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Synthesis of Ceria Supported Iron-Ruthenium Oxide Catalyst and Its Structural Transformation from Subnanometer Clusters to Single Atoms during Fischer-Tropsch Synthesis Reaction

Abstract

Formation of supported metal/metal oxide single-atom catalysts (SAC), as well as their structural evolutions during catalytic reactions, have attracted much research interest in the fields of both inorganic chemistry and catalysis recently. In this work, we report the synthesis of iron (ca. 10 at.%) oxide catalysts with the doping of small-amount (0.50.6 at.%) ruthenium oxide, which have been deposited onto the surface of ceria nanorods by an optimized deposition-precipitation (DP) route. Multiple characterizations including X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM) and nitrogen adsorption/desorption confirmed the identically structural and textural properties of ceria support after the DP step. The aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) combined with electron energy loss spectroscopy (EELS) observed the formation of subnanometer iron species in the fresh samples. Furthermore, the X-ray absorption fine structure (XAFS) technique by the aids of related data-analysis verified the generation of noncrystalline iron oxide clusters composed by Fe3+ ions dominantly. Here, the addition of secondary metal (ruthenium) greatly promoted the dispersion of Fe over the ceria nanorods. After the catalytic reaction of Fischer-Tropsch synthesis (FTS), the transformation from subnanometer iron oxide species to ionic Fe+ single atoms has been revealed and confirmed by the corresponding profile fits on the extended X-ray absorption fine structure (EXAFS) spectra. In contrast to the normal coarsening process, the FTS conditions (up to 300 C, 2 MPa, CO/H2 = 1/1) did drive the creation of such iron single atoms solely coordinated by oxygen ions.

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Publication details

The article was received on 08 Aug 2017, accepted on 10 Oct 2017 and first published on 12 Oct 2017


Article type: Research Article
DOI: 10.1039/C7QI00470B
Citation: Inorg. Chem. Front., 2017, Accepted Manuscript
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    Synthesis of Ceria Supported Iron-Ruthenium Oxide Catalyst and Its Structural Transformation from Subnanometer Clusters to Single Atoms during Fischer-Tropsch Synthesis Reaction

    X. Wang, X. Fu, W. Yu, C. Ma, C. Jia and R. Si, Inorg. Chem. Front., 2017, Accepted Manuscript , DOI: 10.1039/C7QI00470B

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