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Observed changes in the mechanism and rates of Pu(V) reduction on hematite as a function of total plutonium concentration.

Changes in aqueous- and solid-phase plutonium oxidation states were monitored as a function of time and plutonium concentration in hematite (α-Fe2O3) suspensions containing initially Pu(V). Batch kinetic experiments were conducted at plutonium concentrations between 10(-8) and 10(-6) M at pH 5 and 0.3 g/L (9.3 m(2)/L) hematite. Surface-mediated reduction of Pu(V) was observed under all conditions studied. However, differences in the reaction kinetics demonstrate that the mechanism of Pu(V) reduction changes as a function of plutonium concentration. Adsorption of Pu(V) was found to be the rate-limiting step at plutonium concentrations less than approximately 10(-7) M Pu(V). Plutonium reduction in these systems was attributed to trace amounts of Fe(II) in the hematite structure. Reduction of Pu(V) was found to be the rate-limiting step at concentrations higher than approximately 10(-6) M Pu(V) and is attributed to the formation of PuO(2+x)·nH2O nanoparticles and the Nernstian favorability of Pu(IV) surface complexes. The reaction order with respect to plutonium concentration was found to be -0.68 ± 0.09, indicating that there is a concentration dependence in these systems. This work strongly suggests that the kinetics of experiments carried out under high plutonium concentrations (i.e., >10(-7) M Pu) cannot be directly extrapolated to environmental concentrations of plutonium.