The carbonate complexation of plutonium(IV)

Plutonium(IV) carbonate complexes are expected to be of particular importance in typical groundwaters at the Yucca Mountain site of the candidate nuclear waste repository being studied by the Nevada Nuclear Waste Storage Investigations Project. The chemistry of these complexes is also important in the areas of nuclear fuel reprocessing and purification, actinide separations, and environmental studies. This report describes initial experiments performed to determine the identity and equilibrium quotients of plutonium(IV) carbonate complexes. These experiments were performed at pH values between 7.2 and 9.6 using a spectrophotometric method. In addition, a brief review of the published literature on Pu(IV) carbonate complexes is presented. Since Pu(IV) exhibits low solubility in the near-neutral pH range, a complex-competition reaction where citrate ligands compete with carbonate ions for the plutonium will be employed. This will permit us to study the pure carbonate system; study the mixed carbonate/citrate system, and confirm and extend the literature work on the pure citrate system. The current experiments have demonstrated the existence of at least three distinct species in the pH region studied. This work will continue in the extended study of the pure citrate system, followed by the investigation of the citrate/carbonate complex/competition reaction. 9 refs., 4 figs.,more » 2 tabs.« less