Dynamic response of physisorbed hydrogen molecules on lanthanide-modified zirconia nanoparticles
- Argonne National Lab., IL (United States)
- Nagoya Institute of Technology, Tajimi, Gifu (Japan)
Ultrafine lanthanide (Ln = Ce and Nd)-modified zirconia powders synthesized by a coprecipitation method exhibit high surface areas and adsorption sites that are essential for catalytic applications. We report a study of the surface chemistry of Ce{sub 0.1}Zr{sub 0.9}O{sub 2} and Nd{sub 0.1}Zr{sub 0.9}O{sub 1.95} powders. First, the specific surface area and porosity are characterized by nitrogen isotherm-adsorption measurements. Second, the motion of hydrogen molecules physisorbed on Ce- and Nd-doped zirconias is studied by inelastic neutron scattering. Nitrogen adsorption-desorption isotherm measurements yield a BET surface area (26.1 m{sup 2}/g) and mesopore size ({approximately}5 nm radius) in Ce{sub 0.1}Zr{sub 0.9}O{sub 2} as compared to those (72.3 m{sup 2}/g and {approximately}3 nm) in Nd{sub 0.1}Zr{sub 0.9} O{sub 1.95}. The vibrational densities of states of H{sub 2} on Ce{sub 0.1}Zr{sub 0.9}O{sub 2} and Nd{sub 0.1}Zr{sub 0.9}O{sub 1.95} were measured at 20 K over the 0-200 meV energy range for three hydrogen coverage. The spectra for both samples consist of two parts: a sharp peak at {approximately}14.5 meV and a broad component extending beyond 200 meV. The sharp peak corresponds to transitions from the J=0 to J=1 rotational states of bulk hydrogen molecules, and its intensity decreases with decreasing H{sub 2} coverage. The broad component corresponds to overdamped motion of surface adsorbed hydrogen molecules. The major difference in the latter component between the Ce- and Nd-doped samples is an excess of intensities in the 5-14 meV region in Nd{sub 0.1}Zr{sub 0.9}O{sub 1.95}. The confined motion of adsorbed H{sub 2} on the different micropore and mesopore surfaces of Ce{sub 0.1}Zr{sub 0.9}O{sub 2} and Nd{sub 0.1}Zr{sub 0.9}O{sub 1.95} is discussed.
- Research Organization:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- USDOE Office of Energy Research, Washington, DC (United States)
- DOE Contract Number:
- W-31-109-ENG-38
- OSTI ID:
- 565560
- Report Number(s):
- ANL/ER/CP-94630; CONF-970893-; ON: DE98050019; TRN: 98:002488
- Resource Relation:
- Conference: ICNS `97: satellite conference, Argonne, IL (United States), 25-26 Aug 1997; Other Information: PBD: 1997
- Country of Publication:
- United States
- Language:
- English
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