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Alpha-recoil effect on the dissolution of betafite: rapid natural annealing of radiation damage within a metamict phase

Conference · · Mater. Res. Soc. Symp. Proc.; (United States)
OSTI ID:5474307

Betafite, a radioactive mineral, is the Ti-rich member of the pyrochlore group, A/sub 1-2/B/sub 2/X/sub 6/Y/sub 0-1/, (Fd3m, Z = 8), where A = Ca, Na, U, Th, REE (rare earth elements, Y, Ba, Sr, Bi, Pb; B = Nb, Ti, Ta, Zr, Sn, Fe: X = oxygen; Y = 0, OH and F. The pyrochlore structure (or structural derivatives, e.g. zirconolite in SYNROC) is a common constituent of polyphase, crystalline radioactive waste forms. Naturally occurring minerals with this structure often occur in the metamict state. Therefore, a principal concern is the effect of alpha-recoil damage on the structure and dissolution behavior of synthetic, analogue, waste-form phases which contain actinides. The authors describe the dissolution behavior of /sup 238/U, /sup 234/U, /sup 232/Th, /sup 230/Th and /sup 228/Th in betafite during leaching in a bicarbonate-carbonate solution. Results indicate enhanced leaching of recently produced alpha-recoil damage as evidenced by the more rapid dissolution rate of /sup 228/Th relative to /sup 232/Th and /sup 230/Th, and only slightly enhanced leaching of older damage as evidenced by a small increase in the dissolution rate of /sup 234/U relative to /sup 238/U. These experiments demonstrate that individual alpha-recoil tracks are preserved for some time as disordered regions of higher chemical reactivity in already fully-damaged, aperiodic structures. The authors estimate an annealing time for the alpha-recoil tracks of 2000 +/- 1300 yr in the metastable, aperiodic structure. Similar alpha-recoil tracks should be formed and annealed in other aperiodic nuclear waste forms, such as borosilicate glass.

Research Organization:
Israel Institute of Technology, Haifa
DOE Contract Number:
FG04-84ER45099
OSTI ID:
5474307
Report Number(s):
CONF-850995-
Journal Information:
Mater. Res. Soc. Symp. Proc.; (United States), Journal Name: Mater. Res. Soc. Symp. Proc.; (United States) Vol. 50; ISSN MRSPD
Country of Publication:
United States
Language:
English