0000000000393891
AUTHOR
Nidhu Lal Banik
Stabilization of polynuclear plutonium(IV) species by humic acid
Abstract Although the formation of tetravalent plutonium (Pu(IV)) polymers with natural organic matter was previously observed by spectroscopy, there is no quantitative evidence of such reaction in batch experiments. In the present study, Pu(IV) interaction with humic acid (HA) was investigated at pH 1.8, 2.5 and 3, as a function of HA concentration and for Pu total concentration equal to 6 × 10−8 M. The finally measured Pu(IV) concentrations ([Pu(IV)]eq) are below Pu(IV) solubility limit. Pu(IV)–HA interaction can be explained by the complexation of Pu(IV) monomers by HA up to [Pu(IV)]eq ∼ 10−8 M. However, the slope of the log–log Pu(IV)–HA binding isotherm changes from ∼0.7 to ∼3.5 for hi…
Modeling plutonium sorption to kaolinite: Accounting for redox equilibria and the stability of surface species
Abstract Plutonium with its particularly complex redox chemistry may be thermodynamically stable in the states + III to + VI depending on the redox conditions in the environment. Mineral surfaces can also affect Pu redox speciation. Therefore, the interpretation of Pu sorption data becomes particularly challenging, even for simplified laboratory experiments. The present study focuses on Pu sorption to kaolinite. Am(III), Th(IV), Np(V) and U(VI) literature sorption data are used as analogues for the corresponding Pu redox states to calibrate a simple surface complexation model, and the Nernst formalism is applied. Two independent pH–pe diagrams, one for the kaolinite surface and another for …