Deep groundwater physicochemical components affecting actinide migration

Abstract

To better understand the migration behavior of actinides in deep groundwater (GW), the interactions between doped tracers and deep GW components were investigated. La, Sm, Ho, and U tracers (10 or 100 ppb) were doped into sedimentary rock GW samples collected from 250 to 350 m deep boreholes in the experimental gallery of the Horonobe Underground Research Laboratory (URL), Hokkaido, Japan. To evaluate the effect of GW composition on the chemical speciation of actinides, the same tracers were doped into crystalline rock GW samples collected from 300 to 500 m deep boreholes in the experimental gallery at the Mizunami URL, Gifu Prefecture, Japan. Each GW sample was sequentially filtered through a micro-pore filter (0.2 μm) and ultrafilters with a 10 kDa nominal molecular weight limit. Next, the filtrate solutions were analyzed using inductively coupled plasma–mass spectrometry to determine the concentration of tracers retained in solution during each filtration step, and the used filters were analyzed using time-of-flight secondary ion mass spectrometry element mapping and X-ray absorption fine structure spectroscopy to determine the chemical species of the tracers trapped on each filter. It was determined that lanthanide migration was controlled by the amount of phosphates in the Horonobe GW. Therefore, it was expected that the solubility of minor actinides (MAs), which exhibit a similar chemical behavior to that of lanthanides, would be controlled by the formation of phosphates in sedimentary rock GW. Moreover, the data on the Mizunami GW indicated that a fraction of lanthanides and MAs formed hydroxides and/or hydroxocarbonates.