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Journal article

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

From

Department of Chemical and Biochemical Engineering, Technical University of Denmark1

CHEC Research Centre, Department of Chemical and Biochemical Engineering, Technical University of Denmark2

University of Houston3

Haldor Topsoe AS4

Abstract 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 °C.

The estimated S-content in the catalysts before and after 4 h regeneration at 550 °C in NO, NH3, O2 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 °C leads to higher reversible and irreversible deactivation, but has no significant impact at 550 °C. Furthermore, the irreversible deactivation is always higher when exposed at 200 °C than at 550 °C, and in wet conditions, compared to a dry feed.

The deactivation is predominantly reversible, making regeneration at 550 °C a realistic approach to handle S-poisoning in exhaust systems.

Language: English
Year: 2018
Pages: 38-45
ISSN: 18733883 and 09263373
Types: Journal article
DOI: 10.1016/j.apcatb.2017.12.018
ORCIDs: Hammershøi, Peter S. and Jensen, Anker D.

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