Uranium(V) incorporation mechanisms and stability in Fe(II)/Fe(III) (oxyhydr)oxides

Hananah E. Roberts, Katherine Morris, Gareth T. W. Law, J. Frederick W. Mosselmans, Pieter Bots, Kristina Kvashnina, Samuel Shaw

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Abstract

Understanding interactions between radionuclides and mineral phases underpins site environmental clean-up and waste management in the nuclear industry. Transport and fate of radionuclides in many subsurface environments are controlled by adsorption, redox and mineral incorporation processes. Interactions of iron (oxyhydr)oxides with uranium have been extensively studied due to the abundance of uranium as an environmental contaminant and ubiquity of iron (oxyhydr)oxides in engineered and natural environments. Despite this, detailed mechanistic information regarding the incorporation of uranium into Fe(II) bearing magnetite and green rust is sparse. Here, we present a co-precipitation study where U(VI) was reacted with environmentally relevant iron(II/III) (oxyhydr)oxide mineral phases. Based on diffraction, microscopic, dissolution and spectroscopic evidence, we show the reduction of U(VI) to U(V) and stabilisation of the U(V) by incorporation within the near-surface and bulk of the particles during co-precipitation with iron (oxyhydr)oxides. U(V) was stable in both magnetite and green rust structures and incorporated via substitution for octahedrally coordinated Fe in a uranate-like coordination environment. As the Fe(II)/Fe(III) ratio increased, a proportion of U(IV) was also precipitated as surface associated UO2. These novel observations have significant implications for the behaviour of uranium within engineered and natural environments.
Original languageEnglish
Pages (from-to)421-426
Number of pages6
JournalEnvironmental Science and Technology Letters
Volume4
Issue number10
Early online date8 Sep 2017
DOIs
Publication statusPublished - 19 Oct 2017

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Keywords

  • radionuclides
  • environmental cleanup
  • waste management
  • nuclear industry

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