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Facile incorporation of technetium into magnetite, magnesioferrite, and hematite by formation of ferrous nitrate in situ : precursors to iron oxide nuclear waste forms

Journal Article · · Dalton Transactions
DOI:https://doi.org/10.1039/C8DT01356J· OSTI ID:1485476
 [1];  [2]
  1. Chemical Sciences Division; Lawrence Berkeley National Laboratory; Berkeley; USA
  2. Geosciences Division; Pacific Northwest National Laboratory; Richland; USA
Technetium (99Tc) is a problematic fission product for the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate, the stable Tc species in aerobic environments. One approach to preventing 99Tc contamination is using durable waste forms based on environmentally stable natural analogs such as hematite (-Fe2O3) or magnesioferrite (MgFe2O4). The incorporation of Tc into hematite, magnesioferrite, and magnetite (Fe3O4) by means of simple, aqueous chemistry is presented starting from TcO4- in 5 M nitric acid. A combination of X-ray diffraction and X-ray absorption fine structure spectroscopy reveals that Tc(IV) replaces Fe(III) within the iron oxide structures. Following incorporation, Tc doped samples were suspended in deionized water under aerobic conditions, and the release rate of Tc under these conditions was determined. The results of this work show that Tc leaches more quickly from Fe3O4 than from -Fe2O3 or MgFe2O4.
Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Environmental Management (EM)
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1485476
Report Number(s):
PNNL-SA-132453
Journal Information:
Dalton Transactions, Journal Name: Dalton Transactions Journal Issue: 30 Vol. 47; ISSN 1477-9226; ISSN ICHBD9
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English

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The abiotic reductive removal and subsequent incorporation of Tc( iv ) into iron oxides: a frontier review journal January 2019

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