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Title: Nature of Active Sites and Surface Intermediates during SCR of NO with NH 3 by Supported V 2O 5–WO 3/TiO 2 Catalysts

Abstract

In this study, time-resolved in situ IR was performed during selective catalytic reduction of NO with NH 3 on supported V 2O 5–WO 3/TiO 2 catalysts to examine the distribution and reactivity of surface ammonia species on Lewis and Brønsted acid sites. While both species were found to participate in the SCR reaction, their relative population depends on the coverage of the surface vanadia and tungsta sites, temperature, and moisture. Although the more abundant surface NH 4 +, ads intermediates dominate the overall SCR reaction, especially for hydrothermally aged catalysts, the minority surface NH 3,ads intermediates exhibit a higher specific SCR activity (TOF). Lastly, the current study serves to resolve the long-standing controversy about the active sites for SCR of NO with NH 3 by supported V 2O 5–WO 3/TiO 2 catalysts.

Authors:
ORCiD logo [1];  [1];  [2]; ORCiD logo [2];  [3]
  1. Lehigh Univ., Bethlehem, PA (United States). Operando Molecular Spectroscopy & Catalysis Laboratory, Department of Chemical & Biomolecular Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division and Center for Nanophase Materials Sciences
  3. Operando Molecular Spectroscopy &, Catalysis Laboratory, Department of Chemical &, Biomolecular Engineering, Lehigh University, Bethlehem, Pennsylvania 18015, United States
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1468067
Grant/Contract Number:  
AC05-00OR22725; SC0012577
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 44; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhu, Minghui, Lai, Jun-Kun, Tumuluri, Uma, Wu, Zili, and Wachs, Israel E. Nature of Active Sites and Surface Intermediates during SCR of NO with NH3 by Supported V2O5–WO3/TiO2 Catalysts. United States: N. p., 2017. Web. doi:10.1021/jacs.7b09646.
Zhu, Minghui, Lai, Jun-Kun, Tumuluri, Uma, Wu, Zili, & Wachs, Israel E. Nature of Active Sites and Surface Intermediates during SCR of NO with NH3 by Supported V2O5–WO3/TiO2 Catalysts. United States. doi:10.1021/jacs.7b09646.
Zhu, Minghui, Lai, Jun-Kun, Tumuluri, Uma, Wu, Zili, and Wachs, Israel E. Mon . "Nature of Active Sites and Surface Intermediates during SCR of NO with NH3 by Supported V2O5–WO3/TiO2 Catalysts". United States. doi:10.1021/jacs.7b09646. https://www.osti.gov/servlets/purl/1468067.
@article{osti_1468067,
title = {Nature of Active Sites and Surface Intermediates during SCR of NO with NH3 by Supported V2O5–WO3/TiO2 Catalysts},
author = {Zhu, Minghui and Lai, Jun-Kun and Tumuluri, Uma and Wu, Zili and Wachs, Israel E.},
abstractNote = {In this study, time-resolved in situ IR was performed during selective catalytic reduction of NO with NH3 on supported V2O5–WO3/TiO2 catalysts to examine the distribution and reactivity of surface ammonia species on Lewis and Brønsted acid sites. While both species were found to participate in the SCR reaction, their relative population depends on the coverage of the surface vanadia and tungsta sites, temperature, and moisture. Although the more abundant surface NH4+,ads intermediates dominate the overall SCR reaction, especially for hydrothermally aged catalysts, the minority surface NH3,ads intermediates exhibit a higher specific SCR activity (TOF). Lastly, the current study serves to resolve the long-standing controversy about the active sites for SCR of NO with NH3 by supported V2O5–WO3/TiO2 catalysts.},
doi = {10.1021/jacs.7b09646},
journal = {Journal of the American Chemical Society},
number = 44,
volume = 139,
place = {United States},
year = {2017},
month = {10}
}

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