Mechanism by which Tungsten Oxide Promotes the Activity of Supported V2O5/TiO2 Catalysts for NOX Abatement: Structural Effects Revealed by 51V MAS NMR Spectroscopy

Jaegers, Nicholas R.; Lai, Jun-Kun; He, Yang; Walter, Eric; Dixon, David A.; Vasiliu, Monica; Chen, Ying; Wang, Chongmin; Hu, Mary Y.; Mueller, Karl T.; Wachs, Israel E.; Wang, Yong; Hu, Jian Zhi

doi:10.1002/anie.201904503

Title: Mechanism by which Tungsten Oxide Promotes the Activity of Supported V₂O₅/TiO₂ Catalysts for NO_X Abatement: Structural Effects Revealed by ⁵¹V MAS NMR Spectroscopy

Journal Article · Mon Jul 08 00:00:00 EDT 2019 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201904503· OSTI ID:1572978

^[1]; Lai, Jun-Kun ^[2]; He, Yang ^[3]; Walter, Eric ^[3]; Dixon, David A. ^[4]; Vasiliu, Monica ^[4]; Chen, Ying ^[3]; Wang, Chongmin ^[3]; Hu, Mary Y. ^[3]; Mueller, Karl T. ^[3]; Wachs, Israel E. ^[2]; Wang, Yong ^[1];

^[3]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
Lehigh Univ., Bethlehem, PA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
The Univ. of Alabama, Tuscaloosa, AL (United States)

Growing concern for environmental pollutants coupled with an expansion of energy demand has promoted significant interest in technologies to abate contaminating species. Nitrogen oxides are particularly alarming due to their numerous detrimental impacts to the environment and public health, where selective catalytic reduction to inert N₂ is an industrially-relevant mitigation technology. Herein, we provide unique, molecular-level insight on the structure and reactivity of V₂O₅(-WO₃)/TiO₂ catalysts employed at stationary facilities for NO_x removal. Detailed catalytic testing, spectroscopy (nuclear magnetic resonance, Raman, and electron paramagnetic resonance), and electronic structure-based predictions of ⁵¹V chemical shifts help clarify the promotional role of tungsten oxide and identify an active site requirement for SCR of NO_x. We show that progressive addition of vanadia to the catalyst surface increases the catalytic SCR performance and promotes the formation of larger vanadium domains, demonstrating the proportional relationship of SCR reaction rate to [VO_x loading]2 for supported V₂O₅/TiO₂ catalysts with increasing surface vanadia coverage. Tungsten oxide incorporation enhances catalyst reactivity which is shown to stem not from electronic effects, but from changes to the vanadium structure as observed spectroscopically. The progressive addition of tungsten oxide to the catalyst surface also increases the catalytic performance and promotes the formation of larger vanadium domains, which are beneficial for catalytic turnover in a two-site model. Further, unique monomeric species are confidently ascribed to distorted tetrahedral and square pyramidal structures, resolving a long-standing uncertainty in literature assignments for the signals. These findings provide strong support for both the dual-site requirement for the SCR reaction and the important structural promotional effect that tungsten offers for mitigation of these harmful pollutants.

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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); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

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

Grant/Contract Number:: AC05-76RL01830; SC0012577; 66628

OSTI ID:: 1572978

Alternate ID(s):: OSTI ID: 1547078

Report Number(s):: PNNL-SA-141251; ANIE; TRN: US2001090

Journal Information:: Angewandte Chemie (International Edition), Vol. 58, Issue 36; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 102 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
heterogeneous catalysis
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Title: Mechanism by which Tungsten Oxide Promotes the Activity of Supported V2O5/TiO2 Catalysts for NOX Abatement: Structural Effects Revealed by 51V MAS NMR Spectroscopy

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