Technetium Stabilization in Low-Solubility Sulfide Phases: A Review

Pearce, Carolyn I.; Icenhower, Jonathan P.; Asmussen, R. Matthew; Tratnyek, Paul G.; Rosso, Kevin M.; Lukens, Wayne W.; Qafoku, Nikolla P.

doi:10.1021/acsearthspacechem.8b00015

Title: Technetium Stabilization in Low-Solubility Sulfide Phases: A Review

Journal Article · Tue May 08 00:00:00 EDT 2018 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.8b00015· OSTI ID:1528900

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sandia National Laboratory, Carlsbad, NM (United States)
Oregon Health & Science Univ., Portland, OR (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Technetium (Tc) contamination remains a major environmental problem at nuclear reprocessing sites, e.g., the Hanford Site, WA, USA. At these site, Tc is present in liquid waste destined for immobilization in a waste form or has been released into the subsurface environment. The high environmental risk associated with Tc is due to its long half-life (213,000 years) and the mobility of the oxidized anionic species Tc(VII)O4-. Under reducing conditions, TcO4- is readily reduced to Tc(IV), which commonly exists as a relatively insoluble and therefore immobile, hydrous Tc oxide (TcO2•nH2O). The stability of Tc(IV) sequestered as solid phases depends on the solubility of the solid and susceptibility to re-oxidation to TcO4-, which in turn depend on the (bio-geo)chemical conditions of the environment and/or nuclear waste streams. Unfortunately, the solubility of crystalline TcO2 or amorphous TcO2•H2O is still above the maximum contaminant level (MCL) established by the US EPA (900 pCi/L), and the kinetics of TcO2 oxidative dissolution can be on the order of days to years. In addition to oxygen, sulfur can form complexes that can significantly affect the adsorption, solubility and re-oxidation potential of Tc, especially Tc(IV). The principal technetium sulfides areTcS2 and Tc2S7 but much less is known about the mechanisms of formation, stabilization and re-oxidation of Tc sulfides. A common assumption is that sulfides are less soluble that their oxyhydrous counterparts. Determination of the molecular structure of Tc2S7 in particular has been hampered by the propensity of this phase to precipitate as an amorphous substance. Recent work indicates that the oxidation state of Tc in Tc2S7 is Tc(IV), in apparent contradiction to its nominal stoichiometry. Technetium is relatively immobile in reduced sediments and soils, but in many cases the exact sink for Tc has not been identified. Experiments and modeling have demonstrated that both abiotic and biologic mechanisms can exert strong controls on Tc mobility and that Tc binding or uptake into sulfide phases can occur. These and similar investigations also show that extended exposure to oxidizing conditions results in transformation of sulfide-stabilized Tc(IV) to a Tc(IV)O2-like phase without formation of measurable dissolved TcO4-, suggesting a solid-state transformation in which Tc(IV)-associated sulfide is preferentially oxidized before the Tc(IV) cation. This transformation of Tc(IV) sulfides to Tc(IV) oxides may be the main process that limits remobilization of Tc as Tc(VII)O4-. The efficacy of the final waste form to retain Tc also strongly depends on the ability of oxidizing species to enter the waste and convert Tc(IV) to Tc(VII). Many waste form designs are reducing (e.g., salt stone), therefore, attempt to restrict access of oxidizing species such that diffusion is the rate-limiting step in remobilization of Tc

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Environmental Management (EM); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC02-05CH11231; SC0001376; AC06-76RL01830

OSTI ID:: 1528900

Alternate ID(s):: OSTI ID: 1601827

Report Number(s):: PNNL-SA-132805; ark:/13030/qt1dd339gd

Journal Information:: ACS Earth and Space Chemistry, Vol. 2, Issue 6; ISSN 2472-3452

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

Citation information provided by
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