The Influence of Glass Leachate on the Hydraulic, Physical, Mineralogical and Sorptive Properties of Hanford Sediment

Kaplan, Daniel I. ; Serne, R. Jeffrey ; Schaef, Herbert T. ; Lindenmeier, Clark W. ; Parker, Kent E. ; Owen, Antionette T. ; McCready, David E. ; Young, James S.

Pacific Northwest National Laboratory (U.S.)

关键词: Hydraulics;    Ilaw Pa;    Kaolinite;    Hydrologic Changes;    Sorptive Properties Ilaw Pa;   

DOI  :  10.2172/15010298
RP-ID  :  PNNL-14325
RP-ID  :  AC05-76RL01830
RP-ID  :  15010298

美国|英语

来源: UNT Digital Library

【 摘 要 】

The Immobilized Low Activity Waste (ILAW) generated from the Hanford Site will be disposed of in a vitrified form. It is expected that leachate from the vitrified waste will have a high pH and high ionic strength. The objective of this study was to determine the influence of glass leachate on the hydraulic, physical, mineralogical, and sorptive properties of Hanford sediments. Our approach was to put solutions of NaOH, a simplified surrogate for glass leachate, in contact with quartz sand, a simplified surrogate for the Hanford subsurface sediment, and Warden soil, an actual Hanford sediment. Following contact with three different concentrations of sodium hydroxide solutions, changes in hydraulic conductivity, porosity, moisture retention, mineralogy, aqueous chemistry, and soil-radionuclide distribution coefficients were determined. Under chemical conditions approaching the most caustic glass leachate conditions predicted in the near-field of the ILAW disposal site, approximated by 0.3 M NaOH, significant changes in mineralogy were observed. The clay minerals of the Hanford sediment evidenced the greatest dissolution thereby increasing the relative proportions of the more resistant minerals, e.g., quartz, feldspar, and calcite, in the remaining mass. Some re-precipitation of solids (mostly amorphous gels) was observed after caustic contact with both solids; these precipitates increased the moisture retention in both sediments, likely because of water retained within the gel coatings. The hydraulic conductivities were slightly lower but, because of experimental artifacts, these reductions should not be considered significant. Thus, there does not seem to be large differences in the hydraulic properties of the quartz sand or Warden silt loam soil after 192 days of contact with caustic fluids similar to glass leachate. The long term projected impact of the increased moisture retention has not been evaluated but likely will not make past simplified performance projections invalid. Despite the fact that some clay minerals, smectites and kaolinite, almost totally dissolved within a year of contact with 3.0 M NaOH (and by inference after longer time frames for 0.3 M NaOH, a more realistic surrogate for ILAW glass leachate) other sorbing minerals such as illite and chlorite do not appreciably react. The net result on sorption of common and risk relevant mobile radionuclides is not expected to be significant. Specifically, little change in Cs-Kd values and a significant increase in Sr-Kd values were measured in the simulated glass leachates versus natural groundwater. The difference in the sorptive responses of the radionuclides was attributed to differences in sorption mechanisms (Cs sorbs strongly to high-energy sites, whereas Sr sorbs primarily by cation exchange but also is sensitive to pH mediated precipitation reactions). Caustic treated sediments contacted with NaOH solutions radiotraced with Sr exhibited high Kd’s likely because of precipitation with CaCO3. In caustic solutions there was no appreciable adsorption for the three anions I-, SeO42-, or TcO4-. In the “far field” vadose zone in past performance projections, some sorption has been allowed for selenate. Even if the caustic glass leachate completely dominates the entire vadose zone below the repository, such that there will be no sorption of selenate, the dilution and pH neutralization that will occur in the upper unconfined aquifer will allow selenate adsorption to occur onto the aquifer sediments. It is recommended that a future performance assessment sensitivity run be performed to address this point.