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5D operando tomographic diffraction imaging of a catalyst bed

We report the results from the first 5D tomographic diffraction imaging experiment of a complex Ni–Pd/CeO(2)–ZrO(2)/Al(2)O(3) catalyst used for methane reforming. This five-dimensional (three spatial, one scattering and one dimension to denote time/imposed state) approach enabled us to track the che...

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Detalles Bibliográficos
Autores principales: Vamvakeros, A., Jacques, S. D. M., Di Michiel, M., Matras, D., Middelkoop, V., Ismagilov, I. Z., Matus, E. V., Kuznetsov, V. V., Drnec, J., Senecal, P., Beale, A. M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6232103/
https://www.ncbi.nlm.nih.gov/pubmed/30420610
http://dx.doi.org/10.1038/s41467-018-07046-8
Descripción
Sumario:We report the results from the first 5D tomographic diffraction imaging experiment of a complex Ni–Pd/CeO(2)–ZrO(2)/Al(2)O(3) catalyst used for methane reforming. This five-dimensional (three spatial, one scattering and one dimension to denote time/imposed state) approach enabled us to track the chemical evolution of many particles across the catalyst bed and relate these changes to the gas environment that the particles experience. Rietveld analysis of some 2 × 10(6) diffraction patterns allowed us to extract heterogeneities in the catalyst from the Å to the nm and to the μm scale (3D maps corresponding to unit cell lattice parameters, crystallite sizes and phase distribution maps respectively) under different chemical environments. We are able to capture the evolution of the Ni-containing species and gain a more complete insight into the multiple roles of the CeO(2)-ZrO(2) promoters and the reasons behind the partial deactivation of the catalyst during partial oxidation of methane.