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Speciation of Technetium in Sulfuric Acid/Hydrogen Sulfide Solutions
Author(s) -
Ferrier Maryline,
Roques Jérôme,
Poineau Frederic,
Sattelberger Alfred P.,
Unger Jeremy,
Czerwinski and Kenneth R.
Publication year - 2014
Publication title -
european journal of inorganic chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.667
H-Index - 136
eISSN - 1099-0682
pISSN - 1434-1948
DOI - 10.1002/ejic.201301410
Subject(s) - chemistry , x ray absorption fine structure , sulfuric acid , sulfide , density functional theory , sulfate , spectroscopy , technetium , inorganic chemistry , absorption (acoustics) , hydrogen sulfide , absorption spectroscopy , sulfur , nuclear chemistry , computational chemistry , organic chemistry , acoustics , physics , quantum mechanics
The reaction between Tc VII and H 2 S (g) in 12 M H 2 SO 4 has been studied. This reaction produced a black solid and a brown supernate. The solid was analyzed by energy dispersive X‐ray (EDX) and X‐ray absorption fine structure (XAFS) spectroscopy and the results were consistent with the presence of Tc 2 S 7 . The speciation of technetium in the supernate was performed by UV/Visible and XAFS spectroscopy. Experiments showed that in 12 M H 2 SO 4 an intermediate Tc V sulfate complex was formed. Analysis indicated that the final complex present in solution was a polymeric species with a Tc–O–Tc core coordinated to sulfate ligands. Density Functional Theory (DFT) calculations showed that the proposed complexes were stable and that the theoretical structure was in good agreement with XAFS data.