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Title: Reaction Pathways and Kinetics for Selective Catalytic Reduction (SCR) of Acidic NO x Emissions from Power Plants with NH 3

Abstract

We report that selective catalytic reduction (SCR) of NO x with NH 3 by supported vanadium oxide catalysts is an important technology for reducing acidic NO x emissions from stationary sources and mobile diesel vehicles. However, rational design of improved catalysts is still hampered by a lack of consensus about reaction pathways and kinetics of this critical technology. The SCR fundamentals were resolved by applying multiple time-resolved in situ spectroscopies (ultraviolet–visible light (UV-vis), Raman and temperature-programmed surface reaction (TPSR)) and isotopically labeled molecules ( 18O 2, H 2 18O, 15N 18O, ND 3). Finally, this series of experiments directly revealed that the SCR reaction occurs at surface V 5+O 4 sites that are maintained in the oxidized state by O 2 and the rate-determining step involves the reduction of V 5+O 4 sites by NO and NH 3, specifically the breaking of N–H bonds during the course of formation or decomposition of the NO–NH 3 intermediate.

Authors:
ORCiD logo [1];  [1];  [2];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Lehigh Univ., Bethlehem, PA (United States). Operando Molecular Spectroscopy & Catalysis Laboratory
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division and Center for Nanophase Materials Sciences
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:
1468069
Grant/Contract Number:  
AC05-00OR22725; SC0012577
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 7; Journal Issue: 12; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; NH3; NO; SCR; spectroscopy; TPSR; UV-vis; vanadium oxide

Citation Formats

Zhu, Minghui, Lai, Jun-Kun, Tumuluri, Uma, Ford, Michael E., Wu, Zili, and Wachs, Israel E. Reaction Pathways and Kinetics for Selective Catalytic Reduction (SCR) of Acidic NOx Emissions from Power Plants with NH3. United States: N. p., 2017. Web. doi:10.1021/acscatal.7b03149.
Zhu, Minghui, Lai, Jun-Kun, Tumuluri, Uma, Ford, Michael E., Wu, Zili, & Wachs, Israel E. Reaction Pathways and Kinetics for Selective Catalytic Reduction (SCR) of Acidic NOx Emissions from Power Plants with NH3. United States. doi:10.1021/acscatal.7b03149.
Zhu, Minghui, Lai, Jun-Kun, Tumuluri, Uma, Ford, Michael E., Wu, Zili, and Wachs, Israel E. Fri . "Reaction Pathways and Kinetics for Selective Catalytic Reduction (SCR) of Acidic NOx Emissions from Power Plants with NH3". United States. doi:10.1021/acscatal.7b03149. https://www.osti.gov/servlets/purl/1468069.
@article{osti_1468069,
title = {Reaction Pathways and Kinetics for Selective Catalytic Reduction (SCR) of Acidic NOx Emissions from Power Plants with NH3},
author = {Zhu, Minghui and Lai, Jun-Kun and Tumuluri, Uma and Ford, Michael E. and Wu, Zili and Wachs, Israel E.},
abstractNote = {We report that selective catalytic reduction (SCR) of NOx with NH3 by supported vanadium oxide catalysts is an important technology for reducing acidic NOx emissions from stationary sources and mobile diesel vehicles. However, rational design of improved catalysts is still hampered by a lack of consensus about reaction pathways and kinetics of this critical technology. The SCR fundamentals were resolved by applying multiple time-resolved in situ spectroscopies (ultraviolet–visible light (UV-vis), Raman and temperature-programmed surface reaction (TPSR)) and isotopically labeled molecules (18O2, H218O, 15N18O, ND3). Finally, this series of experiments directly revealed that the SCR reaction occurs at surface V5+O4 sites that are maintained in the oxidized state by O2 and the rate-determining step involves the reduction of V5+O4 sites by NO and NH3, specifically the breaking of N–H bonds during the course of formation or decomposition of the NO–NH3 intermediate.},
doi = {10.1021/acscatal.7b03149},
journal = {ACS Catalysis},
number = 12,
volume = 7,
place = {United States},
year = {2017},
month = {11}
}

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