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High temperature reactive separation process for combined carbon dioxide and sulfur dioxide capture from flue gas and enhanced hydrogen production with in-situ carbon dioxide capture using high reactivity calcium and biomineral sorbents

Iyer, Mahesh Venkataraman
http://rave.ohiolink.edu/etdc/view?acc_num=osu1135961929

Abstract Details

2006, Doctor of Philosophy, Ohio State University, Chemical Engineering.
Carbon dioxide separation is the most expensive step of the three-fold carbon management program of separation, transportation and sequestration. This study describes a novel high temperature reactive separation process using CaO fines for capturing carbon dioxide from flue gas. CaO reacts with carbon dioxide to form calcium carbonate, which is then regenerated back by calcining to give a pure carbon dioxide stream and the CaO. High reactivity CaO obtained from mesoporous Precipitated Calcium Carbonate (PCC), synthesized using surface modifiers, demonstrates superior performance over naturally occurring limestone such as Linwood Carbonate (LC) and dolomite. Life cycle testing of the PCC sorbent shows a capture capacity of 40-36 wt% over 50-100 Carbonation-Calcination Reaction cycles, which is significantly higher than most of the other high temperature sorbents reported in literature. The presence of sulfur dioxide in flue gas causes the parasitic sulfation reaction. Kinetic investigations of the simultaneous carbonation and sulfation reactions of the PCC-CaO were conducted for varying parameters such as residence time, reaction temperatures (500-700 °C) and sulfur dioxide concentrations (100-3000 ppm). They reveal the existence of a maximum in the ratio of extent of carbonation to that of sulfation for increasing residence time. Process analyses reveal that the CCR process is more energy efficient and economical as compared to several commercially available processes. Enhancement in the production of high purity hydrogen from fuel gas, obtained from coal gasification, is limited by thermodynamics. However, this constraint can be overcome by concurrent water-gas shift (WGS) and carbonation reactions to enhance H2 production by incessantly driving the equilibrium-limited WGS reaction forward and in-situ removing the CO2 product from the gas mixture. Experimental evidence at 600 °C demonstrates that PCC-CaO performance dominates over that of naturally occurring limestone sorbents resulting in a pure hydrogen stream. Chicken eggshell, a bioceramic composite rich in calcium, offers a unique combination of particle strength, reactivity towards carbonation and cost. Chemically treated refuse eggshells can be used as high reactivity agglomerated calcium sorbents thereby resolving the engineering challenges for the commercial deployment of the CaO fines based CCR process.
Liang-Shih Fan (Advisor)
282 p.
CO2 Capture; SO2 Capture; Carbonation; Sulfation; Calcium Oxide Sorbents; Enhanced Hydrogen Production; Chicken Eggshell sorbent; Water Gas Shift Reaction; Multicyclic testing

Recommended Citations

Citations

  • Iyer, M. V. (2006). High temperature reactive separation process for combined carbon dioxide and sulfur dioxide capture from flue gas and enhanced hydrogen production with in-situ carbon dioxide capture using high reactivity calcium and biomineral sorbents [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1135961929

    APA Style (7th edition)

  • Iyer, Mahesh. High temperature reactive separation process for combined carbon dioxide and sulfur dioxide capture from flue gas and enhanced hydrogen production with in-situ carbon dioxide capture using high reactivity calcium and biomineral sorbents. 2006. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1135961929.

    MLA Style (8th edition)

  • Iyer, Mahesh. "High temperature reactive separation process for combined carbon dioxide and sulfur dioxide capture from flue gas and enhanced hydrogen production with in-situ carbon dioxide capture using high reactivity calcium and biomineral sorbents." Doctoral dissertation, Ohio State University, 2006. http://rave.ohiolink.edu/etdc/view?acc_num=osu1135961929

    Chicago Manual of Style (17th edition)

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This open access ETD is published by The Ohio State University and OhioLINK.