Browse > Article

Effect of $SO_2$ on DeNOx by Ammonia in Simultaneous Removal of SOx and NOx over Activated Coke  

Kim, Hark-Joon (Department of Energy and Chemical Engineering Kyungnam University)
Yoon, Cho-Hee (Department of Environmental Engineering, Kyungnam University)
Publication Information
Abstract
The $SO_2$ and $NO_x$ removal with an activated coke catalyst was conducted by a two-stage reaction which first $SO_2$ was oxidized to $H_2SO_4$ and then $NO_x$ was reduced to $N_2$. But if unreacted sulfur dioxide entered in the second stage, the $NO_x$ reduction was hindered by the reaction with ammonia. In this study, experimental investigations by using lab-scale column apparatus on the product and the reactivity of $SO_2$ with ammonia over coke catalyst which was activated with sulfuric acid was carried out through ultimate analysis DTA, TGA and SEM of catalyst before and after the reaction. Also, the effect of reaction emperature on the reactivity of $SO_2$ with ammonia was determined by means of breakthrough curves with time. The obtained results from this study were summarized as following; Activated cokes were decreased carbon component and increased oxygen and sulfur components in comparison with original cokes. The products over coke catalyst were faced fine crystal of $(NH_4)_2SO_4$, which results in the pressure loss of reacting system. The order of general reactivity in terms of the reaction temperature after breakthrough for $SO_2$ was found to be $150^{\circ}C$ > $200^{\circ}C$ > $100^{\circ}C$. This was related to adsorption amounts of ammonia on the activated cokes.
Keywords
$NO_x$ and $SO_x$ removal; Activated coke catalyst; Ammonium sulfate; Sulfur dioxide; Ammonia adsorption;
Citations & Related Records
연도 인용수 순위
  • Reference
1 Nimmo, W., Patsias,A. A., Hampartsoumian, E., Gibbs, B. M. and Williams, P. T.", Simultaneous reduction of $NO_x$ and $SO_x$ emissions from coal combustion by calcium magensium acetate", Fuel, 83, 149-155(2004).   DOI   ScienceOn
2 Guar, V., Asthana, R. and Verma, N., "Removal of $SO_2$ by activated carbon fibers in the presence of $O_2$ and $H_2O$", Carbon, 44, 46-60(2006).   DOI   ScienceOn
3 Lizzio, A. A. and Debarr, J.", Mechanism of $SO_2$ removal by carbon", Energy Fuel, 11, 284-291(1997).   DOI   ScienceOn
4 Wang, Y., Liu, Z, Zhan, L., Huang, Z., Liu, Q. and Ma, J., "Performance of an activated carbon honeycomb supported $V_2O_5$ catalyst in simultaneous $SO_2$ and NO removal,"Chem. Eng. Sci., 59, 5283-5290(2004)   DOI   ScienceOn
5 Wang, L., Li, C., Yin, H., Feng, L.,, Yu, Y. and Hou, Y.," Sulfur removal of FCC gasoline by selective adsorption over activated semi-coke", Chem. Technol. fuels oils, 45(2),85-91(2009).   DOI   ScienceOn
6 Le, L. M. and Bandosz.," The role of water surface acidity on the reactive adsorption of ammonia on modified activated carbons", Carbon, 45, 568-578(2007).   DOI   ScienceOn
7 Shawwa, A. R., Smith, W. D. and Sego, C. D., "Color and chlorinated organics removal from pulp mill wastewater using acitvated petroleum coke", Water Res., 35(3),745-749(2001).   DOI   ScienceOn
8 Ertl, G., Knozinger, H., Weitkamp, J., Environmental catalysis, 1st ed., Wiley-VCH, Weinheim, pp 142-148(1999).
9 Kiyoura, R. and Urano, K., "Mechanism, kinetics, and equilibrium of thermal decomposition of ammonium sulfate", Ind. Eng. Chem. Process Des. Develop., 9(4), 489-494(1990).
10 Kasaoka, S., Hara,Y. and Sakaoka, E., "Adsorption of mixtures of nitrogen oxide and sulfur oxide on activated carbon", Bull. Chem. Soc. Jpn., 11, 1737-1742(1977).
11 Humeres, E., Moreira, R. F. P. M. and Peruch, M.," Reduction of $SO_2$ on different carbons", Carbon, 40, 751-760(2002).   DOI   ScienceOn
12 Kasakabe, K., Kashima, M., Morooka, S. and Kato, Y.," Rate of nitric oxide with ammonia on coke catalysts activated with sulfuric acid", Fuel, 67(5), 714-718(1988).   DOI   ScienceOn
13 DiPanfilo, R. and Egiebor, N. O., "Activated carbon production from synthetic crude coke", Fuel Proc. Technol., 46, 157-169(1996).   DOI   ScienceOn
14 Yamamoto. K., Seki, M. and Kawazoe, K., "Rate of oxidation of sulfur dioxide on activated carbon surfaces", Bull. Chem. Soc. Jpn.,1046-1052(1972).
15 Yamamoto. K., Seki, M. and Kawazoe, K., "Effect of sulfuric acid accumulation on the rate of sulfur dioxide oxidation on activated carbon surface", Bull. Chem. Soc. Jpn.,1268-1279 (1973).
16 山本協子, 關道治, "活性炭に對する排中亞硫酸ガスの吸着 狀態", 工業化學雜誌", 74(8), 78-83(1971).
17 Tsuji K. and Shiraishi,I.," Combined desurfurization, denitrification and reduction of air toxics using activated coke", Fuel, 76(2), 549-560(1997).   DOI
18 Lui, Q., Li, C. and Li, Y., "$SO_2$ removal from flue gas by activated semi-cokes the temperature of catalysts and determination of operating conditions", Carbon., 41, 2217-2223 (2003).   DOI   ScienceOn
19 Lu, L., Guo, J., Jin, F. and Zeng, H.," Removal of $SO_2$ from $O_{2^{-}}$containing flue gas by ACF impregnated with $NH_3$", Chemosphere, 62, 823-826(2006).   DOI   ScienceOn
20 Olson, G. D., Tsuji, K. and Shirashi, I., "The reduction of gas phase air toxics from combustion and incineration sources using the MET-Mitsui-BF activated coke process", Fuel Proc. Technol., 65/66, 393-405(2000).   DOI   ScienceOn
21 Centi, G. and Perathoner, S.," Performances of $SO_x$ traps derived from Cu/Al hydrotalcite for the protection of $NO_x$ traps from the deactivation by sulfur", Appl. Catal., 70, 172-178 (2007).   DOI   ScienceOn
22 Li, J., Kobayashi, N. and Hu, Y.," The activated coke preperation for $SO_x$ adsorption by using flue gas from coal power plant", Chem. Eng. Proc., 47, 118-127(2008).   DOI   ScienceOn
23 Muniz, J., Marban, G. and Fuertes, A. B., "Low temperature selective catalytic reduction of NO over modified activated carbon fibers", Appl. Catal. B: Environ., 27, 27-36 (2000).   DOI   ScienceOn
24 Li, K., Ling, L., Lu, C. and Qiao, W"., Catalytic removal of $SO_2$ over ammonia-activated carbon fiber", Carbon., 39, 1803-1808 (2001).   DOI   ScienceOn
25 Mochida, I., Korai, Y., Shirahama, M., Kawano, S., Hada, T., Seo, Y., Yoshikawa, Y. and Yasutake, A., "Removal of $SO_x$ and $NO_x$ over activated carbon fibers", Carbon., 38, 227-239(2000).   DOI   ScienceOn
26 Nishijima, A., Kurita, M., Kiyozumi, Y. and Kobayashi, R., "New type active carbon catalyst for simultaneous removal of $SO_x$ and $NO_x$", Bull. Chem. Soc. Jpn., 53(11), 3356-3360(1980).   DOI   ScienceOn
27 Hong, I., Jiang, H., Park, Y. D., Kim, J. Y. and Ha, B. -H., "Metal dispersed activated carbon fibers and their application for removal of $SO_x$", Chem. Phys. Lett., 366, 572-577 (2002).   DOI   ScienceOn
28 Feng, O., Zhu, R-S., Sato, K., Haneda, M. and Hamada, H., "Promotion of surface $SO_x$ on the selective catalytic reduction of NO by hydrocarbons over $Ag/Al_2O_3$", Appl. Surf. Sci., 252, 6390-6393(2006).   DOI   ScienceOn