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Related Experiment Videos

Hydrogen adsorption kinetics on Pd/Ce0.8Zr0.2O2.

F C Gennari1, C Neyertz, G Meyer

  • 1Centro Atómico Bariloche (CNEA) and Instituto Balseiro (UNCuyo), (8400) SC de Bariloche, A. Bustillo km 9.5, Río Negro, Argentina. gennari@cab.cnea.gov.ar

Physical Chemistry Chemical Physics : PCCP
|May 20, 2006
PubMed
Summary

Hydrogen adsorption on palladium supported on ceria-zirconia is pressure-dependent. High pressures cause severe reduction, forming oxygen vacancies and deactivating the catalyst for future hydrogen uptake.

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Area of Science:

  • Materials Science
  • Catalysis
  • Surface Chemistry

Background:

  • Palladium (Pd) supported on ceria-based oxides is crucial for catalytic applications.
  • Understanding hydrogen adsorption mechanisms on these materials is key to optimizing performance.
  • Ceria-zirconia solid solutions offer enhanced oxygen storage capacity and redox properties.

Purpose of the Study:

  • To investigate hydrogen adsorption and the reduction behavior of Pd/Ce(0.8)Zr(0.2)O(2) under varying hydrogen pressures.
  • To elucidate the impact of reduction on the material's structure and subsequent hydrogen adsorption capacity.
  • To understand the electronic interactions between Pd and the Ce(0.8)Zr(0.2)O(2) support during hydrogen interaction.

Main Methods:

  • Temperature-programmed reduction (TPR)

Related Experiment Videos

  • Volumetric hydrogen adsorption measurements
  • Infrared (IR) spectroscopy

    • Main Results:

    • Hydrogen uptake and reduction rate at 353 K are strongly dependent on hydrogen partial pressure.
    • High hydrogen pressures lead to the reduction of PdO, surface, and bulk Ce(0.8)Zr(0.2)O(2), forming oxygen vacancies even below 373 K.
    • Hydrogen adsorption is largely irreversible, evidenced by increased Ce(3+) electronic transitions and surface dehydroxylation, negatively impacting further adsorption.

    Conclusions:

    • Severe reduction at high hydrogen pressures, while forming oxygen vacancies, leads to irreversible changes.
    • The formation of Ce(3+) and loss of surface hydroxyl groups deactivate the palladium catalyst electronically, reducing its hydrogen uptake capacity and rate.
    • Careful control of hydrogen pressure is necessary to maintain the catalytic activity of Pd/Ce(0.8)Zr(0.2)O(2) for hydrogen adsorption.