Selective Catalytic Reduction of NO by NH3 with WO3-TiO2 Catalysts: Influence of Catalyst Synthesis Method

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

doi:10.1016/j.apcatb.2016.01.072

Title: Selective Catalytic Reduction of NO by NH₃ with WO₃-TiO₂ Catalysts: Influence of Catalyst Synthesis Method

Journal Article · Tue Feb 02 00:00:00 EST 2016 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2016.01.072· OSTI ID:1295096

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

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

A series of supported WO₃/TiO₂ catalysts was prepared by a new synthesis procedure involving co-precipitation of an aqueous TiO(OH)₂ and (NH₄)₁₀W₁₂O₄₁*5H₂O slurry under controlled pH conditions. The morphological properties, molecular structures, surface acidity and surface chemistry of the supported WO₃/TiO₂ catalysts were determined with BET, in situ Raman, in situ IR and temperature-programmed surface reaction (TPSR) spectroscopy, respectively. Isotopic ¹⁸O-¹⁶O exchange demonstrated that tungsten oxide was exclusively present as surface WO_x species on the TiO₂ support with mono-oxo W=O coordination. In contrast to previous studies employing impregnation synthesis that found only surface one mono-oxo O=WO₄ site on TiO₂, the co-precipitation procedure resulted in the formation of two distinct surface WO_x species: mono-oxo O=WO₄ (~1010-1017 cm^-1) on low defect density patches of TiO₂ and a second mono-oxo O=WO₄ (~983-986 cm^-1) on high defect density patches of TiO₂. The concentration of the second WO_x surface species increases as a function of solution pH. Both surface WOx sites, however, exhibited the same NO/NH₃ SCR reactivity. The co-precipitated WO₃-TiO₂ catalysts synthesized in alkaline solutions exhibited enhanced performance for the NO/NH₃ SCR reaction that is ascribed to the greater number of surface defects on the resulting TiO2 support. For the co-precipitated catalyst prepared at pH10, surface NH₄⁺ species on Br nsted acid sites were found to be more reactive than surface NH₃* species on Lewis acid sites for SCR of NO with NH₃.

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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)

Grant/Contract Number:: AC05-00OR22725; SC0012577; 51274263; 51204220

OSTI ID:: 1295096

Alternate ID(s):: OSTI ID: 1358764

Journal Information:: Applied Catalysis. B, Environmental, Vol. 188; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 43 works

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Catalysts
Co-precipitated
TiO2
WO3
Spectroscopy
Raman
IR
Temperature programmed surface reaction (TPSR)
Reaction
NO
NH3
Selective catalytic reduction (SCR)

Title: Selective Catalytic Reduction of NO by NH3 with WO3-TiO2 Catalysts: Influence of Catalyst Synthesis Method

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Title: Selective Catalytic Reduction of NO by NH₃ with WO₃-TiO₂ Catalysts: Influence of Catalyst Synthesis Method