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Study of Trona ( Sodium Sesquicarbonate)

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Study of Trona ( Sodium Sesquicarbonate) UNIVERSITY OF CINCINNATI Date:___________________ I, _________________________________________________________, hereby submit this work as part of the requirements for the degree of: in: It is entitled: This work and its defense approved by: Chair: _______________________________ _______________________________ _______________________________ _______________________________ _______________________________ A Modeling and Experimental Study of the Conversion of Trona to Increase Its Reactivity with SO2 in Dry Injection System A dissertation submitted to the Division of Research and Advanced Studies of the University of Cincinnati in partial fulfillment of the requirements for the degree of DOCTORATE OF PHILOSOPHY (Ph.D.) In the Department of Civil and Environmental Engineering of the College of Engineering 2007 by Kyungmin Jacob Cho M.S. Hankuk University of Foreign Studies, Korea, 2000 B.S. Hankuk University of Foreign Studies, Korea, 1998 Committee Chair: Dr. Tim C. Keener ABSTRACT The first objective of this study was to develop a cost‐effective method of converting Na2CO3 fraction of parent trona to NaHCO3 to achieve more efficient removal of SO2 in dry injection systems. The conversion experiment was performed by varying the level of water vapor, partial pressure of CO2, and reaction temperature in a pressurized reactor in order to produce modified trona. While temperature, reaction time and partial pressure of CO2 had a little effect, water vapor level significantly affected the conversion process. Then, the reaction of SO2 with parent and modified trona was studied using an entrained flow reactor under simulating flue gases at the temperature of ~177oC while varying the stoichiometric ratio of trona to SO2 from 0.4 to 2.5. The experimental results indicated that modified trona is more efficient in removing SO2 compared to parent trona at the tested stoichiometric ratio of 1.0 and 2.0, with a larger enhancement (15%) observed at the stoichiometric ratio of 2.0. Also, modified trona was observed to have better SO2 removal efficiency in all the particle size ranges, with a larger enhancement (47%) measured in the size range of 75μm < dp <125μm. Based on the result of the conversion experiment, three different models such as the unreacted shrinking core model (the USC model), the grain model, and the deactivation model for the conversion reaction of trona to NaHCO3 were compared to explain kinetics underlying the conversion reaction. In those models, the deactivation model was shown good agreement with the experimental data obtained from the conversion reaction of trona to NaHCO3. It gave the value of 0.94 as an average correlation coefficient with the experimental data. Two different reaction mechanisms were observed as temperature increased because it might be heat transfer effect in exothermic reaction. Finally, based on the kinetics and mechanism of how trona decomposes to Na2CO3 as it reacts with SO2 in a fabric filter collector, a model for SO2 removal by trona injection in a fabric filter collector was proposed. The model incorporates a simplified pore plugging reaction rate expression, a parallel reaction scheme based on the shrinking core model, and a plug flow reactor model. The model shows good agreement with experimental data using parent and modified trona and provides quantitative indications of system performance as a function of a change in SO2 concentration, experimental temperature, stoichiometric ratio, and the amount of NaHCO3. ACKNOWLEDGEMENT First of all, I would like to express my deepest gratitude to my advisor, Dr. Tim. C. Keener, for his continuous support, guidance and motivation throughout my Ph. D. study. I also would like to take this opportunity to thank my dissertation committee, Dr. Soon‐Jai Khang, for his constructive suggestions, time and effort that significantly helped me with the modeling part of my dissertation, Dr. Mingming Lu and Dr. George Sorial for serving in my dissertation committee. Special thanks go to Solvay Company, in particular to Mr. John Maziuk for partial funding this project and providing all trona. In addition, I would like to thank the members of our research group who have supported and provided me help and friendship over the years. Finally, I would like to thank my parents and family who have supported me throughout my education. This dissertation is dedicated especially to them. TABLE OF CONTENTS CHAPTER 1. Introduction to Flue Gas Desulfurization ..................................................... 1 ABSTRACT ..................................................................................................................................... 2 1.1. Coal Consumption ................................................................................................................... 4 1.2. Acid Rain SO2 Reduction Program .......................................................................................... 8 1.3. Flue Gas Desulfurization (FGD) Technology ........................................................................... 9 1.3.1. Wet FGD Technology ................................................................................................... 11 1.3.2. Dry FGD Technology ................................................................................................... 12 1.4. Sorbents .................................................................................................................................. 13 1.5. Research Objectives ................................................................................................................ 16 1.6. References ............................................................................................................................... 17 CHAPTER 2. Conversion of Trona to Sodium Bicarbonate ............................................. 20 ABSTRACT ................................................................................................................................... 21 2.1. Introduction ............................................................................................................................ 23 2.1.1. Sulfation of Trona ......................................................................................................... 24 2.1.2. Conversion of Ttona ..................................................................................................... 27 2.2. Experimental Prodedure ........................................................................................................ 29 2.2.1. Materials ....................................................................................................................... 29 2.2.2. Experimental Procedure ............................................................................................... 29 2.2.3. Scanning Electron Microscopy ..................................................................................... 33 2.2.4. Measurement of SO2 Removal Efficiency .................................................................... 33 2.3. Results and Discussion ........................................................................................................... 37 2.3.1. Effect of temperature .................................................................................................... 37 2.3.2. Effect of reaction time .................................................................................................. 39 2.3.3. Effect of CO2 pressure .................................................................................................. 41 2.3.4. Effect of water vapor .................................................................................................... 44 2.3.5. Indentification of the final product produced by the conversion ................................ 48 2.3.6. Removal efficiency ....................................................................................................... 53 2.3.6.1. Effect of molar ratio .......................................................................................... 53 2.3.6.2. Effect of temperature ........................................................................................ 56 2.3.6.3. Effect of particle size ........................................................................................ 59 2.3.7. SEM observation .......................................................................................................... 63 2.4. Conclusions ............................................................................................................................ 64 2.5. References ............................................................................................................................... 66 i CHAPTER 3. Modeling for Dry Injection Process using Trona ...................................... 69 ABSTRACT ................................................................................................................................... 70 3.1. Introduction ............................................................................................................................ 71 3.1.1. Reaction of trona with SO2 ........................................................................................... 72 3.2. Model Development ............................................................................................................... 74 3.2.1. Conversion of trona to grainy material ........................................................................ 77 3.2.2. Duct Section.................................................................................................................
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