Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 36, Pages 12609-12616Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201904503
Keywords
heterogeneous catalysis; NMR spectroscopy; NOx; selective catalytic reduction (SCR); vanadium
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences, and Geosciences Catalysis Program [DE-AC05-RL01830]
- Center for Understanding AMP
- Control of Acid Gas-Induced Evolution of Materials for Energy (UN-CAGE-ME), an Energy Frontier Research Center - DOE, Office of Science, Office of Basic Energy Sciences [DE-SC0012577]
- Department of Energy's Office of Biological and Environmental Research at Pacific Northwest National Laboratory (PNNL)
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [66628]
- US Department of Energy [DE-AC06-76RLO 1830]
- Seattle Chapter of the Achievement Rewards for College Scientists
- Robert Ramsay fund of The University of Alabama
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The selective catalytic reduction (SCR) of NOx with NH3 to N-2 with supported V2O5(-WO3)/TiO2 catalysts is an industrial technology used to mitigate toxic emissions. Long-standing uncertainties in the molecular structures of surface vanadia are clarified, whereby progressive addition of vanadia to TiO2 forms oligomeric vanadia structures and reveals a proportional relationship of SCR reaction rate to [surface VOx concentration](2), implying a 2-site mechanism. Unreactive surface tungsta (WO3) also promote the formation of oligomeric vanadia (V2O5) sites, showing that promoter incorporation enhances the SCR reaction by a structural effect generating adjacent surface sites and not from electronic effects as previously proposed. The findings outline a method to assess structural effects of promoter incorporation on catalysts and reveal both the dual-site requirement for the SCR reaction and the important structural promotional effect that tungsten oxide offers for the SCR reaction by V2O5/TiO2 catalysts.
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