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Hierarchical Vanadia Model Catalysts for Ammonia Selective Catalytic Reduction

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Abstract

There is an ongoing debate on the structure of titania supported vanadia used for catalytic partial oxidation reactions as well as for abatement of nitrogen oxide (NOx) by ammonia selective catalytic reduction (NH3-SCR). To gain further insight into the essential features of the catalyst composition of the surface we introduce a new class of vanadia model catalysts based on monodispersed silica particles as a platform. The evaluation of the influence of different catalyst components (TiO2, WO3) and different vanadia synthesis approaches (incipient wetness, ion-exchange) is facilitated by the hierarchical structure of the catalysts as well as the controlled synthesis approach. Catalysts tested under industrial ammonia SCR conditions show a strong dependence on the catalyst composition. In particular, the presence of crystalline titania and tungsta leads to a strong increase in NO conversion. Detailed catalyst characterization by X-ray diffraction and by visible Raman, UV Raman, UV–Vis and X-ray photoelectron spectroscopies provides insight into the bulk structure, the surface composition as well as the vanadia surface structure of the catalysts. The potential of UV resonance Raman spectroscopy for structural analysis of vanadia model catalysts for SCR is highlighted. Differences in catalytic activity are discussed in light of the structural results and the available literature.

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Notes

  1. The subtraction of the crystalline contributions was performed as part of a fit analysis taking the TiO2- and WO3-related peaks in the spectra of VOx/TiO2/SiO2 (iwi) and VOx/WO3/TiO2/SiO2 (iwi) as a basis.

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Acknowledgements

The authors would like to thank Karl Kopp, Nicolas Sobel, and Anastasia Filtschew for help with the ALD coatings, some of the spectroscopic experiments, and technical support. The authors also thank Jean-Christophe Jaud (TU Darmstadt) from the research group of Wolfgang Donner (TU Darmstadt) for performing the XRD experiments and Gitte Marquardt (Haldor Topsøe) for performing the activity measurements. C.H. gratefully acknowledges the Alexander von Humboldt-Foundation for supporting his stay at Haldor Topsøe.

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Authors and Affiliations

  1. Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technische Universität Darmstadt, Alarich-Weiss-Str. 8, 64287, Darmstadt, Germany

    Christian Hess, Philipp Waleska & Michaela Ratzka

  2. Haldor Topsøe A/S, Nymøllevej 55, 2800, Kongens Lyngby, Denmark

    Ton V. W. Janssens, Søren B. Rasmussen & Pablo Beato

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  1. Christian Hess
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  2. Philipp Waleska
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  3. Michaela Ratzka
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  4. Ton V. W. Janssens
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  5. Søren B. Rasmussen
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  6. Pablo Beato
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Corresponding authors

Correspondence to Christian Hess or Søren B. Rasmussen.

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Hess, C., Waleska, P., Ratzka, M. et al. Hierarchical Vanadia Model Catalysts for Ammonia Selective Catalytic Reduction. Top Catal 60, 1631–1640 (2017). https://doi.org/10.1007/s11244-017-0843-8

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