Fundamental chemistry, Characterization, and Separation of Technetium Complexes in Hanford Waste Page: 4 of 4
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excess IDA), Tc-nitrido-IDA, 6, Tc-nitrido-EDDA, 7, Tc-EDDA (8, with holding reductant,
HSO3, and excess EDDA). All the samples are dissolved in water except for Tc-nitrido-EDDA,
which is in 0.05 M NaOH. All the samples were approximate 1 x 10-3 M. Samples 1, 3, 5 and 8
look like Tc(IV) species. Samples 1, 5 and 8 were stable while 3 showed some decomposition.
The stability of 5 relative to 3 was apparently due to the excess reductant and IDA present; a
situation not unlike a Hanford tank waste environment where complexant concentrations are
large relative to technetium and radiolysis maintains a reducing environment. Samples 2 and 4
were stable and appear to be Tc(V) species. The Oxidation State of 6 and 7 are unclear at this
point; however 7 appeared to decompose. It should be noted that those samples that showed
decomposition did not appear to be forming pertechnetate on the time scale of this experiment,
three weeks. However, samples 1, 2, and 3, at 5 x 105 M, decomposed to pertechnetate within 24
hours during an attempted analysis by capillary electrophoresis mass spectrometry. Lastly the X-
ray absorption fine structure spectroscopy (EXAFS) suggested that the red IDA complex is
monomeric, the blue IDA complex is dimeric, and the Tc-EDDA is a polynuclear complex.
3. PLANNED ACTIVITIES: Future efforts are being directed towards fully characterizing
these complexes. Pure samples have already been prepared using size exclusion chromatography
and are awaiting FT-Raman analysis at the CMR building here at LANL. In addition, samples
are being prepared for shipment to Atlantic Microlabs in Georgia for elemental analysis. We also
have time scheduled in July at the synchotron facility at Stanford for x-ray absorption analysis in
collaboration with David Blanchard from PNNL.
4. INFORMATION ACCESS: A talk on this work will be presented at the EMSP symposium
at the American Chemical Society meeting this August in New Orleans. Recent publications
dealing with the technetium speciation problem are listed below.
Norman C. Schroeder, Susan D. Radzinski, Kenneth R. Ashley, Anh P. Truong, and Patrycja A.
Szczepaniak, iTechnetium Oxidation State Adjustment for Hanford Waste Processing,i in
Science and Technology for Disposal of Radioactive Tank Waste, N. J. Lombardo and W. W.
Schulz, eds., Plenum Publishing Corporation, New York, NY, (1998).
K. R. Ashley, G. D. Whitener, N. C. Schroeder, J. R. Ball, and S. D. Radzinski, in Progress in
Metal Ion Separation and Preconcentration, ACS Symposium Series 716, A. H. Bond, M. L.
Dietz, and R. D. Rogers, Eds., American Chemical Society, Washington, D C., 1999, p. 219.
Norman C. Schroeder, Susan D. Radzinski, Kenneth R. Ashley, Anh P. Truong, Glenn D.
Whitener, "Feed Adjustment Chemistry for Hanford 101-SY and 103-SY Tank Waste: Attempts
to Oxidize the Non-Pertechnetate Species," in preparation.
Norman C. Schroeder, Jason R. Ball, and Susan D. Radzinski Kenneth R. Ashley Kenneth R.
Ashley, "Reillex6-HPQ Anion Exchange Column Chromatography: Removal of Pertechnetate
from DSSF-5 Simulant at Various Flow Rates," submitted to Solvent Extraction and Ion
Exchange.
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Schroeder, Norman C.; Blanchard, David L., Jr. & Ashley, Kenneth R. Fundamental chemistry, Characterization, and Separation of Technetium Complexes in Hanford Waste, report, June 1999; Los Alamos, New Mexico. (https://digital.library.unt.edu/ark:/67531/metadc786929/m1/4/: accessed April 19, 2024), University of North Texas Libraries, UNT Digital Library, https://digital.library.unt.edu; crediting UNT Libraries Government Documents Department.