Plutonium-238 alpha-decay damage study of the ceramic waste form.

An accelerated alpha-decay damage study of a glass-bonded sodalite ceramic waste form has recently been completed. The purpose of this study was to investigate the physical and chemical durability of the waste form after significant exposure to alpha decay. This accelerated alpha-decay study was performed by doping the ceramic waste form with {sup 238}Pu which has a much greater specific activity than {sup 239}Pu that is normally present in the waste form. The alpha-decay dose at the end of the four year study was approximately 1 x 10{sup 18} alpha-decays/gram of material. An equivalent time period for a similar dose of {sup 239}Pu would require approximately 1100 years. After four years of exposure to {sup 238}Pu alpha decay, the investigation observed little change to the physical or chemical durability of the ceramic waste form (CWF). Specifically, the {sup 238}Pu-loaded CWF maintained it's physical integrity, namely that the density remained constant and no cracking or phase de-bonding was observed. The materials chemical durability and phase stability also did not change significantly over the duration of the study. The only significant measured change was an increase of the unit-cell lattice parameters of the plutonium oxide and sodalite phases of the material and an increase in the release of salt components and plutonium of the waste form during leaching tests, but, as mentioned, these did not lead to any overall loss of waste form durability. The principal findings from this study are: (1) {sup 238}Pu-loaded CWF is similar in microstructure and phase composition to referenced waste form. (2) Pu was observed primarily as oxide comprised of aggregates of nano crystals with aggregates ranging in size from submicron to twenty microns in diameter. (3) Pu phases were primarily found in the intergranular glassy regions. (4) PuO phase shows expected unit cell volume expansion due to alpha decay damage of approximately 0.7%, and the sodalite phase unit cell volume has expanded slightly by 0.3% again, presumably due to alpha-decay damage. (5) No bulk sample swelling was observed. (6) No amorphization of sodalite or actinide bearing phases was observed after four years of alpha-decay damage. (7) No microcracks or phase de-bonding were observed in waste form samples aged for four years. (8) In some areas of the {sup 238}Pu doped ceramic waste form material bubbles and voids were found. Bubbles and voids with similar size and density were also found in ceramic waste form samples without actinide. These bubbles and voids are interpreted as pre-existing defects. However, some contribution to these bubbles and voids from helium gas can not be ruled out. (9) Chemical durability of {sup 238}Pu CWF has not changed significantly after four years of alpha-decay exposure except for an increase in the release of salt components and Pu. Still, the plutonium release from CWF is very low at less than 0.005 g/m{sup 2}