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Study on the Desulfurization Characteristic of Limestone Depending on the Operating Parameters of In-Furnace Desulfurization for Oxy-Fuel Combustion Using Drop Tube Furnace

순산소연소 조건에서 Drop tube furnace를 이용한 운전변수에 따른 석회석의 탈황특성 연구

  • Published : 2011.12.01

Abstract

Oxy-fuel combustion with many advantages such as high combustion efficiency, low flue gas flow rate and low NOx emission has emerged as a promising CCS technology for coal combustion facilities. In this study, the effects of the direct sulfation reaction on $SO_2$ removal efficiency were evaluated in a drop tube furnace under typical oxy-fuel combustion conditions represented by high concentrations of $CO_2$ and $SO_2$ formed by gas recirculation to control furnace combustion temperature. The effects of the operating parameters including the reaction temperature, $CO_2$ concentration, $SO_2$ concentration, Ca/S ratio and humidity on $SO_2$ removal efficiency were investigated experimentally. $SO_2$ removal efficiency increased with reaction temperature up to 1,200 due to promoted calcination of limestone reagent particles. And $SO_2$ removal efficiency increased with $SO_2$ concentrations and the humidity of the bulk gas. The increase of $SO_2$ removal efficiency with $CO_2$ concentrations showed that $SO_2$ removal by limestone was mainly done by the direct sulfation reaction under oxy-fuel combustion conditions. From the impact assessment of operation parameters, it was shown that these parameters have an effects on the desulfurization reaction by the order of the Ca/S ratio > residence time > $O_2$ concentration > reaction temperature > $SO_2$ concentration > $CO_2$ concentration > water vapor. The semi-empirical model equation for to evaluate the effect of the operating parameters on the performance of in-furnace desulfurization for oxy-fuel combustion was established.

순산소연소는 높은 연소 효율과 적은 배가스량, 낮은 질소산화물 농도를 장점으로 하고 있으며 연소온도 조절을 위한 배가스 재순환에 의해 배출되는 연소가스중의 $CO_2$ 농도를 95%까지 농축이 가능하므로 석탄 연소설비에 대한 유망한 CCS 기술로 부각되고 있다. 본 연구는 순산소연소 조건에서 배가스의 재순환을 통한 $CO_2$ 농도 증가에 기인하는 직접 황화반응이 탈황효율에 미치는 영향을 평가하고 반응온도, $CO_2$ 농도, $SO_2$ 농도상승이 $SO_2$ 제거효율에 미치는 영향과 배가스 중 수분 등이 $SO_2$ 제거효율에 미치는 영향을 실험적으로 고찰하였다. 반응온도 $1,200^{\circ}C$까지 온도 상승에 따라 $SO_2$의 제거효율은 증가하였고 Ca/S비, $CO_2$ 농도와 수분이 증가할수록 $SO_2$ 제거효율이 증가하였다. 이러한 운전변수는 영향인자 평가를 통하여 Ca/S 비>체류시간>$O_2$농도>반응온도>$SO_2$농도>$CO_2$농도>수분농도의 순으로 탈황반응에 영향을 미치는 것으로 나타났다. 또한 운전변수별 실험결과를 이용하여 로내 건식탈황에 있어서 각 운전변수별 성능 영향인자를 평가할 수 있는 반경험적 모델식을 도출하였다.

Keywords

References

  1. An, Y. M., Jo, H. D., Park, Y. S., Keel, S. I. and Lee, H. K., "Study on the In-Furnace Desulfurization for Oxy-Fuel Combustion Flue Gases Using Drop Tube Furnace," Korea Chem. Eng. Res. (HWAHAK KONGHAK), 47(4),512-517(2009).
  2. An, Y. M., Jo, H. D., Park, Y. S., Keel, S. I. and Lee, H. K., "Study on Calcination Characteristics of Limestones for In-furnace Desulfurization in Oxy-Fuel Combustion," Korea Society of Environmental Eng., 31(5), 371-377(2009).
  3. Buhre, B. J. P., Elliott, L. K., Sheng, C. D., Gupta, R. P. and Wall, T. F., "Oxy-fuel Combustion Technology for Coal-fired Power Generation," Prog. Energy Combus. Sci., 31(4), 283-307(2005). https://doi.org/10.1016/j.pecs.2005.07.001
  4. Tan, Y., Croiset, E., Douglas, M. A. and Thambimuthu, K. V., "Combustion Characteristics of Coal in a Mixture of Oxygen and Recycled Flue Gas," Fuel, 85(4), 507-512(2006). https://doi.org/10.1016/j.fuel.2005.08.010
  5. Lee, H. K., "Flue Gas Desulfurization," J. SAREK, 36(12), 34- 41(2007).
  6. Cheng, J., Zhou, J., Liu, L., Zhou, Z., Huang, Z., Cao, X., Zhao, Z. and Cen, K., "Sulfur Removal at High Temperature During Coal Combustion in Furnaces: a Review," Prog. Energy Combus. Sci., 29(5), 381-405(2003). https://doi.org/10.1016/S0360-1285(03)00030-3
  7. Snow, M. J. H. and Long, J. P., "Direct Sulfation of Calcium Carbonate," Ind. Eng. Chem. Res., 27(2), 268-273(1988). https://doi.org/10.1021/ie00074a011
  8. Han, K. H., Song, Y. S., Ryu, J. I., Son, J.-E. and Jin, G.-T., "The Characteristics of $SO_{2}$ Emission with Korean Anthracite in a Pressurized Fluidized Bed Combustor," HWAHAK KONGHAK, 41(1), 86-92(2003).
  9. Zhong, Q., "Direct Sulfation Reaction of $SO_{2}$ with Calcium Carbonate," Thermochimica acta, 260, 125-136(1995). https://doi.org/10.1016/0040-6031(95)90486-7
  10. Liu, H., Katagiri, S. and Okazaki, K., "Drastic SOx Removal and Influences of Various Factors in $O_{2}/CO_{2}$ Pulverized Coal Combustion System," Energy Fuels, 15(2), 403-412(2000).
  11. Chen, C. and Zhap, C., "Calcination and Sintering Characteristics of Limestone Under $O_{2}/CO_{2}$ Combustion Atmosphere," Fuel process. Technol., 88(2), 171-178(2007). https://doi.org/10.1016/j.fuproc.2006.03.003
  12. Chen, C. and Zhap, C., "Mechanism of Highly Efficient In-Furnace Desulfurization by Limestone under $O_{2}/CO_{2}$ Coal Combustion Atmosphere," Ind. Eng. Chem. Res., 45, 5078-5085(2006). https://doi.org/10.1021/ie060196x
  13. Liu, H., Katagiri, S. and Okazaki, K., "Decomposition Behavior and Mechanism of Calcium Sulfate Under the Condition of $O_{2}/CO_{2}$ Pulverized Coal Combusion," Chem. Eng. Comm, 187, 199- 214(2001). https://doi.org/10.1080/00986440108912888
  14. Zeman, F., "Effect of Steam Hydration on Performance of Lime Sorbent for $CO_{2}$ Capture," Int. J. Greenhouse Gas Control., 2(2), 203-209(2007).
  15. Cheng, J., Zhou, J., Liu, L., Zhou, Z., Huang, Z., Cao, X., Zhao, Z. and Cen, K., "Sulfur Removal At High Temperature During Coal Combustion in Furnaces: a Review," Prog. Energy Combus. Sci., 29(5), 381-405(2003). https://doi.org/10.1016/S0360-1285(03)00030-3
  16. Oh, K. J., Hong, S. C., Kim, J. Y. and Do, D. S., "The Effect of Limestone Properties on Desulfurization in a Fluidized Bed Combustor," Korea society of environmental eng., 13(1), 37-44 (1991).
  17. Yoo, K. S., Song, B. H., Kim, S. D. and Kim, K. T., "Toxic Gas Cleaning Technology Sorbents in Waste Incinerators," J. Korea Solid Wastes Engineering Society, 14(6), 611-622(1997).
  18. Gutierrez Ortiz, F. J. and Ollero, P., "Flue-Gas Desulfurization in an Advanced in-Duct Desulfurization Process: An Empirical Model from an Experimental Pilot-Plant Study," Ind. Eng. Chem. Res. 42(25), 6625-6637(2003). https://doi.org/10.1021/ie030185t

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