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

Lukens, Wayne W.; Saslow, Sarah A.

doi:10.1039/C8DT01356J

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 · 01 January 2018 · Dalton Transactions

DOI:https://doi.org/10.1039/C8DT01356J· OSTI ID:1485476

^[1]; ^[2]

Chemical Sciences Division; Lawrence Berkeley National Laboratory; Berkeley; USA
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 Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Environmental Management (EM)

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1485476

Report Number(s):: PNNL-SA-132453; ICHBD9

Journal Information:: Dalton Transactions, Vol. 47, Issue 30; ISSN 1477-9226

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

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