Journal article
Chemical Trends in Solid Alkali Pertechnetates
Inorganic chemistry, Vol.56(5), pp.2533-2544
03/06/2017
Handle:
https://hdl.handle.net/2376/108838
PMID: 28221786
Abstract
Insight into the solid-state chemistry of pure technetium-99 (99Tc) oxides is required in the development of a robust immobilization and disposal system for nuclear waste stemming from the radiopharmaceutical industry, from the production of nuclear weapons, and from spent nuclear fuel. However, because of its radiotoxicity and the subsequent requirement of special facilities and handling procedures for research, only a few studies have been completed, many of which are over 20 years old. In this study, we report the synthesis of pure alkali pertechnetates (sodium, potassium, rubidium, and cesium) and analysis of these compounds by Raman spectroscopy, X-ray absorption spectroscopy (XANES and EXAFS), solid-state nuclear magnetic resonance (static and magic angle spinning), and neutron diffraction. The structures and spectral signatures of these compounds will aid in refining the understanding of 99Tc incorporation into and release from nuclear waste glasses. NaTcO4 shows aspects of the relatively higher electronegativity of the Na atom, resulting in large distortions of the pertechnetate tetrahedron and deshielding of the 99Tc nucleus relative to the aqueous TcO4 –. At the other extreme, the large Cs and Rb atoms interact only weakly with the pertechnetate, have closer to perfect tetrahedral symmetry at the Tc atom, and have very similar vibrational spectra, even though the crystal structure of CsTcO4 is orthorhombic while that of RbTcO4 is tetragonal. Further trends are observed in the cell volume and quadrupolar coupling constant.
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Details
- Title
- Chemical Trends in Solid Alkali Pertechnetates
- Creators
- Jamie Weaver - Pacific Northwest National LaboratoryChuck Z Soderquist - Pacific Northwest National LaboratoryNancy M Washton - Pacific Northwest National LaboratoryAndrew S Lipton - Pacific Northwest National LaboratoryPaul L Gassman - Pacific Northwest National LaboratoryWayne W Lukens - Lawrence Berkeley National LaboratoryAlbert A Kruger - U.S. Department of Energy (DOE), Office of River ProtectionNathalie A Wall - Department of ChemistryJohn S McCloy - Washington State University
- Publication Details
- Inorganic chemistry, Vol.56(5), pp.2533-2544
- Academic Unit
- Chemistry, Department of; Mechanical and Materials Engineering, School of
- Publisher
- American Chemical Society
- Identifiers
- 99900546768401842
- Language
- English
- Resource Type
- Journal article