NSUF 14-448: Synchrotron XAS and EXAFS Study of Technetium-99 Relevant to the Nuclear Fuel Cycle

The synchrotron radiation techniques of X-ray Absorption Near Edge Spectroscopy (XANES) and Extended X-ray Absorption Fine Structure (EXAFS) Spectroscopy are among the very few techniques giving oxidation state and nearest neighbor information in compounds and materials that do not crystallize suitably or are not available in sufficient quantities for X-ray diffraction analysis. Technetium-99 is an important radionuclide in the nuclear fuel cycle as a major fission product from both uranium and plutonium, and in environmental remediation at nuclear sites such as the DOE site in Hanford, Washington. We propose to perform XANES and EXAFS experiments at the Advanced Photon Source at Argonne National Laboratory (APS, Argonne, IL) to determine the end products of immobilization reactions of pertechnetate with sulfide in the presence of various olefinic acids. The results will allow us to determine the oxidation state of the Tc and the nearest neighbors to the Tc metal center (i.e., its coordination environment). The information will provide mechanistic information on the factors influencing the immobilization reaction that are important in both environmental remediation and potential nuclear fuel reprocessing technologies. We believe that understanding the products of these Tc reactions will allow the development of better immobilization methods and may lead to potential separation methods. It should be fairly straightforward to analyze the Tc compounds and the goal is to have this data analyzed quickly. To provide a base for further exploration, we propose to perform the work and the analysis over the years 2013-2014.

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Abstract The synchrotron radiation techniques of X-ray Absorption Near Edge Spectroscopy (XANES) and Extended X-ray Absorption Fine Structure (EXAFS) Spectroscopy are among the very few techniques giving oxidation state and nearest neighbor information in compounds and materials that do not crystallize suitably or are not available in sufficient quantities for X-ray diffraction analysis. Technetium-99 is an important radionuclide in the nuclear fuel cycle as a major fission product from both uranium and plutonium, and in environmental remediation at nuclear sites such as the DOE site in Hanford, Washington. We propose to perform XANES and EXAFS experiments at the Advanced Photon Source at Argonne National Laboratory (APS, Argonne, IL) to determine the end products of immobilization reactions of pertechnetate with sulfide in the presence of various olefinic acids. The results will allow us to determine the oxidation state of the Tc and the nearest neighbors to the Tc metal center (i.e., its coordination environment). The information will provide mechanistic information on the factors influencing the immobilization reaction that are important in both environmental remediation and potential nuclear fuel reprocessing technologies. We believe that understanding the products of these Tc reactions will allow the development of better immobilization methods and may lead to potential separation methods. It should be fairly straightforward to analyze the Tc compounds and the goal is to have this data analyzed quickly. To provide a base for further exploration, we propose to perform the work and the analysis over the years 2013-2014.
Award Announced Date 2013-11-22T00:00:00
Awarded Institution None
Facility None
Facility Tech Lead Jeff Terry
Irradiation Facility None
PI Silvia Jurisson
PI Email [email protected]
Project Type APS
RTE Number 448