Reversible and irreversible deactivation of Cu-CHA NH3-SCRcatalysts by SO2 and SO3

被引:100
|
作者
Hammershoi, Peter S. [1 ,2 ]
Jangjou, Yasser [3 ,4 ]
Epling, William S. [3 ,4 ]
Jensen, Anker D. [2 ]
Janssens, Ton V. W. [1 ,5 ]
机构
[1] Haldor Topsoe Res Labs, Haldor Topsoes Alle 1, DK-2800 Lyngby, Denmark
[2] Tech Univ Denmark, Dept Chem & Biochem Engn, Soltofts Plads B229, DK-2800 Lyngby, Denmark
[3] Univ Houston, Dept Chem & Biomol Engn, 4800 Calhoun Rd, Houston, TX 77204 USA
[4] Univ Virginia, Dept Chem Engn, 102 Engineers Way, Charlottesville, VA 22904 USA
[5] Umicore Denmark ApS, Nojsomhedsvej 20, DK-2800 Lyngby, Denmark
关键词
NH3-SCR; Cu-CHA; Deactivation; Sulfur oxides; Regeneration; SELECTIVE CATALYTIC-REDUCTION; CU-SAPO-34 SCR CATALYST; NH3-SCR REACTION; SULFUR; IMPACT; CU/SSZ-13; CU-SSZ-13; AMMONIA; COPPER; SITES;
D O I
10.1016/j.apcatb.2017.12.018
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Sulfur oxides are a common source for the deactivation of Cu-exchanged CHA zeolite based catalysts used for NOx reduction in diesel exhausts by selective catalytic reduction with NH3 (NH3-SCR). Since water and possible formation of SO3 affect the deactivation of Cu-CHA catalysts, the deactivation in the presence of SO2 or a mixture of SO2 and SO3 was studied by measuring the SCR activity in wet and dry gas at 200 and 550 degrees C. The estimated S-content in the catalysts before and after 4 h regeneration at 550 degrees C in NO, NH3, O-2 and H2O was related to the deactivation. The deactivation can be divided into two parts: a reversible deactivation that is restored by the regeneration treatment, and an irreversible part. The irreversible deactivation does not affect the activation energy for NH3-SCR and display a 1:1 correlation with the S-content, consistent with deactivation by Cu-sulfate formation. The reversible deactivation results in a lower activation energy and a deactivation that is larger than expected from the S-content. The presence of SO3 at 200 degrees C leads to higher reversible and irreversible deactivation, but has no significant impact at 550 degrees C. Furthermore, the irreversible deactivation is always higher when exposed at 200 degrees C than at 550 degrees C, and in wet conditions, compared to a dry feed. The deactivation is predominantly reversible, making regeneration at 550 degrees C a realistic approach to handle S-poisoning in exhaust systems.
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页码:38 / 45
页数:8
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