Impeding 99Tc(IV) mobility in novel waste forms

Lee, Mal-Soon; Um, Wooyong; Wang, Guohui; Kruger, Albert A.; Lukens, Wayne W.; Rousseau, Roger; Glezakou, Vassiliki-Alexandra

doi:10.1038/ncomms12067

Title: Impeding ⁹⁹Tc(IV) mobility in novel waste forms

Journal Article · Thu Jun 30 00:00:00 EDT 2016 · Nature Communications

DOI: https://doi.org/10.1038/ncomms12067 · OSTI ID:1282477

Lee, Mal-Soon ^[1]; Um, Wooyong ^[2]; Wang, Guohui ^[3]; Kruger, Albert A. ^[4]; Lukens, Wayne W. ^[5]; Rousseau, Roger ^[1]; Glezakou, Vassiliki-Alexandra ^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Fundamental and Computational Sciences Directorate
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate; Pohang Univ. of Science and Technology (POSTECH) (South Korea)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate
United States Dept. of Energy, Richland, WA (United States). Office of River Protection
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Technetium (⁹⁹Tc) is a long-lived radioactive fission product whose mobility in the subsurface is largely governed by its oxidation state1. Immobilization of Tc in mineral substrates is crucial for radioactive waste management and environmental remediation. Tc(IV) incorporation in spinels2, 3 has been proposed as a novel method to increase Tc retention in glass waste forms. However, experiments with Tc-magnetite under high temperature and oxic conditions showed re-oxidation of Tc(IV) to volatile pertechnetate Tc(VII)O4-.4, 5 Here we address this problem with large-scale ab initio molecular dynamics simulations and propose that elevated temperatures, 1st row transition metal dopants can significantly enhance Tc retention in the order Co > Zn > Ni. Experiments with doped spinels at T=700 ºC provided quantitative confirmation of increased Tc retention in the same order predicted by theory. This work highlights the power of modern state-of-the-art simulations to provide essential insights and generate bottom-up design criteria of complex oxide materials at elevated temperatures.

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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 Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC05-76RL01830; AC02-05CH11231; AC02-76SF00515

OSTI ID:: 1282477

Report Number(s):: PNNL-SA--114552; 830403000

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption Sun, Qi; Zhu, Lin; Aguila, Briana Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09630-y	journal	April 2019
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