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Hydrogen chemisorption on gallium oxide polymorphs.

Sebastián E Collins1, Miguel A Baltanás, Adrian L Bonivardi

  • 1Instituto de Desarrollo Tecnológico para la Industria Química (CONICET, UNL) Güemes 3450, S3000GLN Santa Fe, Argentina.

Langmuir : the ACS Journal of Surfaces and Colloids
|January 26, 2005
PubMed
Summary

Chemisorption of hydrogen on gallia polymorphs reveals two distinct adsorption pathways. This process correlates with surface area and can characterize gallium cation sites on gallium oxide surfaces.

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Area of Science:

  • Surface Science
  • Materials Chemistry
  • Catalysis

Background:

  • Gallium oxide (Ga2O3) polymorphs exhibit diverse surface properties relevant to catalysis and materials science.
  • Understanding hydrogen chemisorption on metal oxides is crucial for various chemical processes.

Purpose of the Study:

  • To investigate the chemisorption of H(2) on alpha-, beta-, and gamma-Ga(2)O(3) polymorphs.
  • To elucidate the reaction pathways, thermodynamics, and surface species involved in hydrogen adsorption.
  • To explore the potential of H(2) chemisorption for characterizing gallia surface properties.

Main Methods:

  • Temperature-programmed adsorption equilibrium (TPA) and desorption (TPD) experiments.
  • In situ transmission infrared spectroscopy to identify surface species and bonding.

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  • Langmuir's adsorption model to determine thermodynamic parameters.

    • Main Results:

    • Two distinct infrared signals (2003 and 1980 cm(-1)) assigned to H bonded to coordinatively unsaturated (cus) gallium cations (tetrahedral and octahedral).
    • A linear correlation was found between the integrated intensity of the Ga-H infrared band and the Brunauer-Emmett-Teller (BET) surface area of gallia.
    • Two chemisorption pathways were identified: an endothermal, homolytic dissociation (Type I) on cus-gallium sites (Deltah(I) = 155 +/- 25 kJ mol(-1)) and an exothermic, heterolytic adsorption on Ga-O-Ga species (desorption energy = 77 +/- 10 kJ mol(-1)).

    Conclusions:

    • Hydrogen dissociatively chemisorbs on all bulk gallium oxide polymorphs via two distinct pathways.
    • H(2) chemisorption can serve as a valuable tool for estimating the specific surface area of gallia.
    • The study provides insights into the nature and proportion of gallium cation coordination sites on gallia surfaces.