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Title: Impact of sulfation and desulfation on NOx reduction using Cu-chabazite SCR catalysts

Abstract

This bench reactor study investigates the impact of gaseous sulfur on the NOx reduction activity of Cu-chabazite SCR (Cu-CHA) catalysts at SO2 concentrations representative of marine diesel engine exhaust. After two hours of 500 ppm SO2 exposure at 250 and 400 °C in the simulated diesel exhaust gases, the NOx reduction activity of the sulfated Cu-CHA SCR catalysts is severely degraded at evaluation temperatures below 250 °C; however, above 250 °C the impact of sulfur exposure is minimal. EPMA shows that sulfur is located throughout the washcoat and along the entire length of the sulfated samples. Interestingly, BET measurements reveal that the sulfated samples have a 20% decrease in surface area. Moreover, the sulfated samples show a decrease in NOx/nitrate absorption during NO exposure in a DRIFTS reactor which suggests that Cu sites in the catalyst are blocked by the presence of sulfur. SO2 exposure also results in an increase in NH3 storage capacity, possibly due to the formation of ammonium sulfate species in the sulfated samples. In all cases, lean thermal treatments as low as 500 °C reverse the effects of sulfur exposure and restore the NOx reduction activity of the Cu-CHA catalyst to that of the fresh condition.

Authors:
 [1];  [2];  [3];  [1];  [3]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Mokpo National Maritime Univ., Mokpo (Republic of Korea)
  3. Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1201286
Alternate Identifier(s):
OSTI ID: 1257872
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 258; Journal Issue: P2; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Marine diesel; Cu-chabazite; NH3 SCR; sulfur poisoning

Citation Formats

Brookshear, Daniel William, Nam, Jeong -Gil, Nguyen, Ke, Toops, Todd J., and Binder, Andrew J. Impact of sulfation and desulfation on NOx reduction using Cu-chabazite SCR catalysts. United States: N. p., 2015. Web. doi:10.1016/j.cattod.2015.04.029.
Brookshear, Daniel William, Nam, Jeong -Gil, Nguyen, Ke, Toops, Todd J., & Binder, Andrew J. Impact of sulfation and desulfation on NOx reduction using Cu-chabazite SCR catalysts. United States. https://doi.org/10.1016/j.cattod.2015.04.029
Brookshear, Daniel William, Nam, Jeong -Gil, Nguyen, Ke, Toops, Todd J., and Binder, Andrew J. 2015. "Impact of sulfation and desulfation on NOx reduction using Cu-chabazite SCR catalysts". United States. https://doi.org/10.1016/j.cattod.2015.04.029. https://www.osti.gov/servlets/purl/1201286.
@article{osti_1201286,
title = {Impact of sulfation and desulfation on NOx reduction using Cu-chabazite SCR catalysts},
author = {Brookshear, Daniel William and Nam, Jeong -Gil and Nguyen, Ke and Toops, Todd J. and Binder, Andrew J.},
abstractNote = {This bench reactor study investigates the impact of gaseous sulfur on the NOx reduction activity of Cu-chabazite SCR (Cu-CHA) catalysts at SO2 concentrations representative of marine diesel engine exhaust. After two hours of 500 ppm SO2 exposure at 250 and 400 °C in the simulated diesel exhaust gases, the NOx reduction activity of the sulfated Cu-CHA SCR catalysts is severely degraded at evaluation temperatures below 250 °C; however, above 250 °C the impact of sulfur exposure is minimal. EPMA shows that sulfur is located throughout the washcoat and along the entire length of the sulfated samples. Interestingly, BET measurements reveal that the sulfated samples have a 20% decrease in surface area. Moreover, the sulfated samples show a decrease in NOx/nitrate absorption during NO exposure in a DRIFTS reactor which suggests that Cu sites in the catalyst are blocked by the presence of sulfur. SO2 exposure also results in an increase in NH3 storage capacity, possibly due to the formation of ammonium sulfate species in the sulfated samples. In all cases, lean thermal treatments as low as 500 °C reverse the effects of sulfur exposure and restore the NOx reduction activity of the Cu-CHA catalyst to that of the fresh condition.},
doi = {10.1016/j.cattod.2015.04.029},
url = {https://www.osti.gov/biblio/1201286}, journal = {Catalysis Today},
issn = {0920-5861},
number = P2,
volume = 258,
place = {United States},
year = {Fri Jun 05 00:00:00 EDT 2015},
month = {Fri Jun 05 00:00:00 EDT 2015}
}

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Cited by: 44 works
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Works referenced in this record:

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Works referencing / citing this record:

Mechanism-based kinetic modeling of Cu-SSZ-13 sulfation and desulfation for NH 3 -SCR applications
journal, January 2019


Lean and rich aging of a Cu/SSZ-13 catalyst for combined lean NO x trap (LNT) and selective catalytic reduction (SCR) concept
journal, January 2019


Effects of SO 2 on Cu-SSZ-39 catalyst for the selective catalytic reduction of NO x with NH 3
journal, January 2020