Graduate Thesis Or Dissertation

 

Dissolution of uranium dioxide microspheres in carbonate and hydrogen peroxide solutions Public Deposited

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  • Uranium dioxide has been used in industry both as a fuel for power reactors and as a target for the production of radioisotopes. One of the most important radioisotopes produced using these targets is molybdenum-99 (Mo-99, 65.94hr half-life), which is the parent isotope to technetium-99m (Tc-99m, 6.01hr half-life), a radioisotope used in 70% of diagnostic medical isotope procedures performed in the United States of America. [1] [2] Molybdenum-99, produced by either the thermal neutron fission of uranium-235 in nuclear reactors or by neutron activation of molybdenum-98, is purified, packaged, and shipped to hospitals worldwide. The maximal activity of Tc-99m is reached in 22.9hrs, so it can be milked from the parent Mo-99 repeatedly. Mo-99 is one of many fission products generated during the thermal neutron fission of uranium-235. For production of Mo-99, irradiation targets based on metallic uranium, uranium alloys, or uranium dioxide are produced. After neutron irradiation in a reactor, the uranium target must first be dissolved in a suitable medium. This has traditionally been done using boiling nitric acid solutions. In literature and in industry, the use of alkaline solutions, specifically carbonate salt solutions combined with hydrogen peroxide, are being explored as an alternative to the nitric acid based dissolution process. The carbonate-peroxide dissolution scheme has several advantages over traditional nitric acid dissolutions including less damage to equipment during operation and smaller volumes of waste produced during process. This thesis research work explores the initial dissolution rates of uranium dioxide in carbonate medium containing hydrogen peroxide. Effect of three different counter cations- ammonium, sodium, and potassium - on the dissolution behavior of uranium was investigated. The kinetic factors of dissolution, activation energy, frequency factor, and reaction order with respect to both the carbonate salt and hydrogen peroxide were found for each of these systems. Information in this thesis is organized into six chapters and list of cited literature sources.
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