1. Molecular to Macroscopic Insights: Technetium immobilization through iron(II) phosphate
- Author
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(0009-0008-0609-7997) Börner, C., Roßberg, A., (0000-0002-0038-1638) Müller, K., Schild, D., Seewald, F., (0000-0002-4505-3865) Stumpf, T., (0000-0003-4433-9500) Mayordomo, N., (0009-0008-0609-7997) Börner, C., Roßberg, A., (0000-0002-0038-1638) Müller, K., Schild, D., Seewald, F., (0000-0002-4505-3865) Stumpf, T., and (0000-0003-4433-9500) Mayordomo, N.
- Abstract
Technetium (Tc) is an element originating mostly from the fission of ²³⁵U and ²³⁹Pu with a yield of 6%.¹ Therefore, ⁹⁹Tc is mainly found in high-level radioactive waste, e.g. from nuclear power or reprocessing plants.² The waste disposal is the subject of numerous studies due to the long half-life of many radionuclides (e.g. ⁹⁹Tc: 2.1 · 10⁵ years)¹ and their high radiotoxicity. One of the most widely accepted strategies is the deep geological underground repository. This approach relies on a multi-barrier system designed to minimize the risk of a worst-case scenario, where water intrusion could lead to the corrosion of the waste canister and the subsequent release of radionuclides. For the long-term safety, including the construction of effective barriers, it is essential to study the interaction of radionuclides with the various minerals present in the repository at a fundamental level. Tc poses a particular challenge due to its complex redox chemistry high mobility in its oxidized form TcO₄¯, under oxidising conditions. However, Tc migration decreases significantly when Tc(VII) is reduced to Tc(IV), as it then forms precipitates or becomes immobilized by mineral surfaces such as Fe(II) minerals.³ Vivianite (Fe₃(PO₄)₂ · 8 H₂O) is a naturally occurring Fe(II) mineral under reducing conditions⁵ and can be formed by microorganisms.⁶ Phosphate phases are already being considered as an immobilisation matrix for other radionuclides relevant in deep geological repositories (e.g. ²³⁵U, ²³⁷Np, ²³⁹Pu, ²⁴³Am).⁷ ⁸ This study investigates the retention of Tc by synthetic vivianite particles as a function of pH, Tc concentration and ionic strength on a macroscopic and molecular scale. In addition, Tc(IV) reoxidation experiments were performed.⁴ The synthesis of vivianite was carried out by precipitation from a solution mixture of an iron(II) sulphate and ammonium hydrogen phosphate, as described by Roldán et al..⁹ The product was characterised by Raman microscopy, Mössbauer spec
- Published
- 2024