Incorporation of H2 in vitreous silica, qualitative and quantitative determination from Raman and infrared spectroscopy.
Résumé
Incorporation mechanisms of H2 in silica glass were studied with Raman and infrared (IR) microspectroscopy. Hydrogenated samples were prepared at temperatures between 800°C and 955°C at 2 kbar total pressure. Hydrogen fugacities (fH2) were controlled using the double capsule technique with the iron–wüstite (IW) buffer assemblage generating fH2 of 1290–1370 bars corresponding to H2 partial pressures (PH2) of 960–975 bars. We found that silica glass hydrogenated under such conditions contains molecular hydrogen (H2) in addition to SiH and SiOH groups. H2 molecules dissolved in the quenched glasses introduce a band at 4136 cm−1 in the Raman spectra which in comparison to that of gaseous H2 is wider and is shifted to lower frequency. IR spectra of hydrogenated samples contain a band at 4138 cm−1 which we assign to the stretching vibration of H2 molecules located in non-centrosymmetric sites. The Raman and IR spectra indicate that the dissolved H2 molecules interact with the silicate network. We suggest that the H2 band is the envelope of at least three components due to the occupation of at least three different interstitial sites by H2 molecules. Both, Raman and IR spectra of hydrogenated glasses contain bands at not, vert, similar2255 cm−1 which may be due to the vibration of SiH groups.
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