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The dissolution mechanism of sulphur in hydrous silicate melts. I: Assessment of analytical techniques in determining the sulphur speciation in iron-free to iron-poor glasses

Research output: Contribution to journalArticle

  • Kevin Klimm
  • Simon C. Kohn
  • Luke A. O'Dell
  • Roman E. Botcharnikov
  • Mark E. Smith
Original languageEnglish
Pages (from-to)237-249
Number of pages13
JournalChemical Geology
Volume322
DOIs
DatePublished - 5 Sep 2012

Abstract

S K-edge XANES, lambda (SK alpha) wavelength shift, S-33 MAS NMR and Raman spectroscopy have been applied to a series of experimentally synthesised hydrous sulphur bearing silicate glasses to determine the oxidation state of sulphur dissolved in the glass. Glasses investigated include soda-lime glass (SLG), K2Si4O9 (KSG) and albitic (Albite) and trondhjemitic (TROND) glass compositions. The four spectroscopic techniques are compared with each other to investigate the applicability of each technique as a method to determine the sulphur oxidation state and structural aspects of sulphur dissolution in silicate melts.

XANES and Raman spectroscopy provide the most comprehensive information on the S-speciation and S6+ and S2- (plus S4+ in the case of XANES) can be detected. XANES allows detection of S-species at lower concentrations (

The linear combination of XANES spectra of glasses containing either only S2- or S6+ provides direct constraints on the S6+/Sigma S of glasses containing a mixture of S2- and S6+. In addition the Raman intensities of bands related to S6+ and S2- can also be used to quantify S6+/Sigma S and determined values are in good agreement with those obtained by XANES at least for S contents of >150 ppm. XANES and Raman both show that the dissolution of S2- is different in Fe-free and Fe-bearing hydrous glasses. In Fe-free glasses S2- is present as SH- and H2S whereas Fe-S complexes are observed in the presence of Fe. (C) 2012 Elsevier B.V. All rights reserved.

    Research areas

  • X-RAY-ABSORPTION, VIBRATIONAL SPECTROSCOPY, S K-edge XANES, FLUID INCLUSIONS, WAVELENGTH SHIFTS, OXIDATION-STATE, lambda (SK alpha) wavelength shift, Raman spectroscopy, Sulphur oxidation state, S-33 MAS NMR, RAMAN-SPECTROSCOPY, BOROSILICATE WASTE GLASSES, INDIVIDUAL PHASES, Silicate glass, XANES SPECTROSCOPY

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