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Title: Sulfate promotion of selective catalytic reduction of nitric oxide by ammonia on ceria

Abstract

Selective catalytic reduction of nitric oxide by ammonia (NH3-SCR) is a promising technology for NOx emission control. In this work, the recently discovered sulfate promotion effect in this reaction was thoroughly investigated on ceria. Sulfates derived from different organic S precursors all exhibit a promotion effect. Mechanistic studies generate a reaction network including both Langmuir–Hinshelwood and Eley–Rideal mechanisms. Sulfates were shown to be versatile promoters with multiple functions: they tune the adsorption of reactants towards a more balanced intermediate coverage by creating strong Lewis acid sites, facilitate *NH2 formation, and suppress ammonia oxidation through surface oxygen deactivation. The comparison between sulfates and the classic inorganic promoter FeOx revealed that sulfates are more effective, especially at high temperature. This is mainly attributed to the high coverages of Eley–Rideal intermediates and low ammonia oxidation activity on sulfated ceria. Overall, this work provides fundamental understanding of the role of surface sulfates in NH3-SCR, which are essential under actual operation conditions. This understanding presents an exciting opportunity for future catalyst design with high durability and low cost.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Indiana Univ., Bloomington, IN (United States)
Publication Date:
Research Org.:
Indiana Univ., Bloomington, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1612500
Alternate Identifier(s):
OSTI ID: 1499819
Grant/Contract Number:  
SC0016367
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Catalysis Science and Technology
Additional Journal Information:
Journal Volume: 9; Journal Issue: 8; Journal ID: ISSN 2044-4753
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; NH3-SCR; sulfate promotion; reaction mechanism; in situ DRIFT

Citation Formats

Chen, Linxiao, Agrawal, Vaibhav, and Tait, Steven L. Sulfate promotion of selective catalytic reduction of nitric oxide by ammonia on ceria. United States: N. p., 2019. Web. doi:10.1039/c8cy02590h.
Chen, Linxiao, Agrawal, Vaibhav, & Tait, Steven L. Sulfate promotion of selective catalytic reduction of nitric oxide by ammonia on ceria. United States. https://doi.org/10.1039/c8cy02590h
Chen, Linxiao, Agrawal, Vaibhav, and Tait, Steven L. 2019. "Sulfate promotion of selective catalytic reduction of nitric oxide by ammonia on ceria". United States. https://doi.org/10.1039/c8cy02590h. https://www.osti.gov/servlets/purl/1612500.
@article{osti_1612500,
title = {Sulfate promotion of selective catalytic reduction of nitric oxide by ammonia on ceria},
author = {Chen, Linxiao and Agrawal, Vaibhav and Tait, Steven L.},
abstractNote = {Selective catalytic reduction of nitric oxide by ammonia (NH3-SCR) is a promising technology for NOx emission control. In this work, the recently discovered sulfate promotion effect in this reaction was thoroughly investigated on ceria. Sulfates derived from different organic S precursors all exhibit a promotion effect. Mechanistic studies generate a reaction network including both Langmuir–Hinshelwood and Eley–Rideal mechanisms. Sulfates were shown to be versatile promoters with multiple functions: they tune the adsorption of reactants towards a more balanced intermediate coverage by creating strong Lewis acid sites, facilitate *NH2 formation, and suppress ammonia oxidation through surface oxygen deactivation. The comparison between sulfates and the classic inorganic promoter FeOx revealed that sulfates are more effective, especially at high temperature. This is mainly attributed to the high coverages of Eley–Rideal intermediates and low ammonia oxidation activity on sulfated ceria. Overall, this work provides fundamental understanding of the role of surface sulfates in NH3-SCR, which are essential under actual operation conditions. This understanding presents an exciting opportunity for future catalyst design with high durability and low cost.},
doi = {10.1039/c8cy02590h},
url = {https://www.osti.gov/biblio/1612500}, journal = {Catalysis Science and Technology},
issn = {2044-4753},
number = 8,
volume = 9,
place = {United States},
year = {Sat Mar 02 00:00:00 EST 2019},
month = {Sat Mar 02 00:00:00 EST 2019}
}

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Cited by: 24 works
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  • Sreekanth, Pavani M.; Peña, Donovan A.; Smirniotis, Panagiotis G.
  • Industrial & Engineering Chemistry Research, Vol. 45, Issue 19
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Works referencing / citing this record:

Improvement in alkali metal resistance of commercial V2O5–WO3/TiO2 SCR catalysts modified by Ce and Cu
journal, August 2019