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Title: Nature of Active Sites and Surface Intermediates during SCR of NO with NH3 by Supported V2O5–WO3/TiO2 Catalysts

Abstract

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.

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)
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. https://doi.org/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. https://doi.org/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 = {Mon Oct 23 00:00:00 EDT 2017},
month = {Mon Oct 23 00:00:00 EDT 2017}
}

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Alkali-driven active site shift of fast SCR with NH 3 on V 2 O 5 –WO 3 /TiO 2 catalyst via a novel Eley–Rideal mechanism
journal, January 2019

  • Xiang, Jinyao; Du, Xuesen; Wan, Yuyi
  • Catalysis Science & Technology, Vol. 9, Issue 21
  • DOI: 10.1039/c9cy01565e

In situ decorated MOF-derived Mn–Fe oxides on Fe mesh as novel monolithic catalysts for NO x reduction
journal, January 2020

  • Yao, Heyan; Cai, Sixiang; Yang, Bo
  • New Journal of Chemistry, Vol. 44, Issue 6
  • DOI: 10.1039/c9nj05960a

A zeolitic vanadotungstate family with structural diversity and ultrahigh porosity for catalysis
journal, September 2018


Improved NO x reduction in the presence of alkali metals by using hollandite Mn–Ti oxide promoted Cu-SAPO-34 catalysts
journal, January 2018

  • Zha, Kaiwen; Kang, Lin; Feng, Chong
  • Environmental Science: Nano, Vol. 5, Issue 6
  • DOI: 10.1039/c8en00226f

Poisoning effects of lead species on the V 2 O 5 ‐WO 3 /TiO 2 type NH 3 ‐selective catalytic reduction catalyst
journal, April 2019

  • Ali, Zulfiqar; Lu, Qiang; Iqbal, Tahir
  • Asia-Pacific Journal of Chemical Engineering, Vol. 14, Issue 3
  • DOI: 10.1002/apj.2309

Mechanism by which Tungsten Oxide Promotes the Activity of Supported V 2 O 5 /TiO 2 Catalysts for NO X Abatement: Structural Effects Revealed by 51 V MAS NMR Spectroscopy
journal, September 2019

  • Jaegers, Nicholas R.; Lai, Jun‐Kun; He, Yang
  • Angewandte Chemie International Edition, Vol. 58, Issue 36
  • DOI: 10.1002/anie.201904503

The effects of H 2 O on a vanadium-based catalyst for NH 3 -SCR at low temperatures: a quantitative study of the reaction pathway and active sites
journal, January 2019

  • Liu, Kuo; Yan, Zidi; He, Hong
  • Catalysis Science & Technology, Vol. 9, Issue 20
  • DOI: 10.1039/c9cy01370a

Doping effect of Sm on the TiO 2 /CeSmO x catalyst in the NH 3 -SCR reaction: structure–activity relationship, reaction mechanism and SO 2 tolerance
journal, January 2019

  • Liu, Hao; Sun, Chuanzhi; Fan, Zhongxuan
  • Catalysis Science & Technology, Vol. 9, Issue 13
  • DOI: 10.1039/c9cy00731h

Polymeric vanadyl species determine the low-temperature activity of V-based catalysts for the SCR of NO x with NH 3
journal, November 2018