Impeding 99Tc(IV) mobility in novel waste forms

Mal-Soon Lee, Wooyong Um (), Guohui Wang, Albert A. Kruger, Wayne W. Lukens, Roger Rousseau and Vassiliki-Alexandra Glezakou ()
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Mal-Soon Lee: Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland
Wooyong Um: Energy and Environment Directorate, Pacific Northwest National Laboratory
Guohui Wang: Energy and Environment Directorate, Pacific Northwest National Laboratory
Albert A. Kruger: Office of River Protection
Wayne W. Lukens: Lawrence Berkeley National Laboratory
Roger Rousseau: Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland
Vassiliki-Alexandra Glezakou: Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland

Nature Communications, 2016, vol. 7, issue 1, 1-6

Abstract: Abstract Technetium (99Tc) is an abundant, long-lived radioactive fission product whose mobility in the subsurface is largely governed by its oxidation state. Tc immobilization is crucial for radioactive waste management and environmental remediation. Tc(IV) incorporation in spinels has been proposed as a novel method to increase Tc retention in glass waste forms during vitrification. However, experiments under high-temperature and oxic conditions show reoxidation of Tc(IV) to volatile pertechnetate, Tc(VII). Here we examine this problem with ab initio molecular dynamics simulations and propose that, at elevated temperatures, doping with first row transition metal can significantly enhance Tc retention in magnetite in the order Co>Zn>Ni. Experiments with doped spinels at 700 °C provide quantitative confirmation of the theoretical predictions in the same order. This work highlights the power of modern, state-of-the-art simulations to provide essential insights and generate theory-inspired design criteria of complex materials at elevated temperatures.

Date: 2016
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DOI: 10.1038/ncomms12067

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