To achieve net-zero emissions by the year 2050, carbon capture, utilization and storage technologies must be implemented to decarbonize sectors with hard-to-abate emissions. Pressurized chemical looping (PCL) with a novel reactor design called a plug flow with internal recirculation (PFIR) fluidized bed reactor is proposed as an attractive carbon capture technology to decarbonize small- and medium-scale emitters. The objective of this work was to examine solid circulation rate, gas leakage between reactors, and purge gas fate in a cold flow chemical looping facility. These parameters were used to better understand the PFIR reactor and will be used to validate a computational particle fluid dynamic (CPFD) model of the PFIR reactor to inform the reactor operation and design for a hot flow PCL pilot plant. An energy balance across the fuel reactor was used to determine the solid circulation rate of the bed material, while helium and argon tracer gases were used to determine the amount of gas leaking between reactor sections and the fate of the purge gas, respectively. Statistical analyses were completed to determine the statistical significance of the data. At the base case condition, the solid circulation rate was 3000 kg/h. Approximately 10% of the fluidizing gas that entered the air reactor moved to the fuel reactor indicating that, with reacting flow, there will be nitrogen infiltrating the fuel reactor, decreasing the purity of the carbon dioxide effluent stream. Furthermore, approximately 31% of the fluidizing gas entering the fuel reactor moved to the air reactor, indicating that, with reacting flow, there will be natural gas leaking into the air reactor, which will increase carbon dioxide emissions. Finally, over half of the purge gases move to the adjacent reactor, which helps prevent gas leakage between reactor sections. The effect of static bed height, weir opening height and purge configuration on solid circulation rate, gas leakage and purge fate were investigated. The bed height has a small effect on the solid circulation rate and no effect of gas leakage, over the range of bed heights tested. Furthermore, increasing the weir opening height increases both solid circulation rate and gas leakage until the top of the circulation zone is reached. After this point, there is no change in either solid circulation rate or gas leakage. In terms of purge configuration, there appears to be no benefit for having two purge rows. Either one purge row or having a row of blanked tuyeres appear to be optimal as they decrease gas leakage, while having little effect on solid circulation rate. At the jet velocity tested, the vertical purge configuration prevented the solids from circulating, so it is not recommended for this purge configuration to be used in a PFIR reactor without further testing of different jet velocities. Across all configurations, it was shown that as more purge gas moves into the adjacent reactor section, less gas leakage between reactor sections occurs. It iii was also determined that the primary method of gas movement between the reactor sections is likely via bubbles and/or jets. The next step is to complete the validation of CPFD model of the PFIR reactor using the data presented herein. Additional conditions can also be run in the cold flow chemical looping pilot facility to fill in any gaps that are found during the CPFD model validation, or to fill in research gaps in better understanding the PFIR reactor.

As a carbon neutral and renewable source of energy, biomass carries a high potential to help sustain the future energy demand. The co-firing of coal and biomass mixtures is an alternative fuel route for the existing coal based reactors. The main challenges associated with co-firing involves proper understanding of the co-firing behavior of blended coal-biomass fuels, and proper understanding of advanced gasification systems used for converting such blended fuels to energy. The pyrolysis and combustion behavior of coal-biomass mixtures was quantified by devising laboratory experiments and mathematical models. The pyrolysis-combustion behavior of blended fuels was quantified on the basis of their physicochemical, kinetic, energetic and evolved gas behavior during pyrolysis/combustion. The energetic behavior of fuels was quantified by applying mathematical models onto the experimental data to obtain heat of pyrolysis and heat of combustion. Fuel performance models were developed to compare the pyrolysis and combustion performance of non-blended and blended fuels. The effect of blended fuel briquetting was also analyzed to find solutions related to coal and biomass co-firing by developing a bench scale fuel combustion setup. The collected data was analyzed to identify the effects of fuel blending and briquetting on fuel combustion performance, ignitability, flammability and evolved pollutant gases. A further effort was made in this research to develop the understanding of fluidized bed hydrodynamics. A lab scale cold-flow fluidized bed setup was developed and novel non-intrusive techniques were applied to quantify the hydrodynamics behavior. Particle Image Velocimetry and Digital Image Analysis algorithms were used to investigate the evolution of multiple inlet gas jets located at its distributor base. Results were used to develop a comprehensive grid-zone phenomenological model and determine hydrodynamics parameters such as jet particle entrainment velocities and void fraction among others. The results were further used to study the effect of fluidization velocity, particle diameter, particle density, distributor orifice diameter and orifice pitch on the solid circulation in fluidized beds. / Ph. D.