Water Sorption and Gamma Radiolysis Studies for Uranium Oxides [electronic resource].

Published:: Washington, D.C. : United States. Dept. of Energy, 2002.
Oak Ridge, Tenn. : Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy
Physical Description:: 86 pages : digital, PDF file
Additional Creators:: Oak Ridge National Laboratory, United States. Department of Energy, and United States. Department of Energy. Office of Scientific and Technical Information

Access Online

www.osti.gov

Availability

Finding items...

Restrictions on Access:

Free-to-read Unrestricted online access

Summary:

During the development of a standard for the safe, long-term storage of 233U-containing materials, several areas were identified that needed additional experimental studies. These studies were related to the perceived potential for the radiolytic generation of large pressures or explosive concentrations of gases in storage containers. This report documents the results of studies on the sorption of water by various uranium oxides and on the gamma radiolysis of uranium oxides containing various amounts of sorbed moisture. In all of the experiments, 238U was used as a surrogate for the 233U. For the water sorption experiments, uranium oxide samples were prepared and exposed to known levels of humidity to establish the water uptake rate. Subsequently, the amount of water removed was studied by heating samples in a oven at fixed temperatures and by thermogravimetric analysis (TGA)/differential thermal analysis (DTA). It was demonstrated that heating at 650 C adequately removes all moisture from the samples. Uranium-238 oxides were irradiated in a 6°Co source and in the high-gamma-radiation fields provided by spent nuclear fuel elements of the High Flux Isotope Reactor. For hydrated samples of UO3, H2 was the primary gas produced; but the total gas pressure increase reached steady value of about 10 psi. This production appears to be a function of the dose and the amount of water present. Oxygen in the hydrated UO3 sample atmosphere was typically depleted, and no significant pressure rise was observed. Heat treatment of the UO3 · xH2O at 650 C would result in conversion to U3O8 and eliminate the H2 production. For all of the U3O8 samples loaded in air and irradiated with gamma radiation, a pressure decrease was seen and little, if any, H2 was produced--even for samples with up to 9 wt % moisture content. Hence, these results demonstrated that the efforts to remove trace moisture from U3O8 are not necessary to avoid pressurization of stored uranium oxides caused by gamma-induced radiolysis. In fact, this system can tolerate several percent of sorbed moisture--most of which can be easily removed by heating to only 150 C. To complete the picture of the radiolytic response of uranium oxides that have sorbed moisture, alpha radiolysis experiments have been initiated.

Report Numbers:

E 1.99:ornl/tm-2001/59
ornl/tm-2001/59

Subject(s):

Note:

Published through SciTech Connect.
02/27/2002.
"ornl/tm-2001/59"
Icenhour, A.S.

Type of Report and Period Covered Note:

Topical;

Funding Information:

AC05-00OR22725

View MARC record | catkey: 23781459