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Title: Impact of sulfation and desulfation on NO x reduction using Cu-chabazite SCR catalysts

This bench reactor study investigates the impact of gaseous sulfur on the NO x reduction activity of Cu-chabazite SCR (Cu-CHA) catalysts at SO 2 concentrations representative of marine diesel engine exhaust. After two hours of 500 ppm SO 2 exposure at 250 and 400 °C in the simulated diesel exhaust gases, the NO x 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 NO x/nitrate absorption during NO exposure in a DRIFTS reactor which suggests that Cu sites in the catalyst are blocked by the presence of sulfur. SO 2 exposure also results in an increase in NH 3 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 NO x reduction activity of themore » Cu-CHA catalyst to that of the fresh condition.« less
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:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 258; Journal Issue: P2; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Marine diesel; Cu-chabazite; NH3 SCR; sulfur poisoning
OSTI Identifier:
1201286
Alternate Identifier(s):
OSTI ID: 1257872