Deactivation of Cu/SSZ-13 NH3-SCR catalyst by exposure to CO, H2, and C3H6

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Auvray, Xavier,1986Chalmers tekniska högskola,Chalmers University of Technology (author)

Deactivation of Cu/SSZ-13 NH3-SCR catalyst by exposure to CO, H2, and C3H6

Article/chapterEnglish2019

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2019-11-06
MDPI AG,2019
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LIBRIS-ID:oai:research.chalmers.se:f104ae64-3add-403a-84ec-567351ff9506
https://doi.org/10.3390/catal9110929DOI
https://research.chalmers.se/publication/513990URI

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Language:English
Summary in:English

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Lean nitric oxide (NOx)-trap (LNT) and selective catalytic reduction (SCR) are efficient systems for the abatement of NOx. The combination of LNT and SCR catalysts improves overall NOx removal, but there is a risk that the SCR catalyst will be exposed to high temperatures and rich exhaust during the LNTs sulfur regeneration. Therefore, the effect of exposure to various rich conditions and temperatures on the subsequent SCR activity of a Cu-exchanged chabazite catalyst was studied. CO, H2, C3H6, and the combination of CO + H2 were used to simulate rich conditions. Aging was performed at 800 °C, 700 °C, and, in the case of CO, 600 °C, in a plug-flow reactor. Investigation of the nature of Cu sites was performed with NH3-temperature-programed desorption (TPD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFT) of probe molecules (NH3 and NO). The combination of CO and H2 was especially detrimental to SCR activity and to NH3 oxidation. Rich aging with low reductant concentrations resulted in a significantly larger deactivation compared to lean conditions. Aging in CO at 800 °C caused SCR deactivation but promoted high-temperature NH3 oxidation. Rich conditions greatly enhanced the loss of Brønsted and Lewis acid sites at 800 °C, indicating dealumination and Cu migration. However, at 700 °C, mainly Brønsted sites disappeared during aging. DRIFT spectroscopy analysis revealed that CO aging modified the Cu2+/CuOH+ ratio in favor of the monovalent CuOH+ species, as opposed to lean aging. To summarize, we propose that the reason for the increased deactivation observed for mild rich conditions is the transformation of the Cu species from Z2Cu to ZCuOH, possibly in combination with the formation of Cu clusters. © 2019, MDPI AG. All rights reserved.

Subject headings and genre

NATURVETENSKAP Kemi Oorganisk kemi hsv//swe
NATURAL SCIENCES Chemical Sciences Inorganic Chemistry hsv//eng
TEKNIK OCH TEKNOLOGIER Kemiteknik Annan kemiteknik hsv//swe
ENGINEERING AND TECHNOLOGY Chemical Engineering Other Chemical Engineering hsv//eng
NATURVETENSKAP Kemi Organisk kemi hsv//swe
NATURAL SCIENCES Chemical Sciences Organic Chemistry hsv//eng
Deactivation
Aging
Cu/SSZ-13
Rich conditions
NH SCR 3

Added entries (persons, corporate bodies, meetings, titles ...)

Mihai, Oana,1975Volvo Cars(Swepub:cth)oanam (author)
Lundberg, BjörnVolvo Cars (author)
Olsson, Louise,1974Chalmers tekniska högskola,Chalmers University of Technology(Swepub:cth)louisej (author)
Chalmers tekniska högskolaVolvo Cars (creator_code:org_t)

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In:Catalysts: MDPI AG9:112073-4344

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