Speciation of Heptavalent Technetium in Sulfuric Acid: Structural and Spectroscopic Studies.

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The speciation of Tc(VII) in 12 M sulfuric acid was studied by NMR, UV-visible and XAFS spectroscopy, experimental results were supported by DFT calculation and were in agreement with the formation of TcO{sub 3}OH(H{sub 2}O){sub 2}. In summary, the speciation of heptvalent technetium has been investigated in sulfuric acid. In 12 M H{sub 2}SO{sub 4}, a yellow solution is observed, and its {sup 99}Tc NMR spectrum is consistent with a heptavalent complex. The yellow solution was further characterized by EXAFS spectroscopy, and results are consistent with the formation of TcO{sub 3}(OH)(H{sub 2}O){sub 2}. No technetium heptoxide or sulfato- complexes were ... continued below

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Poineau, Frederic; Weck, Philippe F.; German, Konstantin; Maruk, Alesya; Kirakosyan, Gayane; Lukens, Wayne et al. June 10, 2010.

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The speciation of Tc(VII) in 12 M sulfuric acid was studied by NMR, UV-visible and XAFS spectroscopy, experimental results were supported by DFT calculation and were in agreement with the formation of TcO{sub 3}OH(H{sub 2}O){sub 2}. In summary, the speciation of heptvalent technetium has been investigated in sulfuric acid. In 12 M H{sub 2}SO{sub 4}, a yellow solution is observed, and its {sup 99}Tc NMR spectrum is consistent with a heptavalent complex. The yellow solution was further characterized by EXAFS spectroscopy, and results are consistent with the formation of TcO{sub 3}(OH)(H{sub 2}O){sub 2}. No technetium heptoxide or sulfato- complexes were detected in these conditions. The molecular structure of TcO{sub 3}(OH)(H{sub 2}O){sub 2} has been optimized by DFT techniques, and the structural parameters are well in accordance with those found by XAFS spectroscopy. The experimental electronic spectra exhibit ligand-to-metal charge transfer transitions that have been assigned using TDDFT methods. Calculations demonstrate the theoretical electronic spectrum of TcO{sub 3}(OH)(H{sub 2}O){sub 2} to be in very good agreement with the experimental one. Recent experiments in 12 M H{sub 2}SO{sub 4} show the yellow solution to be very reactive in presence of reducing agents presumably forming low valent Tc species. Current spectroscopic works focus on the speciation of these species.

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  • Journal Name: JCS Dalton; Journal Volume: 39; Journal Issue: 37

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  • Report No.: LBNL-4198E
  • Grant Number: DE-AC02-05CH11231
  • Office of Scientific & Technical Information Report Number: 1004412
  • Archival Resource Key: ark:/67531/metadc834052

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  • June 10, 2010

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  • May 19, 2016, 3:16 p.m.

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  • July 26, 2016, 5:48 p.m.

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Poineau, Frederic; Weck, Philippe F.; German, Konstantin; Maruk, Alesya; Kirakosyan, Gayane; Lukens, Wayne et al. Speciation of Heptavalent Technetium in Sulfuric Acid: Structural and Spectroscopic Studies., article, June 10, 2010; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc834052/: accessed October 19, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.