Influence of catalyst synthesis method on selective catalytic reduction (SCR) of NO by NH3 with V2O5-WO3/TiO2 catalysts

He, Yuanyuan; Ford, Michael E.; Zhu, Minghui; Liu, Qingcai; Tumuluri, Uma; Wu, Zili; Wachs, Israel E.

doi:10.1016/j.apcatb.2016.04.022

Influence of catalyst synthesis method on selective catalytic reduction (SCR) of NO by NH₃ with V₂O₅-WO₃/TiO₂ catalysts

Journal Article · Thu Apr 14 04:00:00 EDT 2016 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2016.04.022· OSTI ID:1295102

He, Yuanyuan ^[1]; Ford, Michael E. ^[2]; Zhu, Minghui ^[2]; Liu, Qingcai ^[3]; Tumuluri, Uma ^[4]; Wu, Zili ^[4]; Wachs, Israel E. ^[2]

Chongqing Univ., Chongqing (China). College of Materials Science and Engineering; Lehigh Univ., Bethlehem, PA (United States). Operando Molecular Spectroscopy & Catalysis Lab.
Lehigh Univ., Bethlehem, PA (United States). Operando Molecular Spectroscopy & Catalysis Lab.
Chongqing Univ., Chongqing (China). College of Materials Science and Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division and Center for Nanophase Materials Sciences

We compared the molecular structures, surface acidity and catalytic activity for NO/NH₃/O₂ SCR of V₂O₅-WO₃/TiO₂ catalysts for two different synthesis methods: co-precipitation of aqueous vanadium and tungsten oxide precursors with TiO(OH)₂ and by incipient wetness impregnation of the aqueous precursors on a reference crystalline TiO₂ support (P25; primarily anatase phase). Bulk analysis by XRD showed that co-precipitation results in small and/or poorly ordered TiO₂(anatase) particles and that VO_x and WO_x do not form solid solutions with the bulk titania lattice. Surface analysis of the co-precipitated catalyst by High Sensitivity-Low Energy Ion Scattering (HS-LEIS) confirms that the VO_x and WO_x are surface segregated for the co-precipitated catalysts. In situ Raman and IR spectroscopy revealed that the vanadium and tungsten oxide components are present as surface mono-oxo O = VO₃ and O = WO₄ sites on the TiO₂ supports. Co-precipitation was shown for the first time to also form new mono-oxo surface VO₄ and WO₄ sites that appear to be anchored at surface defects of the TiO₂ support. IR analysis of chemisorbed ammonia showed the presence of both surface NH₃^* on Lewis acid sites and surface NH₄^+* on Brønsted acid sites. TPSR spectroscopy demonstrated that the specific SCR kinetics was controlled by the redox surface VO₄ species and that the surface kinetics was independent of TiO₂ synthesis method or presence of surface WO₅ sites. SCR reaction studies revealed that the surface WO5 sites possess minimal activity below ~325 °C and their primary function is to increase the adsorption capacity of ammonia. A relationship between the SCR activity and surface acidity was not found. The SCR reaction is controlled by the surface VO₄ sites that initiate the reaction at ~200 °C. The co-precipitated catalysts were always more active than the corresponding impregnated catalysts. Finally, we ascribe the higher activity of the co-precipitated catalysts to the presence of the new surface WO_x sites associated surface defects on the TiO₂ support that increase the ammonia adsorption capacity.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725; SC0012577

OSTI ID:: 1295102

Alternate ID(s):: OSTI ID: 1341096

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Journal Issue: C Vol. 193; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Catalysts
Co-precipitation
HS-LEIS
Incipient-wetness impregnation
Infrared
NH3
NO
O2
Raman
Selective catalytic reduction (SCR)
Spectroscopy
Supported
Synthesis
TPSR
TiO2
V2O5
WO3
XRD