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Catalysts 2018, 8(9), 356; https://doi.org/10.3390/catal8090356

Structural Evolution of Highly Active Multicomponent Catalysts for Selective Propylene Oxidation

1
Institute for Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology, Engesserstraße 20, 76131 Karlsruhe, Germany
2
Institute of Catalysis Research and Technology, Karlsruhe Institute of Technology, Hermann-von-Helmholtz Platz 1, 76344 Eggenstein-Leopoldshafen, Germany
3
ESRF—The European Synchrotron, 71 Avenue des Martyrs, 38000 Grenoble, France
*
Authors to whom correspondence should be addressed.
Received: 3 August 2018 / Revised: 23 August 2018 / Accepted: 24 August 2018 / Published: 27 August 2018
(This article belongs to the Section Metal Catalysis)
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Abstract

Multicomponent Bi-Mo-Fe-Co oxide catalysts prepared via flame spray pyrolysis were tested for selective propylene oxidation, showing high conversion (>70%) and selectivity (>85%) for acrolein and acrylic acid at temperatures of 330 °C. During extended time-on-stream tests (5–7 days), the catalysts retained high activity while undergoing diverse structural changes. This was evident on: (a) the atomic scale, using powder X-ray diffraction, Raman spectroscopy, X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy; and (b) the microscopic scale, using synchrotron X-ray nanotomography, including full-field holotomography, scanning X-ray fluorescence, and absorption contrast imaging. On the atomic scale, sintering, coke formation, growth, and transformation of active and spectator components were observed. On the microscopic scale, the catalyst life cycle was studied at various stages through noninvasive imaging of a ~50-µm grain with 100-nm resolution. Variation of catalyst synthesis parameters led to the formation of notably different structural compositions after reaction. Mobile bismuth species formed agglomerates of several hundred nanometres and segregated within the catalyst interior. This appeared to facilitate the formation of different active phases and induce selectivity for acrolein and acrylic acid. The combined multiscale approach here is generally applicable for deconvolution of complex catalyst systems. This is an important step to bridge model two-component catalysts with more relevant but complex multicomponent catalysts. View Full-Text
Keywords: bismuth molybdate; heterogeneous catalysis; Raman spectroscopy; selective oxidation; synchrotron radiation; tomography; X-ray absorption spectroscopy; X-ray microscopy bismuth molybdate; heterogeneous catalysis; Raman spectroscopy; selective oxidation; synchrotron radiation; tomography; X-ray absorption spectroscopy; X-ray microscopy
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).

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Sprenger, P.; Sheppard, T.L.; Suuronen, J.-P.; Gaur, A.; Benzi, F.; Grunwaldt, J.-D. Structural Evolution of Highly Active Multicomponent Catalysts for Selective Propylene Oxidation. Catalysts 2018, 8, 356.

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