Tackling the Problem of Sulfur Poisoning of Perovskite Catalysts for Natural Gas Combustion

Ilaria Rosso; Guido Saracco; Vito Specchia

Korean Journal of Chemical Engineering, Vol.20, No.2, 222-229, March, 2003

DOI10.1007/BF02697232 Export Citation

Tackling the Problem of Sulfur Poisoning of Perovskite Catalysts for Natural Gas Combustion

Ilaria Rosso^†, Guido Saracco, and Vito Specchia

Dipartimento di Scienza dei Materiali e Ingegneria Chimica-Politecnico di Torino, Corso Duca degli Abruzzi, 24-10129 Turin, Italy

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LaMn0.5Mg0.5O3ㆍy MgO and LaCr0.5-xMnxMg0.5O3ㆍy MgO catalysts (x=0-0.25, y=0-17) were prepared, characterized (XRD, BET, SEM-EDS, TEM, FTIR, chemical and atomic absorption analyses), tested for high-temperature methane combustion and aged in presence of SO2 to investigate sulfur effect on catalytic activity. Different roles of manganese and chromium in the perovskite structure have been assessed: (i) manganese improves the activity of catalysts in the fresh state, whereas chromium worsens it; (ii) owing to its basic nature, manganese makes perovskites more prone to adsorb SO2 and so less resistant to sulfur poisoning, whereas chromium, owing to its acidic nature, has opposite effects; (iii) the partial solubility of chromium oxide in basic media renders Cr-catalyst regeneration by NH3 leaching less effective. MgO promotes catalytic activity of fresh LaCr0.5Mg0.5O3ㆍy MgO catalysts and slows down sulfur poisoning of LaMn0.5Mg0.5O3ㆍy MgO and LaCr0.25Mn0.25Mg0.5O3ㆍ17 MgO catalysts only.

Keywords:LaMn0.5Mg0.5O3ㆍy MgO;LaCr0.5-xMnxMg0.5O3ㆍy MgO;Perovskite;Methane Catalytic Combustion;Sulfur Poisoning

[References]

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Bensitel M, Waqif M, Saur O, Lavalley JC, J. Phys. Chem., 93, 6581 (1989)
Bertolacini RG, Hirschberg EHM, Modica FJ, U.S. Patent, 4,381,991, Standard Oil (1991)
Cerri I, Saracco G, Geobaldo F, Specchia V, Ind. Eng. Chem. Res., 39(1), 24 (2000)
Cerri I, Saracco G, Specchia V, Trimis D, Chem. Eng. J., 82(1-3), 73 (2001)
Ciambelli P, Cimino S, De Rossi S, Lisi L, Minelli G, Porta P, Russo G, Appl. Catal. B: Environ., 29(4), 239 (2001)
Collongue B, Garbowski E, Primet M, J. Chem. Soc.-Faraday Trans., 87, 2493 (1991)
Farrauto RJ, Heck RM, Catal. Today, 51(3-4), 351 (1999)
Garten RL, DallaBetta RA, Schlatter JC, "Catalytic Combustion," Handbook of Heterogeneous Catalysis, Ertl, G., Knozinger, H., Weitkamp, J., eds., VCH, Weinheim (1997)
Klvana D, Kirchnerova J, Gauthier P, Delval J, Chaouki J, Can. J. Chem. Eng., 75(3), 509 (1997)
Klvana D, Vaillancourt J, Kirchnerova J, Chaouki J, Appl. Catal. A: Gen., 109(2), 181 (1994)
Pascal P, "Noveau Traite de Chimie Minerale," Masson, Paris, vol. 14 (1959)
Pfefferle LD, Pfefferle WC, Catal. Rev.-Sci. Eng., 26, 219 (1987)
Rosso I, Garrone E, Geobaldo F, Onida B, Saracco G, Specchia V, Appl. Catal. B: Environ., 30(1-2), 61 (2001)
Rosso I, Garrone E, Geobaldo F, Onida B, Saracco G, Specchia V, Appl. Catal. B: Environ., 34(1), 29 (2001)
Saracco G, Geobaldo F, Baldi G, Appl. Catal. B: Environ., 20(4), 277 (1999)
Saracco G, Scibilia G, Iannibello A, Baldi G, Appl. Catal. B: Environ., 8(2), 229 (1996)
Seiyama T, Catal. Rev.-Sci. Eng., 34, 281 (1992)
Trimm DL, Appl. Catal., 7, 249 (1984)
Wan L, "Poisoning of Perovskite Oxides by Sulphur Dioxide," Properties and Applications of Perovskite-Type Oxides, Tejuca L.G., Fierro, J.L.G. (Eds.), Dekker, New York (1993)
Zwinkels MFM, Jaras SG, GovinMenon P, Catal. Rev.-Sci. Eng., 35, 319 (1993)

[Referenced By]

[1] Arai H, Yamada T, Eguchi K, Seiyama T, Appl. Catal., 26, 265 (1986)

[2] Bensitel M, Waqif M, Saur O, Lavalley JC, J. Phys. Chem., 93, 6581 (1989)

[3] Bertolacini RG, Hirschberg EHM, Modica FJ, U.S. Patent, 4,381,991, Standard Oil (1991)

[4] Cerri I, Saracco G, Geobaldo F, Specchia V, Ind. Eng. Chem. Res., 39(1), 24 (2000)

[5] Cerri I, Saracco G, Specchia V, Trimis D, Chem. Eng. J., 82(1-3), 73 (2001)

[6] Ciambelli P, Cimino S, De Rossi S, Lisi L, Minelli G, Porta P, Russo G, Appl. Catal. B: Environ., 29(4), 239 (2001)

[7] Collongue B, Garbowski E, Primet M, J. Chem. Soc.-Faraday Trans., 87, 2493 (1991)

[8] Farrauto RJ, Heck RM, Catal. Today, 51(3-4), 351 (1999)

[9] Garten RL, DallaBetta RA, Schlatter JC, "Catalytic Combustion," Handbook of Heterogeneous Catalysis, Ertl, G., Knozinger, H., Weitkamp, J., eds., VCH, Weinheim (1997)

[10] Klvana D, Kirchnerova J, Gauthier P, Delval J, Chaouki J, Can. J. Chem. Eng., 75(3), 509 (1997)

[11] Klvana D, Vaillancourt J, Kirchnerova J, Chaouki J, Appl. Catal. A: Gen., 109(2), 181 (1994)

[12] Pascal P, "Noveau Traite de Chimie Minerale," Masson, Paris, vol. 14 (1959)

[13] Pfefferle LD, Pfefferle WC, Catal. Rev.-Sci. Eng., 26, 219 (1987)

[14] Rosso I, Garrone E, Geobaldo F, Onida B, Saracco G, Specchia V, Appl. Catal. B: Environ., 30(1-2), 61 (2001)

[15] Rosso I, Garrone E, Geobaldo F, Onida B, Saracco G, Specchia V, Appl. Catal. B: Environ., 34(1), 29 (2001)

[16] Saracco G, Geobaldo F, Baldi G, Appl. Catal. B: Environ., 20(4), 277 (1999)

[17] Saracco G, Scibilia G, Iannibello A, Baldi G, Appl. Catal. B: Environ., 8(2), 229 (1996)

[18] Seiyama T, Catal. Rev.-Sci. Eng., 34, 281 (1992)

[19] Trimm DL, Appl. Catal., 7, 249 (1984)

[20] Wan L, "Poisoning of Perovskite Oxides by Sulphur Dioxide," Properties and Applications of Perovskite-Type Oxides, Tejuca L.G., Fierro, J.L.G. (Eds.), Dekker, New York (1993)

[21] Zwinkels MFM, Jaras SG, GovinMenon P, Catal. Rev.-Sci. Eng., 35, 319 (1993)