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Reactor production of promethium-147

In this paper, we describe the 147 Pm production yields and level of impurities from several targets that consisted of milligram quantities of highly enriched 146 Nd oxide irradiated at the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory for durations ranging from 24 to180 h. A comparison between theoretical and experimental data are also presented, and attempts were made to empirically evaluate the neutron capture cross-sections of 41.3-d 148m Pm and 5.4-d 148g Pm. For a one-cycle irradiation (~24 days), 147 Pm yield reaches a maximum value of 101.8 MBq/mg (2.75 mCi/mg) at 60 days after the end of bombardment. Because of large neutron capture cross-sections of 147 Pm, the yield of 147 Pm does not significantly increase with longer irradiation. Our estimates of the thermal neutron capture cross-section and resonance integral for 146 Nd at 1.48 ± 0.05 b and 2.56 ± 0.25 b, respectively, were consistent with the reported values. The effective neutron capture cross-section of 147 Pm to 148m Pm was 53.3 ± 2.7 b - a factor of 2 lower than the 98.7 ± 6.5 b calculated from reported cross-sections. The measured σ eff to the ground state (5.37-d 148g Pm) was 82.0 ± 4.1 b; ~34 % lower than the value of 139 ± 0 b calculated from reported cross-sections. In this work, we also describe the development of a chemical process based on extraction and ion-exchange chromatography for separation of 147 Pm from milligram quantities of 146 Nd and other impurities. Sequential separation of Pm from the Nd target and from other radioisotopic impurities ( 153 Gd and 154&155 Eu, 192 Ir, and 60 Co) was achieved using a LN extraction resin in HCl media followed by further purification of Pm from 60 Co and 192 Ir using a low cross-linking cation exchange resin. Based on these data, we estimated that two rounds of purification under our experimental conditions can provide a mass separation factor of > 104 between Pm and Nd. Our data indicate that curie quantities of 147 Pm with suitable chemical and radioisotopic purity for applications in beta voltaic batteries can be produced by irradiating gram quantities of highly enriched 146 Nd in the flux trap of HFIR for one cycle.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Design considerations for three-dimensional betavoltaics

Betavoltaic devices are suitable for delivering low-power over periods of years. Typically, their power density is on the order of nano to micro-Watts per cubic centimeter. In this work we evaluate the potential for using high-aspect ratio three-dimensional semiconductor structures to enhance the power and efficiency of these devices. The Monte Carlo transport code MCNP6 is used to provide realistic estimates of the theoretical levels of charge generation, which is in turn used to make predictions about the power output from three-dimensional betavoltaics. The focus of this work is on silicon and promethium-147, but other semiconductors and radioisotopes are considered as well. In the case of silicon diodes with three-dimensional features that are comparable to what is commercially available we estimate that power densities in the range of 20-25 mW/cm 3 can be achieved at efficiencies of 2.9-5.8% when coupled with promethium-147 oxide.

25 ENERGY STORAGE↗

Extraction of Pm-147 from savannah river site nuclear material management programs

The Savannah River Site (SRS) processes used-nuclear fuel to recover uranium. There are many interesting fission products lost in the raffinate from this separation including 147 Pm. Here, the goal of this work was to recover 147 Pm from SRS waste solutions. A radiochemical separation method typically used for the determination of 147 Pm and 151 Sm was modified to purify significant quantities of 147 Pm from the H Canyon waste solutions. The developed scheme was tested on a small aliquot of waste solution from the processing of used fuel from the High Flux Isotope Reactor at Oak Ridge National Laboratory.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗