidized-bed combustion residue (FBCR) results from mixing coal with limestone during the combustion process. This by-product may be used as a liming agent. A grazing trial was conducted on an acidic mine soil to compare FBCR to dolomitic limestone and no amendment (control). Six steers per treatment were grazed rotationally on three replications (rep) of three .8 ha pastures. Both materials increased soil pH similarly, and reduced plant uptake of Fe, Zn, Mn, and Ni similarly. Calcium concentration increased in forages by both amendments, Mg increased with limestone and S with FBCR application. Cell wall components decreased, while ash and lignin increased with both amendments. Serum mineral levels of cattle were normal except Cu was low. Animal tissues reflected differences in mineral concentration observed in forages. Hay harvested from one rep was used in a mineral balance trial with 18 wethers. Apparent digestibility of dry matter, crude protein and fiber components, and N retention were not affected by treatment. Control animals were in negative Ca balance. Apparent absorption of Mg was higher (P < .01) for limestone treatment animals; S absorption was higher for the FBCR group; and, Zn absorption was higher for controls. Serum mineral levels of sheep were normal except Cu was low. No appreciable accumulation of heavy metals occurred in forage or animal tissues. Low Cu levels observed for all treatment groups indicate a problem inherent of the study site. FBCR appears to be a safe and efficient soil pH amendment. / Master of Science

The effect of the solid-circulation rate and pattern as well as the air-gap size on heat-transfer coefficients between a horizontal, cylindrical heater and vibrated beds of Master Beads (spherical alumina) and glass spheres was studied. Solid piles were observed to form at specific bed locations. Solid-circulation paths were directed from the shallowest toward the deepest region of the vibrated bed. For beds in which the solid pile formed above the heating surface, local solid-circulation loops were observed above and below the heater. Air gaps developed at the top and bottom of the cylindrical heater. Heat-transfer coefficients of 140-350 W/m²K in beds of glass spheres and 180-480 W/m²K in beds of Master Beads were determined for a temperature difference of 30°C between the heater and vibrated bed. The trends in the behavior of the heat-transfer coefficient could be explained in terms of a model that accounted for the air-gap size and particle renewal in the layer closest to the heater. Increased solid-circulation rates improved the heat-transfer performance until larger air-gap sizes eventually compromised any increase in solid circulation. The expansion of the interlayer spacing of H-Magadiite (a layered silicic acid) by the introduction of pillars containing silicon atoms was investigated. A trisiloxane and two trichloroorganosilane compounds were used as the pillaring agents. The interlayer space of H-Magadiite was successfully expanded by pillaring with trichloroorganosilanes. The minimum dimensions of the pores that access the interlayer space of the pillared compounds were determined as being 6.2 Å and 9.5 Å (dimensions at perpendicular directions). Pillaring of H-Magadiite at low pH and temperatures close to 0 °C yielded the highest surface areas, e.g., increasing the surface area from 35 to 130-200 m²/g. The pillared compounds were found to be thermally stable up to temperatures of 650°C. / Ph. D.

Ceramic candle filters were subjected to 500 hour high temperature/ high pressure (HTHP) exposure tests to examine their extended durability in simulated coal pressurized-fluidized bed combustion (PFBC) environments. The candle filter materials analyzed included two SiC filters, one with clay binder and one with a minimal amount of clay binder, a cordierite filter, a mullite candle filter and an aluminosilicate refractory concrete filter. Exposure testing conditions included a range of temperature from 700-850°C and a pressure ranging from 1.7-1.8 MPa. The HTHP tests included exposing the ceramic filter materials to steam and steam-alkali environments. The presence of alkali significantly accelerated the deterioration of the filters. The results of the analysis show that significant crushing strength losses were exhibited by the SiC filters after exposure to HTHP alkali-steam conditions at temperatures as low as 700°C. The expansive and destructive cristobalite phase developed in the SiC filters after most of the treatments. The cordierite candle filter showed a decrease in crushing strength associated with grain growth after each high temperature exposure but few other signs of deterioration were detected. The mullite candle filter and the refractory concrete candle filter showed the least amount of change in crushing strength and overall the most candle stability. / Master of Science

Particulate beds which are mobilized and expanded by the application of mechanical vibrations are called vibrated beds. These beds are generally defined as shallow, if the depth-to-width ratio is less than unity. The dynamics of shallow vibrated beds and the heat transfer from immersed tubes to such beds are investigated using a vibrational frequency of 25 Hz. The vibration equipment is designed to minimize distortions in the applied displacement waveform. Transducers used are of a sufficiently high frequency response to accurately follow the variation of bed properties over a vibrational cycle. An electronic circuit is designed to exactly phase-match data collected by a transducer with the vibrational displacement. The circuit may also be used to trigger a strobe lamp at any phase angle, thus permitting an accurate examination of the evolution of bed characteristics over a cycle. Measurements of floor pressures beneath the bed, indicate cyclic characteristics, caused by the bed motion. Horizontal floor-pressure gradients cause the bed to pile up or bunker within the vessel. In bunkered beds, particle motion is determined by horizontal gas flows, and a compaction wave which propagates diagonally through the bed during the bed-vessel collision. In non-bunkered beds, particle motion is driven largely by wall friction. The observed instant of bed-vessel separation lags the theoretical prediction by several degrees, most likely because of bed expansion associated with the bed lift-off. Different "states" of shallow vibrated beds are identified, each with a unique set of characteristics. One state which exists in ultra-shallow beds of depths between 6 and 15 particle diameters is characterized by a high porosity and good gas-solid interaction, making it potentially useful for studies of reaction kinetics. Surface-to-bed heat-transfer coefficients are measured for Master Beads and glass beads, and found to vary with particle size and vibrational intensity. Heat-transfer coefficients as high as 484 W/m²-K are obtained. Heat transfer depends on particle circulation and the formation of air gaps which periodically surround the heater surface. A simplified theoretical formulation for the heat-transfer coefficient appears to qualitatively predict observed trends in heat transfer. / Ph. D.

Foi realizado um estudo sobre o efeito das concentrações de SO2 na sua absorção por calcários em fornalhas de leito fluidizado. Para observar a influência do SO2 sobre os diferentes parâmetros físicos e químicos do processo, foram criadas atmosferas compostas por quatro concentrações diferentes de SO2, que foram de 500, 1.000, 2.000 e 4.000 ppm. Utilizou-se ainda dois tipos de calcários, o Dolomítico-DP e o Calcítico-CI. O leito fluidizado borbulhante utilizado, possuía 160 mm de diâmetro interno e foi fluidizado com ar à temperatura de 850ºC, contendo SO2 na concentração desejada. Como material do leito foi utilizada areia de quartzo (99,9%), com diâmetro de 385 &#956m e aproximadamente 3,0 Kg de massa. O calcário foi adicionado em bateladas de 50 g com o reator já pré-aquecido, enquanto as variações das concentrações dos gases SO2, CO2, CO e O2 e suas descargas foram monitoradas continuamente na saída do ciclone que era utilizado para retenção do particulado fino. Para adquirir esses dados foi desenvolvido um programa em LabView. O modelo matemático escolhido possibilitou a determinação da conversão, da taxa de conversão e do coeficiente global de taxa de reação para todas as condições testadas. / A study of the effect of the concentrations of SO2 in its absorption by limestones in fluidized bed furnaces was conducted. For the determination of the SO2 influence on the different physical and chemical parameters of process, such as calcinations and sulfatation four different atmospheres were used in the reator with concentrations of SO2 of 500, 1.000, 2.000 and 4.000 ppm. Two types of limestones were used : Dolomitico-DP and Calcitico-CI. The bench scale bubbling fluidized bed reactor had a 160 mm internal diameter and was fluidized with air at 850ºC containing the required concentration of SO2. Bed material was quartz sand (99,9%), with 385 &#956m diameter and approximately 3 Kg of mass. The limestone was introduced in samples of 50 g, in the reactor previously stabilized, and the concentration of the gases SO2, CO2, CO and O2 and their discharges in the reactor exit were continually monitored. For the recording of this parameters a data acquisition program in LabView was developed. A mathematical model was used to allow the determination of the conversion, the conversion rate and the global coefficient of reaction rate for all the tested conditions.

No description available.

Carbon capture and storage technologies are necessary to start lowering greenhouse gas emissions while continuing to utilize existing thermal power generation infrastructure. Calcium looping is a promising technology based on cyclic calcination/carbonation reactions which utilizes limestone as a sorbent. Steam is present in combustion flue gas and in the calciner used for sorbent regeneration. The effect of steam during calcination on sorbent performance has not been extensively studied in the literature. Here, experiments were conducted using a thermogravimetric analyzer (TGA) and subsequently a dual-fluidized bed pilot plant to determine the effect of steam injection during calcination on sorbent reactivity during carbonation. In a TGA, various levels of steam (0-40% vol.) were injected during sorbent regeneration throughout 15 calcination/carbonation cycles. All concentrations of steam were found to increase sorbent reactivity during carbonation. A level of 15% steam during calcination had the largest impact. Steam changes the morphology of the sorbent during calcination, likely by shifting the pore volume to larger pores, resulting in a structure which has an increased carrying capacity. This effect was then examined at the pilot scale to determine if the phase contacting patterns and solids heat-up rates in a fluidized bed were factors. Three levels of steam (0%, 15%, 65%) were injected during sorbent regeneration throughout 5 hours of steady state operation. Again, all levels of steam were found to increase sorbent reactivity and reduce the required sorbent make-up rate with the best performance seen at 65% steam.

Foi realizado um estudo sobre o efeito das concentrações de SO2 na sua absorção por calcários em fornalhas de leito fluidizado. Para observar a influência do SO2 sobre os diferentes parâmetros físicos e químicos do processo, foram criadas atmosferas compostas por quatro concentrações diferentes de SO2, que foram de 500, 1.000, 2.000 e 4.000 ppm. Utilizou-se ainda dois tipos de calcários, o Dolomítico-DP e o Calcítico-CI. O leito fluidizado borbulhante utilizado, possuía 160 mm de diâmetro interno e foi fluidizado com ar à temperatura de 850ºC, contendo SO2 na concentração desejada. Como material do leito foi utilizada areia de quartzo (99,9%), com diâmetro de 385 &#956m e aproximadamente 3,0 Kg de massa. O calcário foi adicionado em bateladas de 50 g com o reator já pré-aquecido, enquanto as variações das concentrações dos gases SO2, CO2, CO e O2 e suas descargas foram monitoradas continuamente na saída do ciclone que era utilizado para retenção do particulado fino. Para adquirir esses dados foi desenvolvido um programa em LabView. O modelo matemático escolhido possibilitou a determinação da conversão, da taxa de conversão e do coeficiente global de taxa de reação para todas as condições testadas. / A study of the effect of the concentrations of SO2 in its absorption by limestones in fluidized bed furnaces was conducted. For the determination of the SO2 influence on the different physical and chemical parameters of process, such as calcinations and sulfatation four different atmospheres were used in the reator with concentrations of SO2 of 500, 1.000, 2.000 and 4.000 ppm. Two types of limestones were used : Dolomitico-DP and Calcitico-CI. The bench scale bubbling fluidized bed reactor had a 160 mm internal diameter and was fluidized with air at 850ºC containing the required concentration of SO2. Bed material was quartz sand (99,9%), with 385 &#956m diameter and approximately 3 Kg of mass. The limestone was introduced in samples of 50 g, in the reactor previously stabilized, and the concentration of the gases SO2, CO2, CO and O2 and their discharges in the reactor exit were continually monitored. For the recording of this parameters a data acquisition program in LabView was developed. A mathematical model was used to allow the determination of the conversion, the conversion rate and the global coefficient of reaction rate for all the tested conditions.