• Nuclear Engineering and Technology
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• v.50 no.6
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• pp.820-828
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• 2018

The growing nuclear threat has amplified the need for developing diverse and accurate nuclear forensics analysis techniques to strengthen nuclear security measures. The work presented here is part of a research effort focused on developing a methodology for reactor-type discrimination of weapons-grade plutonium. To verify the developed methodology, natural $UO_2$ fuel samples were irradiated in a thermal neutron spectrum at the University of Missouri Research Reactor (MURR) and produced approximately $20{\mu}g$ of weapons-grade plutonium test material. Radiation transport simulations of common thermal reactor types that can produce weapons-grade plutonium were performed, and the results are presented here. These simulations were needed to verify whether the plutonium produced in the natural $UO_2$ fuel samples during the experimental irradiation at MURR was a suitable representative to plutonium produced in common thermal reactor types. Also presented are comparisons of fission product and plutonium concentrations obtained from computational simulations of the experimental irradiation at MURR to the nondestructive and destructive measurements of the irradiated natural $UO_2$ fuel samples. Gamma spectroscopy measurements of radioactive fission products were mostly within 10%, mass spectroscopy measurements of the total plutonium mass were within 4%, and mass spectroscopy measurements of stable fission products were mostly within 5%.

• Nuclear Engineering and Technology
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• v.51 no.5
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• pp.1355-1364
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• 2019

A recently published nuclear forensics methodology for source discrimination of separated weapons-grade plutonium utilizes intra-element isotope ratios and a maximum likelihood formulation to identify the most likely source reactor-type, fuel burnup and time since irradiation of unknown material. Sensitivity studies performed here on the effects of random measurement error and the uncertainty in intra-element isotope ratio values show that different intra-element isotope ratios have disproportionate contributions to the determination of the reactor parameters. The methodology is robust to individual errors in measured intra-element isotope ratio values and even more so for uniform systematic errors due to competing effects on the predictions from the selected intra-element isotope ratios suite. For a unique sample-model pair, simulation uncertainties of up to 28% are acceptable without impeding successful source-reactor discrimination. However, for a generic sample with multiple plausible sources within the reactor library, uncertainties of 7% or less may be required. The results confirm the critical role of accurate reactor core physics, fuel burnup simulations and experimental measurements in the proposed methodology where increased simulation uncertainty is found to significantly affect the capability to discriminate between the reactors in the library.

• Nuclear Engineering and Technology
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• v.52 no.6
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• pp.1156-1163
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• 2020

Fuel temperature coefficient (FTC) of PuO₂+ZrO₂ (ROX) fueled LWR cell is analyzed neutronically with reactor- and weapons-grade plutonium fuels in comparison with a U-free PuO₂+ThO₂ (TOX), and a conventional MOX fuel cells. The FTC value of a ROX fueled LWR is smaller compared to a TOX or a MOX fueled LWRs and becomes extremely positive especially, at EOL. This is because when fuel temperature is increased, thermal neutron spectrum is shifted to harder, which is extreme at EOL in ROX fuel than that in TOX and MOX fuels. Consequently at EOL, ²³⁹Pu and ²⁴¹Pu contributes to positive fuel temperature reactivity (FTR) in ROX fuel, while they have negative contribution in TOX and MOX fuels. The FTC problem of ROX fuel is mitigated by additive ThO₂, UO₂ or Er₂O₃. In ROX-additive fuel, the atomic density of fissile Pu becomes more than additive free ROX fuel especially at EOL, which is the main cause to improve the FTC problem. The density of fissile Pu is more effective to decrease the thermal spectrum shifts with increase the fuel temperature than additive ThO₂, UO₂ or Er₂O₃ in ROX fuel.

• Analytical Science and Technology
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• v.17 no.6
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• pp.514-519
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• 2004

Soil samples collected from around the BOMARC Missile Site were measured for their activity concentrations and isotopic ratios of Pu and Am isotopes with particle sizes. The activity concentrations of Pu and Am in the BOMARC soil were remarkably higher than the fallout levels, and the activities decreased nearly exponentially with an increasing particle size of the soil due to a decreasing surface area. The activity ratios of Pu-238 / Pu-239, 240, Pu-241 / Pu-239, 240 and Am-241 / Pu-239, 240 observed in the BOMARC soil were much lower than those attributed to the nuclear reprocess plants and the Chernobyl fallout. Also, the atomic ratio of Pu-240 / Pu-239 in the BOMARC soil was remarkably lower than the fallout value influenced by the nuclear weapons testing and the Chernobyl accident. The atomic ratio of Pu-240 / Pu-239 was so close to the value of the weapons grade Pu released from the crash of a B52 plane in the Thule of the Greenland, such that the Pu isotopes detected in the BOMARC soil could have originated from the weapons grade plutonium.