Adsorption of Sulfur Dioxide from Pseudo Binary Mixtures on Hydrophobic Zeolites: Modeling of the Breakthrough Curves

Adsorption - Tập 8 - Trang 279-289 - 2002
Marcus Mello1, Mladen Eić1
1Department of Chemical Engineering, University of New Brunswick, Fredericton, Canada

Tóm tắt

The adsorption of SO2 from pseudo binary mixtures with water and CO2 on hydrophobic zeolites (MFI and MOR type) was investigated using the breakthrough curve method. The SO2 and water breakthrough curves were compared with theoretical ones based on an axially dispersed plug flow through the column and the linear driving force rate equation. In addition, different semi-predictive multi-component equilibrium equations were used for the breakthrough modeling: Langmuir 1, Langmuir 2 and Langmuir-Freundlich extended models. The overall mass transfer coefficients were derived by matching theoretical with experimental breakthrough curves for single component systems, i.e., water vapor or SO2 in a carrier gas. They were also predicted from a simplified bi-porous adsorbent model and compared with experimentally derived values. The presence of CO2 species in ternary mixtures with water vapor and SO2, even at relatively high concentrations of 9 vol%, had no significant effect on the breakthrough behavior of the other two species. For that reason the CO2 species was ignored in the analysis of the resulting pseudo binary mixtures. The breakthrough model was solved by finite element orthogonal collocation method using the commercial software gPROMS. Both extended Langmuir 1 and Langmuir 2 based models gave reasonable predictions of the water and SO2 breakthrough curves for pseudo binary mixtures involving a mordenite sample for all water concentration levels used in this study (up to 3.5 vol%). However, the same models were successfully used to predict SO2 breakthrough curves for a MFI sample only at low water concentrations, i.e., 1.5 vol%. At the higher water levels both models failed to describe equilibrium behavior in the MFI sample due to the introduction of multi-layer adsorption in the interstices between small MFI-26 crystals.

Tài liệu tham khảo

Arumugam, B.K., J.F. Banks, and P.C. Wankat, “Pressure Effects in Adsorption Systems,” Adsorption, 5, 261–278 (1999). Chen, N.Y., “Hydrophobic Properties of Zeolites,” J. Phys. Chem., 80(1), 60–63 (1976). Chriswell, C.D. and D.T. Gjerde, “Sampling of Stack Gas for Sulfur Dioxide with a Molecular Sieve Adsorbent,” Anal. Chem., 54, 1911–1913 (1982). Do, D.D., Adsorption Analysis: Equilibria and Kinetics, ch. 6, Imperial College Press, London, 1998. Dunn, J.P.,Y. Cai, S. Liebmann, H.G. Stenger, Jr., and D.R. Simpson, “A Test and Demonstration Unit for Concentrating Sulfur Dioxide from Flue Gas,” Ind. Eng. Chem. Res., 35, 1409–1416 (1996). Edwards, M.F. and J.F. Richardson, “Gas Dispersion in Packed Beds,” Chem. Eng. Sci., 23, 109–123 (1968). Glueckauf, E. and J.E. Coates, “Theory of Chromatography. Part IV. The Influence of Incomplete Equilibrium on the Front Boundary of Chromatograms and on the Effectiveness of Separation,” J. Chem. Soc., 1315–1321 (1947). Gollakota, S.V. and C.D. Chriswell, “Study of an Adsorption Process Using Silicalite for Sulfur Dioxide Removal from Combustion Gases,” Ind. Eng. Chem. Res., 27(1), 139–143 (1988). Gregg, S.J. and K.S.W. Sing, Adsorption, Surface Area and Porosity, ch. 3, Academic Press, London, 1967. Ma, Y.H. and C. Mancel, “Diffusion Studies of CO2, NO, NO2 and SO2 on Molecular Sieves Zeolites by Gas Chromatography,” AIChE J., 18(6), 1148–1153 (1972). Ma, Y.H. and A.J. Roux, “Multicomponent Rates of Sorption of SO2 and CO2 in Sodium Mordenite,” AIChE J., 19(5), 1055–1059 (1973). Ma, Y.H., R.J. Byron, P. Feltri, and T.Y. Lee, “Effects of Presorbed Water Vapor upon the Sorption and Diffusion of Sulfur Dioxide in Natural Mordenites,” AIChE Symp. Ser., 74(179), 48–52 (1978). Mello, M., “Adsorption of Sulphur Dioxide from Multicomponent Mixtures on Hydrophobic Zeolites,” Ph.D. Thesis, University of New Brunswick, Canada, 2000. Mello, M., M. Eić, S. Hočevar, and U. Lavrenčič-Štangar, “Modeling of Sulfur Dioxide Breakthrough Curves from Ternary Wet Mixtures on MOR Type Zeolite,” Stu. Surf. Sci. Cat. 135; Also in Zeolites and Mesoporous Materials at the Dawn of the 21st Century, A. Galarneau, F. DiRenzo, F. Fajula, and J. Vedrine (Eds.), CD-ROM, Elsevier, Amsterdam, 2001. Nakamoto, H. and H. Takahashi, “Hydrophobic Natures of Zeolite ZSM-5,” Zeolites, 2, 67–69 (1982). Rouf, S. and M. Eić, “Adsorption of SO2 from Wet Mixtures on Hydrophobic Zeolites,” Adsorption, 4, 25–33 (1998). Roux, A., A.A. Huang, Y.H. Ma, and I. Zwiebel, “Sulfur Dioxide Adsorption on Mordenites,” AIChE Symp. Ser., 69(134), 46–53 (1973). Ruthven, D.M., Principles of Adsorption and Adsorption Processes, ch. 8, John Wiley & Sons, New York, 1984. Ruthven, D.M., Microporous Materials, 22, 537–541 (1998). Sing, K.S.W., “Analysis of Physisorption Isotherms,” in Physical Adsorption: Experiment, Theory and Applications, J. Fraissard Adsorption of Sulfur Dioxide from Pseudo Binary Mixtures 289 (Ed.), pp. 9–16, Kluwer Academic Publishers, Netherlands, 1997. Sing, K.S.W., D.H. Everett, R.A.W. Haul, L. Moscou, R.A. Pierotti, J. Rouquerol, and T. Siemieniewska, “Reporting Physisorption Data for Gas/Solid Systems-with Special Reference to the Determination of Surface Area and Porosity,” Pure Appl. Chem., 57(4), 603–619 (1985). Stenger Jr., H.G., K. Hu, and D. Simpson, “Competitive Adsorption of NO, SO2 and H2O onto Mordenite Synthesized from Perlite,” Gas Sep. and Purif., 7(1), 19–25 (1993a). Stenger Jr., H.G., K. Hu, and D. Simpson, “Chromatographic Separation and Concentration of Sulfur Dioxide in Flue Gases,” Ind. Eng. Chem. Res., 32(11), 2736–2739 (1993b). Tantet, J., M. Eić, and R. Desai, “Breakthrough Study of the Adsorption and Separation of Sulfur Dioxide from Wet Gas Using Hydrophobic Zeolites,” Gas Sep. and Purif., 9(3), 213–220 (1995).