RADIATION-INDUCED DECOMPOSITION OF U(VI) ALTERATION PHASES OF UO2

Utsunomiya, S. ; Ewing, R.C.

United States. Department of Energy. Office of Scientific and Technical Information.

关键词: Uraninites;    Saleeite;    Uranophane;    X-Ray Diffraction;    Irradiation;   

DOI  :  10.2172/860242
RP-ID  :  NA
RP-ID  :  NA
RP-ID  :  860242

美国|英语

来源: UNT Digital Library

【 摘 要 】

U{sup 6+}-phases are common alteration products of spent nuclear fuel under oxidizing conditions, and they may potentially incorporate actinides, such as long-lived {sup 239}Pu and {sup 237}Np, delaying their transport to the biosphere. In order to evaluate the ballistic effects of {alpha}-decay events on the stability of the U{sup 6+}-phases, we report, for the first time, the results of ion beam irradiations (1.0 MeV Kr{sup 2+}) for six different structures of U{sup 6+}-phases: uranophane, kasolite, boltwoodite, saleeite, carnotite, and liebigite. The target uranyl-minerals were characterized by powder X-ray diffraction and identification confirmed by SAED (selected area electron diffraction) in TEM (transmission electron microscopy). The TEM observation revealed no initial contamination of uraninite in these U{sup 6+} phases. All of the samples were irradiated with in situ TEM observation using 1.0 MeV Kr{sup 2+} in the IVEM (intermediate-voltage electron microscope) at the IVEM-Tandem Facility of Argonne National Laboratory. The ion flux was 6.3 x 10{sup 11} ions/cm{sup 2}/sec. The specimen temperatures during irradiation were 298 and 673 K, respectively. The Kr{sup 2+}-irradiation decomposed the U{sup 6+}-phases to nanocrystals of UO{sub 2} at doses as low as 0.006 dpa. The cumulative doses for the pure U{sup 6+}-phases, e.g., uranophane, at 0.1 and 1 million years (m.y.) are calculated to be 0.009 and 0.09 dpa using SRIM2003. However, with the incorporation of 1 wt.% {sup 239}Pu, the calculated doses reach 0.27 and {approx}1.00 dpa in ten thousand and one hundred thousand years, respectively. Under oxidizing conditions, multiple cycles of radiation-induced decomposition to UO{sub 2} followed by alteration to U{sup 6+}-phases should be further investigated to determine the fate of trace elements that may have been incorporated in the U{sup 6+}-phases.