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In situ diffraction monitoring of nanocrystals structure evolving during catalytic reaction at their surface

With decreasing size of crystals the number of their surface atoms becomes comparable to the number of bulk atoms and their powder diffraction pattern becomes sensitive to a changing surface structure. On the example of nanocrystalline gold supported on also nanocrystalline [Formula: see text] we sh...

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Detalles Bibliográficos
Autores principales: Zieliński, Maciej, Kaszkur, Zbigniew, Juszczyk, Wojciech, Sobczak, Janusz
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9879985/
https://www.ncbi.nlm.nih.gov/pubmed/36702875
http://dx.doi.org/10.1038/s41598-023-28557-5
Descripción
Sumario:With decreasing size of crystals the number of their surface atoms becomes comparable to the number of bulk atoms and their powder diffraction pattern becomes sensitive to a changing surface structure. On the example of nanocrystalline gold supported on also nanocrystalline [Formula: see text] we show evolution of (a) the background pattern due to chemisorption phenomena, (b) peak positions due to adsorption on nonstoichiometric [Formula: see text] particles, (c) Au peaks intensity. The results of the measurements, complemented with mass spectrometry gas analysis, point to (1) a multiply twinned structure of gold, (2) high mobility of Au atoms enabling transport phenomena of Au atoms to the surface of ceria while varying the amount of Au in the crystalline form, and (3) reversible [Formula: see text] peaks position shifts on exposure to He–X–He where X is O(2), H(2), CO or CO oxidation reaction mixture, suggesting solely internal alternations of the [Formula: see text] crystal structure. We found no evidence of ceria lattice oxygen being consumed/supplied at any stage of the process. The work shows possibility of structurally interpreting different contributions to the multi-phase powder diffraction pattern during a complex physico-chemical process, including effects of physi-, chemisorption and surface evolution. It shows a way to structurally interpret heterogeneous catalytic reactions even if no bulk phase transition is involved.