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Prognosticating the humic complexation for redox sensitive actinides through analogy, using the charge neutralisation model

Pascal E. Reiller 1, *
* Corresponding author
1 LSRM - Laboratoire de Spéciation des Radionucléides et des Molécules
DPC - Département de Physico-Chimie : DEN/DPC
Abstract : The complexation of redox sensitive elements by humic acid (HA), described through the charge neutralisation model (CNM), has been reviewed in order to have a comprehensive scope. The data acquired in HUMICS program on thorium(IV), and data available in the literature, were reinterpreted according to the CNM, and adapted to uranium(IV), neptunium(IV) and plutonium(IV) through analogy in order to draw a boundary prediction. Otherwise, availabledata obtained in the framework of the CNM were used, or adapted if necessary, for other redox states when the analogy is justified, i.e. Am3+-Cm3+ for Pu3+, NpO2+ for PuO2+ and UO22+ for PuO22+. The obtained speciation diagrams indicate that, when(HA) =100 mg/L, redox sensitive actinides should be reduced to their +IV state when Eh ≤ 650mV/SHE for plutonium, Eh ≤ 100 mV/SHE for neptunium and Eh ≤−20 mV/SHE for U. Plutonium could be present as mixtures of plutonium(III) and (IV) depending on the pH value in reducing ground waters −150 ≤ Eh(mV/SHE) ≤ 150. The known reduction of neptunium(V) to neptunium(IV) in Gorleben ground waters seems also well represented, so is the stability of uranium(VI) in humic solution when Eh ≥ 100 mV/SHE. Conversely, the known association of plutonium(VI) in marine systems is not satisfactorily represented, so does is the uranium behaviour under reducing conditions. Experiments under well-controlled conditions are still needed to ascertain the plutonium and uranium comportment in the presence of humic acid.
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Pascal E. Reiller. Prognosticating the humic complexation for redox sensitive actinides through analogy, using the charge neutralisation model. Radiochimica Acta, R Oldenbourg Verlag GMBH, 2005, 93 (1), pp.43-55. ⟨10.1524/ract.⟩. ⟨cea-00278016⟩



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