PMID: 11918000Mar 29, 2002Paper

Products of pertechnetate radiolysis in highly alkaline solution: structure of TcO2 x xH2O

Environmental Science & Technology
Wayne W LukensDavid K Shuh

Abstract

The chemistry of technetium in certain high-level nuclear waste (HLW) tanks at the Hanford Site complicates the treatment and vitrification of HLW. A major problem is the presence, in certain tanks, of unidentified, lower-valent technetium species, which are difficult to remove from the waste by current separation processes. Radiolytic reduction of TcO4- in alkaline solutions containing selected organic compounds, approximating the conditions in HLW, was investigated to determine the classes of compounds that can be formed under these conditions. Insoluble TcO2 x xH2O is the primary radiolysis product with the majority of organic compounds investigated, including citrate, dibutyl phosphate, and aminopolycarboxylates. X-ray absorption fine structure (XAFS) measurements show that TcO2 x xH2O has a one-dimensional chain structure consisting of edge-sharing TcO6 octahedra with bridging oxide and trans water ligands. When diols, such as ethylene glycol, are present, only soluble, Tc(IV) alkoxide compounds are produced. The XAFS and UV-visible spectra of these compounds provide evidence for a binuclear structure similar to (H2EDTA)2Tc2(mu-O)2. The properties of the Tc(IV) alkoxide complexes were determined and are consistent with tho...Continue Reading

Citations

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Jul 5, 2011·Applied and Environmental Microbiology·Liang ShiJames K Fredrickson
Oct 22, 2015·Environmental Science & Technology·Diana R BrookshawKatherine Morris
Mar 13, 2014·Applied Radiation and Isotopes : Including Data, Instrumentation and Methods for Use in Agriculture, Industry and Medicine·Rūta DruteikienėDalis Baltrūnas
Jan 5, 2017·Environmental Science & Technology·Laura NewsomeJonathan R Lloyd
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May 3, 2019·Journal of Hazardous Materials·Zhihai FuChuanqin Xia
Dec 4, 2019·Journal of Hazardous Materials·Mal-Soon LeeVassiliki-Alexandra Glezakou
Nov 22, 2005·Environmental Science & Technology·Wayne W LukensNorman M Edelstein
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Dec 10, 2016·Environmental Science & Technology·Wayne W LukensDavid K Shuh
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Nov 27, 2021·Environmental Science & Technology·Adam J WilliamsonKatherine Morris

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