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CARBON DIOXIDE SEQUESTRATION: CHEMICAL and PHYSICAL ACTIVATION of AQUEOUS CARBONATION of Mg-BEARING MINERALS and Ph SWING PROCESS

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CARBON DIOXIDE SEQUESTRATION: CHEMICAL and PHYSICAL ACTIVATION of AQUEOUS CARBONATION of Mg-BEARING MINERALS and Ph SWING PROCESS CARBON DIOXIDE SEQUESTRATION: CHEMICAL AND PHYSICAL ACTIVATION OF AQUEOUS CARBONATION OF Mg-BEARING MINERALS AND pH SWING PROCESS DISSERTATION Presented in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy in the Graduate School of The Ohio State University By Ah-Hyung Alissa Park, M.A.Sc. ***** The Ohio State University 2005 Dissertation Committee: Approved by Prof. Liang-Shih Fan, Adviser Prof. Bhavik R. Bakshi Adviser Prof. Jeffrey J. Chalmers Graduate Program in Chemical Engineering ABSTRACT According to the United States Environmental Protection Agency (US EPA), carbon dioxide, the key greenhouse gas, was emitted to the atmosphere from fossil fuel combustion in the United States at nearly 5,788 MMT in 2003, amounting to more than 80 % of the total CO2 emission in the country. The United States is also the world’s largest emitter of carbon dioxide, releasing nearly 25 % of worldwide CO2 emissions. Although policy-makers and the media frequently claim that the effects of elevated atmospheric carbon dioxide levels on global warming are uncertain, there is enough scientific evidence being mounted to support the claim that anthropogenic greenhouse gas emissions are heating the Earth’s surface. In their recent report, the National Academy of Sciences Committee testified that human activities are causing increases in surface air temperatures and subsurface ocean temperature. Thus, to ensure the continued use of fossil fuels, it is essential to reduce CO2 emissions from fossil fuel conversion plants and stabilize CO2 levels in the atmosphere. The containment of carbon dioxide involves several steps including CO2 separation, transportation, and sequestration. This study addresses the sequestration step, employing mineral carbonation. Specifically, mechanistic and kinetic characteristics of aqueous ii carbonation of Mg-bearing minerals, which underline the methodology development for mineral sequestration of CO2, were explored. Mineral carbonation is achieved through mimicry of natural inorganic chemical transformation of CO2, such as the weathering of rocks and dissolution of CO2 in seawater/saline waters to form bicarbonates. This sequestration process presents a safe and permanent method of CO2 containment that is based on chemical fixation of CO2 in the form of geologically and thermodynamically stable mineral carbonates. The total accessible amounts of the Mg-bearing minerals were estimated to significantly exceed the worldwide coal reserves. However, little has been known regarding the fundamental characteristics of CO2-mineral reactions to allow a viable CO2 mineral sequestration technology to be developed. Screening of mineral samples for their application in the CO2 mineral sequestration scheme identified both olivine and serpentine to be the viable candidates. According to the experimental results, the chemically enhanced aqueous carbonation of serpentine showed promising results. From the investigation of serpentine dissolution in various solvents, it was found that a mixture of 1 vol% orthophosphoric acid, 0.9 wt% of oxalic acid, and 0.1 wt% EDTA greatly enhanced the Mg leaching process of ground serpentine while preventing the precipitation of Fe(III) on the surface of the mineral particles. When this acidic solvent was used for the aqueous mineral carbonation, the overall process was limited by the rates of dissolution of CO2 and dissociation of carbonic acid, rather than the dissolution rate of the mineral. iii Next, the effect of the physical activation on the dissolution of serpentine was investigated and a pH swing scheme was developed to improve the overall conversion of the CO2 mineral sequestration process. Various methods of the surface agitation such as ultrasound, acoustic, and internal grinding were examined for their effectiveness in removing the diffusion limiting SiO2 layer in order to promote further dissolution of the inner Mg layer of serpentine. It was found that the fluidization of the serpentine slurry with glass beads was most effective in refreshing the surface of the serpentine particles during the dissolution process. Compared to the external attrition grinding, this method is much less energy intensive. It was also found that the mechanical agitation via the internal grinding alone did not enhance the dissolution of serpentine, while the combination of the internal grinding and Mg-leaching solvent resulted in rapid serpentine dissolution. Using the proposed pH swing scheme, the overall conversion of the mineral carbonation was radically improved. By controlling the pH of the system, three solid products were generated: SiO2-rich solids, iron oxide and MgCO3·3H2O. Since the iron oxide and magnesium carbonate produced were highly pure, these value-added products could eventually reduce the overall cost of the carbon sequestration process. In addition, it was found that the Mg-rich solution prepared during the pH swing process was also effective at removing SO2 from flue gas. Consequently, there is a potential application of this process for a multi-pollutant control system. Finally, in order to completely evaluate the proposed mineral carbonation process for the CO2 sequestration, a life-cycle assessment (LCA) was performed using iv an appropriate system boundary. According to the LCA results, a lower reaction temperature is desired, since most of the energy requirement came from heating the reactor. In addition, it was important to identify and ensure the use of three valuable byproducts in order to carry out the proposed carbon sequestration process as a net consumer of carbon dioxide. v To my parents and brothers for their love and support vi ACKNOWLEDGMENTS I would like to express my sincere gratitude to my adviser, Professor Liang-Shih Fan, for his priceless guidance, encouragement, and support throughout this work. His enthusiasm and drive has been a constant source of inspiration. His patience and indulgence gave me ample time and space to mature not only as a researcher but also as an individual. As I stand at the starting point of my career, I truly appreciate experiencing his passion for research and love for his students. I will always carry the pride in my heart knowing I was a member of Professor Fan’s research group. Thanks also go to Professors Bhavik R. Bakshi, Jeffrey J. Chalmers, David L. Tomakso, Shang-Tian Yang, and Jack L. Zakin for their helpful suggestions and valuable comments. The useful discussion, support, and cooperation from other members in our research group are greatly appreciated. Particularly, I would like to thank Drs. Raja Jadhav, Himanshu Gupta, Raymond Lau, and Ted Thomas for their encouragements and assistance. I also want to express my gratitude to Dr. Bing Du, Dr. Zhe Cui, Yang Ge, Puneet Gupta, Mahesh Iyer, Bartev Sakadjian, Luis Velazquez- Vargas, and William Wang for their assistance and friendship. In addition, I would like to thank two of my undergraduate research assistants, Imogen Pryce and Ee Hui Tan, for their hard work and friendship. It is a pleasure to acknowledge many people in the vii Department of Chemical and Biomolecular Engineering including Leigh Evrard, Paul Green, Ibra Ndoye, Carl Scott, and Sherry Stoneman, who became good friends of mine over the last five years. Most of all, I would like to thank my family for their everlasting love and support. I would like to dedicate this thesis to my parents, Jin Park and Hee-Sup Yoon, who believed in me and gave me the opportunity to be who I really wanted to be, and also to my brothers, Jae-Hyung and Si-Hyung, who are the strength of my everyday triumph, for their continued faith in me. viii VITA March 12, 1973....………………………….. Born – Seoul, Korea September 1995 − May 1998...………….…. B.A.Sc. Chemical Engineering University of British Columbia Vancouver, BC, Canada September 1998 − August 2000...……….…. M.A.Sc. Chemical Engineering University of British Columbia Vancouver, BC, Canada September 2000 − present………………….. Graduate Research Associate Chemical and Biomolecular Engineering The Ohio State University Columbus, OH, USA PUBLICATIONS 1. Park, A.-H. A., Lackner, K. S., and L.-S. Fan, “Carbon Dioxide Capture and Disposal: Carbon Sequestration,” Encyclopedia of Chemical Processing, Ed. K. B. Kim, Marcel Dekker, Inc., (2005). 2. Park, A.-H. A., and L.-S. Fan, “Fluidization,” Encyclopedia of Chemical Processing, Ed. K. B. Kim, Marcel Dekker, Inc., (2005). 3. Park, A.-H. A., and L.-S. Fan, “CO2 Mineral Sequestration: Physically Activated Aqueous Carbonation of Serpentine and pH Swing process”, Chem. Eng. Sci., 59, 5241-5247, (2004). ix 4. Cui, Z., Fan, J., and Park, A.-H. A., “Drag Coefficients for Settling Sphere with Microbubble Drag Reduction Effects”, Powder Technology, 138 (2-3), 132-134, (2003). 5. Park, A.-H. A., Jadhav, R., and L.-S. Fan, “CO2 Mineral Sequestration: Chemically Enhanced Aqueous Carbonation of Serpentine”, CJChE, 81 (3-4), 885-890, (2003). 6. Yao, L., Bi, H. T., and Park, A.-H. A., “Electrostatic Charges in Freely Bubbling Fluidized Beds with Dielectric Particles”, J. Electrostatics, 56, 183-197, (2002). 7. Park, A.-H. A., Bi, X., and Grace, J. R., “Reduction of Electrostatic Charges in Gas- Solid Fluidized Bed”, Chem. Eng. Sci., 57, 53-162, (2002). 8. Park, A.-H. A., Bi, X., Grace, J. R., Chen, A. H., “Modeling Electrostatic Charge Transfer in Gas-Solids Fluidized Beds”, J. Electrostatics., 55, 135-168, (2002). 9. Lee, H., Park, A.-H. A., and Oloman, C., “Stability of Hydrogen Peroxide in Sodium Carbonate Solutions”, TAPPI J., 83(8), 94-101,
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