Geochemical evidence for the application of nanoparticulate colloidal silica gel for in-situ containment of legacy nuclear wastes

Pieter Bots, Joanna Renshaw, Timothy E. Payne, M. Josick Comarmond, Alexandra E.P. Schellenger, Matteo Pedrotti, Eleonora Calì, Rebecca J. Lunn

Research output: Contribution to journalArticle

Abstract

Colloidal silica is a nanoparticulate material that could have a transformative effect on environmental risk management at nuclear legacy sites through their use in in-situ installation of injectable hydraulic barriers. In order to utilize such
nanoparticulate material as a barrier, we require detailed understanding of its impact on the geochemistry of radionuclides in the environment (e.g. fission products such as Sr and Cs). Here we show, through combining leaching experiments with XAS analyses, that colloidal silica induces several competing effects on the mobility of Sr and Cs. First, cations within the colloidal silica gel compete with Sr and Cs for surface complexation sites. Second, an increased number of surface complexation sites is provided by the silica nanoparticles and finally, the elevated pH within the colloidal silica increases the surface complexation to clay minerals and the silica nanoparticles. XAS analyses show that Sr and Cs complex predominantly with the clay mineral phases in the soil through inner-sphere surface complexes (Sr) and through complexation on the clay basal surfaces at Si vacancy sites (Cs). For binary soil – colloidal silica gel systems, a fraction of the Sr and Cs complexes with the amorphous silica-like surfaces through the formation of outer-sphere surface complexes. Importantly, the net effect of nanoparticulate colloidal silica gel is to increase the retention of Sr and Cs, when compared to untreated soil and waste materials. Our research opens the door to applications of colloidal silica gel to form barriers within risk management strategies at legacy nuclear sites.
Original languageEnglish
Pages (from-to)1481-1495
Number of pages15
JournalEnvironmental Science: Nano
Volume7
Issue number5
Early online date30 Mar 2020
DOIs
Publication statusPublished - 1 May 2020

Keywords

  • colloidal silica
  • environmental risk management
  • radionuclides
  • legacy nuclear waste

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  • The DISTINCTIVE university consortium: structural integrity

    Lunn, R., Hamilton, A., Pedrotti, M., Bots, P., Wong, C., El Mountassir, G., Renshaw, J., Maddalena, R., Zhao, C., Sun, L., Stolkin, R., Fairweather, M., Tovey, L., Boxall, C., Hriljac, J., Hyatt, N., Kaltsoyannis, N., Lee, W., Read, D. & Scott, T., 19 Jun 2018, 44th Annual Waste Management Conference (WM2018) : Nuclear and Industrial Robotics, Remote Systems and Other Emerging Technology. Tempe, Arizona, p. 6195-6209 15 p. 18272

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