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

Zhu, Minghui; Lai, Jun-Kun; Tumuluri, Uma; Wu, Zili; Wachs, Israel E.

doi:10.1021/jacs.7b09646

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

Journal Article · Mon Oct 23 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b09646· OSTI ID:1468067

^[1]; Lai, Jun-Kun ^[1]; Tumuluri, Uma ^[2]; ^[2]; Wachs, Israel E. ^[3]

Lehigh Univ., Bethlehem, PA (United States). Operando Molecular Spectroscopy & Catalysis Laboratory, Department of Chemical & Biomolecular Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division and Center for Nanophase Materials Sciences
Operando Molecular Spectroscopy &, Catalysis Laboratory, Department of Chemical &, Biomolecular Engineering, Lehigh University, Bethlehem, Pennsylvania 18015, United States

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 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 NH₃ by supported V₂O₅–WO₃/TiO₂ catalysts.

View Accepted Manuscript (DOE)

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

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

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

OSTI ID:: 1468067

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 44 Vol. 139; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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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 Jaegers, Nicholas R.; Lai, Jun‐Kun; He, Yang Angewandte Chemie, Vol. 131, Issue 36 https://doi.org/10.1002/ange.201904503	journal	July 2019
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 Jaegers, Nicholas R.; Lai, Jun‐Kun; He, Yang Angewandte Chemie International Edition, Vol. 58, Issue 36 https://doi.org/10.1002/anie.201904503	journal	September 2019
Poisoning effects of lead species on the V ₂ O ₅ ‐WO ₃ /TiO ₂ type NH ₃ ‐selective catalytic reduction catalyst Ali, Zulfiqar; Lu, Qiang; Iqbal, Tahir Asia-Pacific Journal of Chemical Engineering, Vol. 14, Issue 3 https://doi.org/10.1002/apj.2309	journal	April 2019
Spectroscopic Insights into the Mechanism of Selective Catalytic Reduction of NO by Ammonia on Sulfuric Acid‐modified Fe ₂ O ₃ Surface Huang, Zhiwei; Zhang, Jie; Du, Yueyao ChemCatChem, Vol. 11, Issue 13 https://doi.org/10.1002/cctc.201900584	journal	June 2019
A zeolitic vanadotungstate family with structural diversity and ultrahigh porosity for catalysis Zhang, Zhenxin; Zhu, Qianqian; Sadakane, Masahiro Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06274-2	journal	September 2018
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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 Liu, Kuo; Yan, Zidi; He, Hong Catalysis Science & Technology, Vol. 9, Issue 20 https://doi.org/10.1039/c9cy01370a	journal	January 2019
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 Xiang, Jinyao; Du, Xuesen; Wan, Yuyi Catalysis Science & Technology, Vol. 9, Issue 21 https://doi.org/10.1039/c9cy01565e	journal	January 2019
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