Radionuclide Solid:liquid partitioning in an aged, reducing-grout wasteform recovered from a disposal facility
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Kaplan, Daniel I. (ORCID:0000000210198386)↗
Engineering topics
Almond, Philip M.
Publications and source records attributed to Almond, Philip M..
Impact of natural organic matter on plutonium vadose zone migration from an NH4Pu(V)O2CO3(s) source
Large amounts of plutonium produced at the Savannah River Site (SRS) in the latter half of the last century led to the release of plutonium to the subsurface. Low-level waste containing plutonium has also been disposed of in the SRS vadose zone. The mobility and risk posed by these plutonium sources is not well understood, in part, because of unknown interactions of the various mobile plutonium species with natural organic matter (NOM). This study investigated the influence of NOM on the behavior of plutonium(V) in the vadose zone through a combination of field lysimeter and laboratory studies. Well-defined solid sources of NH4PuVO2CO3(s) placed in 5-L lysimeters containing vadose zone soils NOM-amended or unamended were exposed to natural SRS meteorological conditions for three years. These lysimeters were removed from the field and analyzed using wet chemistry methods and X-ray absorption spectroscopy (XAS). Plutonium desorption from soils recovered from the lysimeters and laboratory batch sorption experiments using Pu-free soils both indicated that surface mediated reduction of Pu(V) to Pu(IV) was influencing Pu sorption behavior. For both lysimeters (amended and unamended with NOM), Pu migrated slowly through the lysimeter core, with > 95% of the Pu remaining within 2 cm of the source. However, without the NOM amendments, Pu was transported significantly farther than in the presence of NOM. Thus, the presence of NOM appeared to decrease the mobility. Working hypotheses to explain this behavior are that 1) formation of ternary surface-NOM-Pu complexes enhanced Pu sorption affinity causing less mobility and/or 2) formation of these ternary surface-NOM-Pu complexes prevented reoxidaiton of Pu(IV) to more mobile Pu(V) in the pore water.
plutonium, organic matter↗
Dissolution of Low Enriched Uranium from Experimental Breeder Reactor-II Fuel
A dissolution flowsheet for the Low Enriched Uranium (LEU) ingots generated at the Idaho National Laboratory (INL) from the electrochemical processing of the EBR-II fuel was demonstrated at the laboratory scale. Dissolution experiments were performed using samples of the LEU and a carbon steel can and an integrated experiment was performed in which an Al 1100 alloy was dissolved as a surrogate for Spent Nuclear Fuel (SNF) followed by the dissolution of samples of the LEU and carbon steel can to demonstrate the complete flowsheet. The flowsheet allows the dissolution of a SNF batch in an H-Canyon dissolver using existing flowsheets followed by the dissolution of nominally 75 kg of LEU in the 6.4D dissolver or 45 kg of LEU in the 6.1D dissolver which were recovered from the Experimental Breeder Reactor-II (EBR-II) fuel. In the demonstration experiment, the rate of dissolution of the LEU metal was significantly slower than the dissolution rate of the Al 1100 alloy (4.7 versus 27 mg/min/cm 2 ) which projects to a longer cycle time for the LEU metal (compared to a SNF charge). Here, the H 2 generation rates from the dissolution of samples of the LEU metal and a carbon steel can were monitored by mass spectrometry and Raman spectroscopy and were shown to be inconsequential; therefore, the dissolution of the LEU ingots has no significant impact on the generation of H 2 .
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗