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Nuclear Data Sheets for A = 235

Spectroscopic data and level schemes from radioactive decay and nuclear reaction studies are presented here for all nuclei with mass number A=235. The highlight of this evaluation consists of the precise and comprehensive Coulomb excitation study (2012Wa35) on {sup 235}U, which in addition to the 7/2[743] ground state rotational band, extended the 1/2[631], 5/2[622], 5/2[752], and 3/2[631] rotational bands up to Jπ=53/2+, 49/2+, 441/2−, and 43/2+, respectively. This evaluation presents a study (2010Hu02) of the {sup 237}Np({sup 116}Sn, {sup 118}Snγ) reaction where the ground state rotational band 5/2[642] was observed up to Jπ=(53/2+). It is worth for historical knowledge to mention the report on the “Discovery of isotopes of the transuranium elements with 93≤Z≤98” (2013Fr02), where the information for elements Np, Pu, and Am with mass number A=235 is given. {sup 235}Cf has not been observed. The alpha hindrance factors (HF) presented in this evaluation were calculated using values of the radius parameter (r{sub 0}) interpolated from those for even–even adjacent nuclei given by 1998Ak04.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Impact of Reprocessed Uranium Management on the Homogeneous Recycling of Transuranics in PWRs

This article presents the results of a neutronics analysis related to the homogeneous recycling of transuranics (TRU) in PWRs with a MOX fuel using enriched uranium instead of depleted uranium. It also addresses an often, if not always, overlooked aspect related to the recycling of TRU in PWRs, namely the use of reprocessed uranium. From a neutronics point of view, it is possible to multi-recycle the entirety of the plutonium with or without neptunium and americium in a PWR fleet using MOX-EU fuel in between one third and two thirds of the fleet. Recycling neptunium and americium with plutonium significantly decreases the decay heat of the waste stream between 100 to 1,000 years compared to those of an open fuel cycle or when only plutonium is recycled. The uranium present in MOX-EU used fuel still contains a significant amount of 235 uranium and recycling it makes a major difference on the natural uranium needs. For example, a PWR fleet recycling its plutonium, neptunium and americium in MOXEU needs 28 percent more natural uranium than a reference UO 2 open cycle fleet generating the same energy if the reprocessed uranium is not recycled and 19 percent less if the reprocessed uranium is recycled back in the reactors, i.e. a 47 percent difference.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

A multi-collector ICP-MS method for quantification of plutonium, uranium, and americium in hair and nails of occupationally or medically exposed individuals

The 239 Pu, 238 U, and 241 Am concentrations and 239 Pu/ 240 Pu, 235 U/ 238 U, and 236 U/ 238 U atom ratios were measured in the hair and nail samples from individuals who donated their bodies to the United States Transuranium and Uranium Registries. Further, the concentration of 239 Pu ranged from 0.22–15.8 ng/kg. The 240 Pu/ 239 Pu isotopic ratios ranged from 0.026 to 0.127 which is consistent with weapons-grade plutonium. Concentration of uranium fell between 1.84 µg/kg and 29.5 µg/kg and 235 U/ 238 U ratios ranged from 4.8×10 -3 to 7.6×10 -3 . Elevated 236 U/ 238 U atom ratios were measured in two cases and ranged from 5.0×10 -6 – 2.4×10 -5 indicating exposure to spent or reprocessed uranium material. The concentration of 241 Am was measured in four hair samples and ranged from 0.02–0.21 ng/kg.

61 RADIATION PROTECTION AND DOSIMETRY↗

An event-triggered coincidence algorithm for fast-neutron multiplicity assay corrected for cross-talk and photon breakthrough

Here, a model quantifying detector cross-talk and the misidentification of events in fast neutron coincidence distributions is described. This is demonstrated for two experimental arrangements comprising rings of 8 and 15 organic liquid scintillation detectors. Correction terms developed as part of this model are tested with 252 Cf and a relationship is developed between the 235 U enrichment of U 3 O 8 and the order of correlated, fast neutron multiplets induced by an americium–lithium source. The model is also supported by Geant4 simulations. The results suggest that a typical assay, for experimental arrangements that are similar to the examples investigated in this research, will exhibit cross-talk for less than 1% of all detected fast neutrons but, if not accounted for, this can bias the numerical analysis by a margin of 10% and 35% in second- and third-order coincidences (i.e. couplet and triplet counts), respectively. Further, for the case of 252 Cf, it is shown that a relatively low proportion of 4% breakthrough by rays (that is, photons misidentified as neutrons by the pulse-shape discrimination process) can lead to an erroneous increase of 20% in total neutron counts in the assay of a mixed-field, in this case of 252 Cf. These findings will help direct the developments needed to enable organic scintillation detectors with pulse shape discriminators to be applied reliably to nuclear safeguards and non-proliferation verification tasks.

42 ENGINEERING↗

Technical basis for the use of a correlated neutron source in the uranium neutron coincidence collar

Active neutron coincidence systems are commonly used by international inspectorates to verify a material balance across the various stages of the nuclear fuel cycle. The Uranium Neutron Coincidence Collar (UNCL) is one such instrument; it is used to measure the linear density of 235 U (g 235 U/cm of active length in assembly) in fresh light water reactor fuel in nuclear fuel fabrication facilities. The UNCL and other active neutron interrogation detectors have historically relied on americium lithium ( 241 AmLi) sources to induce fission within the sample in question. Californium-252 is under consideration as a possible alternative to the traditional 241 AmLi source. Finally, this work relied upon a combination of experiments and Monte Carlo simulations to demonstrate the technical basis for the replacement of 241 AmLi sources with 252 Cf sources by evaluating the statistical uncertainty in the measurements incurred by each source and assessing the penetrability of neutrons from each source for the UNCL.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Characterization of Delayed-Particle Emission Signatures for Pyroprocessing. Part 1: ABTR Fuel Assembly

A three-part study is conducted using the MCNP6 Monte Carlo radiation-transport code to calculate delayed-neutron (DN) and delayed-gamma (DG) emission signatures for nondestructive assay (NDA) metal-fuel pyroprocessing. In Part 1, MCNP6 is used to produce irradiation-induced used nuclear fuel (UNF) isotopic inventories for an Argonne National Laboratory (ANL) Advanced Burner Test Reactor (ABTR) preconceptual design fuel assembly (FA) model. The initial fuel inventory consists of uranium mixed with light-water-reactor transuranic (TRU) waste and 10 wt% zirconium (U-LWR-SFTRU-10%Zr). To facilitate understanding, parametric evaluation is done using models for 3% and 5% initial 235 U a% enrichments, burnups of 5, 10, 15, 20, 30, …, 120 GWd/MTIHM, and 3-, 5-, 10-, 20-, and 30- year cooling times. Detailed delayed-particle radioisotope source terms for the irradiate FA are created using BAMF-DRT and SOURCES3A. Using simulation tallies, DG activity ratios (DGARs) are developed for 134 Cs/ 137 Cs 134 Cs/ 154 Eu, and 154 Eu/ 137 Cs markers as a function of (1) burnup and (2) actinide mass, including elemental uranium, neptunium, plutonium, americium, and curium. Spectral-integrated DN emission is also tallied. The study reveals a rich assortment of DGAR behavior as a function of DGAR type, enrichment, burnup, and cooling time. Similarly, DN emission plots show variation as a function of burnup and of actinide mass. Sensitivity of DGAR and DN signatures to initial 235 U enrichment, burnup, and cooling time is evident. Comparisons of the ABTR radiation signatures and radiation signatures previously reported for a generic Westinghouse oxide-fuel assembly indicate that there are pronounced differences in the ABTR and Westinghouse oxide-fuel DN and DG signatures. These differences are largely attributable to the initial TRU inventory in the ABTR fuel. The actinide and nonactinide inventories for the FA models serve as source materials for the pre- and postelectrorefining models to be reported in Parts 2 and 3.

07 ISOTOPE AND RADIATION SOURCES↗

Minimum critical masses and their uncertainties for several fissile nuclides and reflectors - 14296

A systematic effort was undertaken to reevaluate the minimum critical mass for several fissile nuclides and reflectors. This was done using MCNP6 in combination with several modern nuclear data libraries, viz. ENDF/B-VII.1, JENDL-4.0 and JEFF-3.1.1. This combination was benchmarked extensively against criticality safety benchmarks. The procedure to extract the minimum critical mass from the MCNP6 calculations was carefully implemented, so that it would have a negligible impact on the accuracy of the end results. All parts of the calculation, i.e. nuclear data processing, MCNP6 models, and post-processing, were applied consistently for all cases, involving varying fissile nuclides and reflectors. Results for the minimum critical mass were generated for {sup 233,235}U, {sup 236,239,241}Pu, {sup 242m}Am, {sup 243,245,247}Cm, and {sup 249,251}Cf, for the case of water moderation and water reflection. For {sup 235}U, the minimum critical mass was also calculated for cases with other reflectors, such as beryllium, heavy water, graphite, lead, and concrete. The results for the water reflection cases are in good agreement with most of the literature values, but for the cases with reflectors such as graphite, lead, or concrete, there are sizable differences. The accuracy of the results was assessed in two ways. First, a comparison was made with criticality safety benchmark results, by selecting benchmarks that resemble the minimum mass systems the most. It was clear that for {sup 233,235}U and {sup 239}Pu with water reflection, the differences in minimum critical masses between the libraries are consistent with the differences obtained for benchmark cases. The difference between the benchmark calculations and the benchmark values is then an indication of the accuracy with which one can simulate comparable systems. Secondly, sensitivity runs were performed with the new MCNP6 sensitivity option, based on ENDF/B-VII.1 nuclear data. For each fissile nuclide, the sensitivity of k{sub eff} to cross sections such as capture, fission, elastic, inelastic was calculated for the minimum critical mass case. The same was done for the {sup 1}H and {sup 16}O cross sections in the moderator and reflector. The uncertainty in k{sub eff} was calculated by combining the sensitivity profiles with the appropriate ENDF/B-VII.1 covariance matrix, using the SUSD code. As a final step, the uncertainty in k{sub eff} can be translated to an uncertainty in the minimum critical mass. (author)

42 ENGINEERING↗

Simulations of a PSD Plastic Neutron Collar for Assaying Fresh Fuel

The potential performance of a notional active coincidence collar for assaying uranium fuel based on segmented detectors constructed from the new PSD plastic fast organic scintillator with pulse shape discrimination capability was investigated in simulation. Like the International Atomic Energy Agency's present Uranium Neutron Collar for LEU (UNCL), the PSD plastic collar would also function by stimulating fission in the 235 U content of the fuel with a moderated 241 Am/Li neutron source and detecting instances of induced fission via neutron coincidence counting. In contrast to the moderated detectors of the UNCL, the fast time scale of detection in the scintillator eliminates statistical errors due to accidental coincidences that limit the performance of the UNCL. However, the potential to detect a single neutron multiple times historically has been one of the properties of organic scintillator detectors that has prevented their adoption for international safeguards applications. Consequently, as part of the analysis of simulated data, a method was developed by which true neutron-neutron coincidences can be distinguished from inter-detector scatter that takes advantage of the position and timing resolution of segmented detectors. Then, the performance of the notional simulated coincidence collar was evaluated for assaying a variety of fresh fuels, including some containing burnable poisons and partial defects. In these simulations, particular attention was paid to the analysis of fast mode measurements. In fast mode, a Cd liner is placed inside the collar to shield the fuel from the interrogating source and detector moderators, thereby eliminating the thermal neutron flux that is most sensitive to the presence of burnable poisons that are ubiquitous in modern nuclear fuels. The simulations indicate that the predicted precision of fast mode measurements is similar to what can be achieved by the present UNCL in thermal mode. For example, the statistical accuracy of a ten-minute measurement of fission coincidences collected in fast mode will be approximately 1% for most fuels of interest, yielding a ~1.4% error after subtraction of a five minute measurement of the spontaneous fissions from 238 U in the fuel, a ~2% error in analyzed linear density after accounting for the slope of the calibration curve, and a ~2.9% total error after addition of an assumed systematic error of 2%.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The prospect of uranium nitride (UN) and mixed nitride fuel (UN-PuN) for pressurized water reactor

Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the addition of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Radionuclide inventories for the F- and H-area seepage basin groundwater plumes

Within the General Separations Areas (GSA) at the Savannah River Site (SRS), significant inventories of radionuclides exist within two major groundwater contamination plumes that are emanating from the F- and H-Area seepage basins. These radionuclides are moving slowly with groundwater migration, albeit more slowly due to interaction with the soil and aquifer matrix material. The purpose of this investigation is to quantify the activity of radionuclides associated with the pore water component of the groundwater plumes. The scope of this effort included evaluation of all groundwater sample analyses obtained from the wells that have been established by the Environmental Compliance & Area Completion Projects (EC&ACP) Department at SRS to monitor groundwater contamination emanating from the F- and H-Area Seepage Basins. Using this data, generalized groundwater plume maps for the radionuclides that occur in elevated concentrations (Am-241, Cm-243/244, Cs-137, I-129, Ni-63, Ra-226/228, Sr-90, Tc-99, U-233/234, U-235 and U-238) were generated and utilized to calculate both the volume of contaminated groundwater and the representative concentration of each radionuclide associated with different plume concentration zones.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗