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Title: Speciation of technetium peroxo complexes in sulfuric acid revisited

We found that the reaction of Tc(+7) with H 2O 2 has been studied in H 2SO 4 and the speciation of technetium performed by UV–visible and 99-Tc NMR spectroscopy. UV–visible measurements show that for H 2SO 4 ≥ 9 M and H 2O 2 = 0.17 M, TcO 3(OH)(H 2O) 2 reacts immediately and blue solutions are obtained, while no reaction occurs for H 2SO 42SO 44 - begins to react for H 2O 2 = 2.12 M and red solutions are obtained. The UV–visible spectra of the red species are identical to the one obtained from the reaction of TcO 4 - with H 2O 2 in HNO 3 and consistent with the presence of TcO(O 2) 2(H 2O)(OH). The 99-Tc NMR spectrum of the red solution exhibits a broad signal centered at +5.5 ppm vs TcO 4 - and is consistent with the presence of a low symmetry Tc(+7) molecule.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [1] ;  [5] ;  [2] ;  [6] ;  [3] ;  [7] ;  [1]
  1. Univ. of Nevada, Las Vegas, NV (United States)
  2. Russian Academy of Sciences (RAS), Moscow (Russian Federation)
  3. Hunter College, New York, NY (United States)
  4. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  5. Medical Inst. REAVIZ, Moscow (Russian Federation)
  6. Russian Academy of Sciences (RAS), Moscow (Russian Federation); Medical Inst. REAVIZ, Moscow (Russian Federation)
  7. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Report Number(s):
SAND-2013-8259J
Journal ID: ISSN 0236-5731; PII: 3434
Grant/Contract Number:
AC04-94AL85000
Type:
Accepted Manuscript
Journal Name:
Journal of Radioanalytical and Nuclear Chemistry
Additional Journal Information:
Journal Volume: 303; Journal Issue: 2; Journal ID: ISSN 0236-5731
Publisher:
Springer
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; technetium; peroxo complexes; speciation; sulfuric acid
OSTI Identifier:
1113042

Poineau, Frederic, German, Konstantin E., Burton-Pye, Benjamin P., Weck, Philippe F., Kim, Eunja, Kriyzhovets, Olga, Safonov, Aleksey, Ilin, Viktor, Francesconi, Lynn C., Sattelberger, Alfred P., and Czerwinski, Kenneth R.. Speciation of technetium peroxo complexes in sulfuric acid revisited. United States: N. p., Web. doi:10.1007/s10967-014-3434-1.
Poineau, Frederic, German, Konstantin E., Burton-Pye, Benjamin P., Weck, Philippe F., Kim, Eunja, Kriyzhovets, Olga, Safonov, Aleksey, Ilin, Viktor, Francesconi, Lynn C., Sattelberger, Alfred P., & Czerwinski, Kenneth R.. Speciation of technetium peroxo complexes in sulfuric acid revisited. United States. doi:10.1007/s10967-014-3434-1.
Poineau, Frederic, German, Konstantin E., Burton-Pye, Benjamin P., Weck, Philippe F., Kim, Eunja, Kriyzhovets, Olga, Safonov, Aleksey, Ilin, Viktor, Francesconi, Lynn C., Sattelberger, Alfred P., and Czerwinski, Kenneth R.. 2014. "Speciation of technetium peroxo complexes in sulfuric acid revisited". United States. doi:10.1007/s10967-014-3434-1. https://www.osti.gov/servlets/purl/1113042.
@article{osti_1113042,
title = {Speciation of technetium peroxo complexes in sulfuric acid revisited},
author = {Poineau, Frederic and German, Konstantin E. and Burton-Pye, Benjamin P. and Weck, Philippe F. and Kim, Eunja and Kriyzhovets, Olga and Safonov, Aleksey and Ilin, Viktor and Francesconi, Lynn C. and Sattelberger, Alfred P. and Czerwinski, Kenneth R.},
abstractNote = {We found that the reaction of Tc(+7) with H2O2 has been studied in H2SO4 and the speciation of technetium performed by UV–visible and 99-Tc NMR spectroscopy. UV–visible measurements show that for H2SO4 ≥ 9 M and H2O2 = 0.17 M, TcO3(OH)(H2O)2 reacts immediately and blue solutions are obtained, while no reaction occurs for H2SO42SO44 - begins to react for H2O2 = 2.12 M and red solutions are obtained. The UV–visible spectra of the red species are identical to the one obtained from the reaction of TcO4 - with H2O2 in HNO3 and consistent with the presence of TcO(O2)2(H2O)(OH). The 99-Tc NMR spectrum of the red solution exhibits a broad signal centered at +5.5 ppm vs TcO4 - and is consistent with the presence of a low symmetry Tc(+7) molecule.},
doi = {10.1007/s10967-014-3434-1},
journal = {Journal of Radioanalytical and Nuclear Chemistry},
number = 2,
volume = 303,
place = {United States},
year = {2014},
month = {8}
}