NEUTRONIC EFFECTS ON TUNGSTEN-186 DOUBLE NEUTRON CAPTURE
Al-Sheikhly, Mohamad I
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Rhenium-188, a daughter product of tungsten-188, is an isotope of great interest in therapeutic nuclear medicine, being used in dozens of laboratory and clinical investigations worldwide. Applications include various cancer therapy strategies, treatment of rheumatoid arthritis, prevention of restenosis following coronary artery angioplasty, and palliation of bone pain associated with cancer metastases. With its half-life of 17 hours, 2.12 MeV (maximum) beta-particle emission, chemical similarity to technetium-99m (the most widely used diagnostic radioisotope), and its availability in a convenient tungsten-188/rhenium-188 generator system, rhenium-188 is a superb candidate for a broad range of applications. Production of 188W is typically via double neutron capture by 186W in a high flux nuclear reactor, predominantly the High Flux Isotope Reactor at the Oak Ridge National Laboratory in Tennessee. Experience at HFIR has shown that production yields (measured in Ci of 188W produced per g of 186W target) decrease considerably as target size increases. While the phenomenon of neutron resonance self-shielding would be expected to produce such an effect, temperature effects on neutron flux distribution and neutron capture rates may also be involved. Experimental investigations of these phenomena have not been previously performed. The work presented in this thesis evaluates the factors that contribute to the decrease in 188W yield from both theoretical and experimental standpoints. Neutron self-shielding and temperature effects were characterized to develop a strategy for target design that would optimize production yield, an important factor in minimizing health care costs. It was determined that decrease in yield due to neutron self-shielding can be attributed to depletion of epithermal neutrons at resonant energies, most significantly within the initial 0.4 mm depth of the target. The results from these studies further show that 188W yield in the interior of the target (beyond 0.4 mm depth) does not decrease as would be expected due to neutron attenuation. This observation was explained by the fact elevated temperatures in the interior of the target result in an increase in the 188W yield through Doppler broadening of cross sections, compensating for reduced yield due to neutron attenuation. Finally, this work supports earlier analyses that questioned the accuracy of the 187W thermal cross section and resonance integral.