An investigation of the characteristics of humic acid and of its effects on the chemistry of the near field of a radioactive waste repository

The work described in this report attempts to assess the possible effects of humic substances in the near field of a radioactive waste repository. Two samples of humic acid were studied by analytical ultracentrifugation. It was found to be an advantage to reduce sample polydispersity before carrying out molecular weight determinations. Ultrafiltration experiments showed that calcium concentrations of greater than 10-3M were sufficient to cause precipitation of humic acid. Boom clay extracts in sodium hydroxide solution were able to maintain high concentrations of americium in the aqueous phase. Extracts of Boom clay in cement-equilibrated water showed less ability to increase americium concentrations. The sorption of americium on BFS/OPC was studied. Distribution ratios of 600 ml g-1 in the absence of humic acid and 500 ml g-1 in its presence were obtained. Size distribution studies on americium showed that humic acid had little effect on the concentration of the radioelement in solutions passed through filters with up to 2 μm pore size. However, size distribution studies on plutonium revealed that more plutonium was associated with each filtered fraction in the experiments which contained Boom clay extract than in those which used cement-equilibrated water. Measurements of the sorption of neptunium on cements showed that this radioelement was strongly sorbed onto both 9:1 BFS/OPC and the Nirex reference backfill. The presence of humic acid extracted from Boom clay did not cause any discernible decrease in the sorption of this radioelement on cement. Thermodynamic calculations, using a simple model, illustrate the important role which calcium could play in controlling the concentrations of actinide humates in the near-field porewater. 31 refs., 19 figs., 12 tabs