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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: _______________________________ _______________________________ _______________________________ _______________________________ _______________________________ Study of Trona ( Sodium Sesquicarbonate) Reactivity with Sulfur Dioxide in a Simulated Flue Gas A thesis submitted to the Division of Research and Advanced Studies of the University of Cincinnati in partial fulfillment of the requirements for the degree of MASTER OF SCIENCE In the Department of Civil and Environmental Engineering of the College of Engineering 2003 by Rangesh Srinivasan B.E. Anna University, Madras, India 2000 Committee Chair: Dr. Tim C. Keener 1 Abstract In the last few years, sulfur dioxide (SO2) has been under heavy scrutiny for reduction and its emissions are being monitored very closely by both federal and state regulatory agencies. Most of the conventional flue gas desulfurization techniques are able to meet the standards but normally come with very high capital and maintenance costs and have other associated problems. Dry injection of sodium-based sorbents has gained a lot of attention in the last few years. With Dry injection, it is possible to achieve almost similar and in some cases even higher SO2 removal efficiencies than with spray dry or wet scrubbing systems. It is proposed to study the reactivity of Trona (Na2CO3.NaHCO3.2H2O) with SO2 in a simulated flue gas stream by means of an entrained flow reactor coupled with a fabric filter simulator. The objective of this study is to provide fundamental kinetic data on the effect of flue gas variables including temperature, particle size, SO2 concentration and stoichiometric ratio on removal of SO2. A drop tube reactor with a fabric filter simulator was developed to simulate sorbent injection and sorbent particle capture. Trona was found to remove SO2 from flue gas at efficiencies that were comparable to those of sodium bicarbonate under certain conditions. It was found that the different variables like temperature, SO2 concentration and especially trona particle size have a very critical effect on removal efficiency. 2 3 ACKNOWLEDGEMENTS I express my sincere thanks to my advisor Professor Tim Keener for providing me with this wonderful research opportunity. Without his guidance and encouragement I wouldn’t have been able to complete my work. I would also like to thank Dr. Soon Jai Khang and Dr. Mingming Lu for agreeing to serve on my thesis committee. I would like to thank Mr. John Mazuik at Solvay Minerals for funding this project and providing all the trona samples. Special thanks to all members of the air quality group for all their help in completing my thesis. Finally, thanks to every one of my friends who made my stay at UC a wonderful and unforgettable experience. 4 5 TABLE OF CONTENTS LIST OF TABLES ii LIST OF FIGURES iii 1. INTRODUCTION 1 1.1 Problem Statement 1 1.2 SO2 background information 2 1.3 Advantages of dry sodium-based sorbent injection 6 1.4 Project Objectives 8 2. LITERATURE REVIEW 9 2.1 Literature Overview 9 3. EXPERIMENTAL SETUP 18 3.1 Entrained Flow Reactor 18 3.2 Sorbent Feeder 21 3.3 Operating Conditions 22 3.4 Experimental Procedure 23 4. RESULTS 26 4.1 Effect of Particle Size on SO2 Removal 26 4.2 Effect of Temperature on SO2 Removal 31 4.3 Effect of Inlet Gas SO2 Concentration on Overall SO2 Removal 36 i 4.4 Effect of Stoichiometric Ratio on SO2 Removal 40 4.5 Model 42 5. CONCLUSIONS AND FUTURE WORK 49 6. REFERENCES 51 APPENDIX 1 EXPERIMENTAL DATA 53 APPENDIX 2 MODEL CALCULATIONS 63 APPENDIX 3 MODEL CALCULATIONS 66 ii LIST OF TABLES Table 1. Flue gas composition 22 Table 2. List of Equipment 23 Table 3. T-200 particle size distribution 27 Table 4. T-200 : Mean mass diameter of particles 28 iii LIST OF FIGURES Fig. 1. Schematic of a dry sodium injection system in a coal fired power plant. 8 Fig. 2. Comparison of nahcolite and trona (200 mesh, A/C : 2.3). 10 Fig. 3. Effect of trona particle size on SO2 removal (A/C : 2.3). 11 Fig. 4. Variation of conversion with time (Temperature : 150 C, SO2 concentration : 3500 ppm). 12 Fig. 5. Variations of conversion of spray dried soda with time at lower temperatures. 12 Fig. 6. SO2 removal with trona (O : Pittsburgh seam coal(1.6 % S, 59 mm sorbent) ; D : West Virginia coal(3.1 % S, 32 mm sorbent)). 13 Fig. 7. Results of a pilot plant dry scrubbing demonstration study using NaHCO3. 15 Fig. 8. Comparison of SO2 removal using trona and sodium bicarbonate. 16 Fig. 9. Effect of stoichiometric ratio on SO2 removal. 17 Fig. 10. Comparison of sorbent costs. 17 Fig. 11. Drop tube reactor schematic. 19 Fig. 12. Drop Tube Reactor. 19 Fig. 13. Fabric Filter Simulator. 20 Fig. 14. Sorbent Feeder System. 21 Fig. 15. Conversion at different stoichiometric ratios (Temperature = 300 F ; Inlet SO2 concentration = 500 ppm ; Particle Size = <38µ). 29 Fig. 16. Effect of particle size on conversion at different stoichiometric ratios (Temperature = 300 F ; Inlet SO2 concentration = 500 ppm). 29 iv Fig. 17. Comparison of conversion at a higher stoichiometric ratio. 30 Fig. 18. Comparison of conversion at a lower stoichiometric ratio. 30 Fig. 19. Conversion at different temperatures (Inlet SO2 concentration : 500 ppm; stoichiometric ratio : 2-4). 32 Fig. 20. Conversion at different temperatures (Inlet SO2 concentration : 500 ppm; stoichiometric ratio : 4-6). 33 Fig. 21. Conversion at different temperatures (Inlet SO2 concentration : 500 ppm; stoichiometric ratio : 8-10). 33 Fig. 22. Conversion at different temperatures (Inlet SO2 concentration : 1000 ppm; stoichiometric ratio : 3-6). 34 Fig. 23. Conversion at different temperatures (Inlet SO2 concentration : 1000 ppm; stoichiometric ratio : 2-4). 34 Fig. 24. Conversion at different temperatures (Inlet SO2 concentration : 1500 ppm; stoichiometric ratio : 2-4). 35 Fig. 25. Conversion at different temperatures (Inlet SO2 concentration : 1500 ppm; stoichiometric ratio = 0-3). 35 Fig. 26. Effect of S02 inlet concentration on conversion (T : 250F, SR : 2-4). 36 Fig. 27. Effect of S02 inlet concentration on conversion (T : 325F, SR : 2-4). 37 Fig. 28. Effect of S02 inlet concentration on conversion (T : 350F, SR : 2-4). 37 Fig. 29. Comparison of utilization at two different inlet SO2 concentrations (SR : 2-4). 38 Fig. 30. Utilization versus Temperature (Inlet SO2 concentration : 500 ppm). 39 Fig. 31. Utilization versus Temperature (Inlet SO2 concentration : 1000 ppm). 39 Fig. 32. Utilization versus Temperature (Inlet SO2 concentration : 1500 ppm). 40 v Fig. 33. Effect of stoichiometry on conversion (Temperature : 275 F; Inlet SO2 concentration : 500 ppm). 41 Fig. 34. Effect of stoichiometry on conversion (Temperature : 300 F; Inlet SO2 concentration : 500 ppm) 41 Fig. 35. Effect of stoichiometry on conversion (Temperature : 250 F; Inlet SO2 concentration : 1500 ppm). 42 Fig. 36. Shrinking core of NaHCO3 and varying exposure times of Na2CO3. 43 Fig. 37. Pore plugging model fit (Inlet SO2 concentration : 500 ppm). 46 Fig. 38. Pore plugging model fit with actual data (Inlet SO2 concentration : 500 ppm). 46 Fig. 39. X¥ versus temperature at different stoichiometric ratios (Inlet SO2 concentration = 500 ppm). 47 Fig. 40. X¥ versus temperature at different stoichiometric ratios (Inlet SO2 concentration = 1500 ppm). 48 vi 1. INTRODUCTION 1.1 Problem Statement Sulfur dioxide (SO2) is arguably the most important pollutant on EPA’s list of six criteria pollutants and reduction in SO2 emissions remains the main focus of EPA’s strategy for cleaner air. SO2 has been associated with health effects ranging from respiratory illnesses to acute and chronic heart and lung disorders. It is also a primary contributor to the formation of particulate matter and acid rain. Ever since the 1990 amendments to the clean air act that revamped air quality management in the United States, there has been a constant effort to research and determine not only economical but more effective technologies for the control of the criteria pollutants, especially SO2. With an emphasis to build new power generation facilities, a majority of which would use coal, this has become all the more pertinent. FGD systems can be classified into wet limestone processes, semi-dry processes that include spray dry lime/limestone injection and dry processes that use sodium or calcium based sorbents. In the last few decades, dry flue gas desulfurization using sodium sorbents like sodium carbonate, sodium bicarbonate and trona has been identified to be a highly efficient process. Dry injection is advantageous because of the simplicity of the process and ease of retrofit with power plants already equipped with bag house filters. At the same time, it also solves disposal problems that are normally associated with wet FGD systems. There has been a lot of research done on the removal of SO2 using sodium bicarbonate (NaHCO3). Studies have shown that more than 90 % SO2 removal can be achieved with sodium bicarbonate even at low stoichiometric ratios. On the contrary, very little work has been done to study SO2 removal using trona. Trona is naturally occurring sodium sesquicarbonate with a chemical compositon as shown. 1 Chemical Formula: (Na2CO3·NaHCO3·2H2O) Composition: Molecular Weight = 226.03 gm Sodium (Na) : 30.51 % Hydrogen (H) : 2.23 % Carbon (C) : 10.63 % Oxygen (O) : 56.63% The largest pure deposit of trona in the United States lies underground near Green River, Wyoming. T-200, which is a natural form of sodium sesquicarbonate, costs less than sodium bicarbonate and has been found to have removal rates of upto 90% for SO2 [1]. It is currently being used in a variety of industries including utilities, municipal waste, chemical and cement plants.
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  • Phase Relations of Nahcolite and Trona at High P-T Conditions

    Phase Relations of Nahcolite and Trona at High P-T Conditions

    Journal of MineralogicalPhase and relationsPetrological of nahcolite Sciences, and Volume trona 104, page 25─ 36, 2009 25 Phase relations of nahcolite and trona at high P-T conditions *,** * Xi LIU and Michael E. FLEET *Department of Earth Sciences, University of Western Ontario, London, ON N6A 5B7, Canada **School of Earth and Space Sciences, Peking University, Beijing 100871, P.R. China Using cold-seal hydrothermal bomb and piston-cylinder apparatus, we have carried out both forward and rever- sal experiments to investigate the phase boundary between nahcolite (NaHCO3) and trona (NaHCO3⋅Na2CO3⋅ 2H2O). We found that the temperature of this phase boundary remains low at least up to 10 kbar, so that this phase transformation maintains its univariant nature in our investigated P-T space. The locus of this phase - boundary in a log(pCO2) T space is defined as log(pCO2) = 0.0240(±0.0001)T – 9.80(±0.06) (with pCO2 in bar and T in K), in excellent agreement with earlier 1 atm experiments at different partial pressures of CO2 (pCO2) and theoretical calculation. Using this equation and literature thermodynamic data, the entropy of trona at 298.15 K is constrained to be 303.8 J mol−1 K−1, essentially identical to earlier estimates from different methods. Our experimental results have also been used to constrain the genesis of nahcolite in some fluid inclusions of diverse origins, and it is suggested that nahcolite in these occurrences is most likely a daughter mineral which crystallized from the fluids as temperature decreased, rather than an accidentally trapped phase. Keywords: Nahcolite, Trona, Phase relations, Entropy, Fluid inclusions INTRODUCTION 2002).