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Microstructure of Rh-Ce particles on silica: Interactions between Ce and SiO sub 2

Journal Article · · Journal of Catalysis; (United States)
;  [1];  [2]
  1. Univ. of Minnesota, Minneapolis (United States)
  2. UNAM, Mexico City (Mexico)
The authors have characterized the microstructure of Rh/Ce on SiO{sub 2} after heat treatments in H{sub 2} and O{sub 2} using TEM, HREM, XPS, and EELS, focusing on the very stable structures formed after heating in H{sub 2}. After initial reduction at 600 C, Rh is present as 50- to 100-{angstrom} metal particles while the Ce forms a uniform amorphous film of Ce{sup 3+} on the SiO{sub 2}. After oxidation at 600 C, Rh is oxidized to Rh{sub 2}O{sub 3} and spreads over the SiO{sub 2} surface while Ce forms small patches and large (> 1,000 {angstrom}) particles of crystalline CeO{sub 2}. After reduction of the oxidized microstructure at 600 C, Rh metal returns with a less uniform particle size distribution, while Ce is reduced to Ce{sup 3+} and structures indicating strong interactions between Ce and Si are formed. Upon reduction in the presence of Rh, the CeO{sub 2} particles are reduced to crystalline Ce{sub 2}Si{sub 2}O{sub 7}. The Ce silicate nucleates at Rh particles and spreads over the support as large thin single-crystal patches. After reoxidation at 650 C, both Ce silicate and CeO{sub 2} were identified using EELS chemical shifts, indicating that the crystalline silicate, once formed, is stable in oxygen. Ce on SiO{sub 2}also showed interaction between Ce and Si, but no crystalline species formed after reduction and only small crystalline CeO{sub 2} particles formed after oxidation. Thus, the formation of the Ce silicate and the oxidation of Ce to CeO{sub 2} are catalyzed by Rh. This work represents the first direct evidence for the formation of a Ce silicate in this system.
OSTI ID:
7080666
Journal Information:
Journal of Catalysis; (United States), Journal Name: Journal of Catalysis; (United States) Vol. 134:1; ISSN 0021-9517; ISSN JCTLA
Country of Publication:
United States
Language:
English

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