SULFUR SPECIATION AND NETWORK STRUCTURAL CHANGES IN SODIUM SILICATE GLASSES: CONSTRAINTS FROM NMR AND RAMAN SPECTROSCOPY

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dc.contributor.author Tsujimura T.
dc.contributor.author Xue X.
dc.contributor.author Kanzaki M.
dc.contributor.author Walter M.J.
dc.date.accessioned 2022-07-05T05:55:42Z
dc.date.available 2022-07-05T05:55:42Z
dc.date.issued 2004
dc.identifier https://www.elibrary.ru/item.asp?id=20995658
dc.identifier.citation Geochimica et Cosmochimica Acta, 2004, 68, 24, 5081-5101
dc.identifier.issn 0016-7037
dc.identifier.uri https://repository.geologyscience.ru/handle/123456789/37928
dc.description.abstract Information about the state of sulfur in silicate melts and glasses is important in both earth sciences and materials sciences. Because of its variety of valence states from S2− (sulfide) to S6+ (sulfate), the speciation of sulfur dissolved in silicate melts and glasses is expected to be highly dependent on the oxygen fugacity. To place new constraint on this issue, we have synthesized sulfur-bearing sodium silicate glasses (quenched melts) from starting materials containing sulfur of different valence states (Na2SO4, Na2SO3, Na2S2O3 and native S) using an internally heated gas pressure vessel, and have applied electron-induced SKα X-ray fluorescence, micro-Raman and NMR spectroscopic techniques to probe their structure. The wavelength shift of SKα X-rays revealed that the differences in the valence state of sulfur in the starting compounds are largely retained in the synthesized sulfur-bearing glasses, with a small reduction for more oxidized samples. The 29Si MAS NMR spectra of all the glasses contain no peaks attributable to the SiO4-nSn (with n > 0) linkages. The Raman spectra are consistent with the coexistence of sodium sulfate (Na2SO4) species and one or more types of more reduced sulfur species containing S-S linkages in all the sulfur-bearing silicate glasses, with the former dominant in glasses produced from Na2SO4-doped starting materials, and the latter more abundant in more reduced glasses. The 29Si MAS NMR and Raman spectra also revealed changes in the silicate network structure of the sulfur-bearing glasses, which can be interpreted in terms of changes in the chemical composition and sulfur speciation.
dc.title SULFUR SPECIATION AND NETWORK STRUCTURAL CHANGES IN SODIUM SILICATE GLASSES: CONSTRAINTS FROM NMR AND RAMAN SPECTROSCOPY
dc.type Статья


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