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Nuclear Data Sheets for A = 139

The experimental nuclear spectroscopic data for known nuclides of mass number 139 (Sn, Sb, Te, I, Xe, Cs, Ba, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy) have been evaluated and presented together with adopted properties for levels and gamma rays. This evaluation represents a revision of previous one (2001Bu16) by T.W. Burrows. Since then extensive new data have become available for many A=139 nuclides although, no excited state data are yet available for {sup 139}Sn, {sup 139}Sb, {sup 139}Tb, and {sup 139}Dy. The decay schemes of {sup 139}Sn, {sup 139}Sb, {sup 139}I, {sup 139}Tb and {sup 139}Dy nuclei are not known, and those for {sup 139}Gd and {sup 139}Eu are poorly known. Particle-transfer data are available for {sup 139}Ba, {sup 139}La, {sup 139}Ce and {sup 139}Pr. Limited high-spin data are available for {sup 139}Te, {sup 139}I, {sup 139}Cs, {sup 139}Ba, {sup 139}La and {sup 139}Ce, while such data are extensive for {sup 139}Pr, {sup 139}Nd, {sup 139}Pm, {sup 139}Sm, {sup 139}Eu and {sup 139}Gd. Recent {sup 139}Pm high-spin data from two independent studies using the same reaction and similar beam energy are in conflict and could be improved using state-of-the-art large gamma-detector arrays in contrast to the smaller arrays currently used. Cases for which no new experimental information are available since the last update have undergone checking resulting in some changes in the current work, but for the most part these are taken from the previous evaluations. Thus, the present work has greatly benefited from all prior NDS evaluations (2001Bu16, 1989Bu12, 1981Pe04, 1974Gr46), but at the same time data presented herein supersede those in the earlier evaluations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Am(VI) Extraction Final Report: FY16

This report summarizes activities related to hexavalent Am extraction for FY16, in completion of FCR&D Milestone M3FT-16IN030103027. Activities concentrated on three areas of research: 1) centrifugal contactor hot testing, 2) Am(VI) stability studies, and 3) alternative oxidant studies. A brief summary of each task follows. Hot Testing: A new engineering-scale oxidation and solvent extraction test bed was built at Idaho National Laboratory to allow for solvent extraction testing of minor actinide separation concepts. The test bed consists of an oxidation vessel, filtration apparatus, four, 3D printed, 2-cm diameter centrifugal contactors, feed/product vessels, and sample ports. This system replaced the previous 3 stage, 5-cm contactor test bed that was used for the initial testing in FY14. In the FY16 hot test, a feed simulant was spiked with 243Am and 139Ce and treated with 60 g/L sodium bismuthate for two hours to oxidize the Am(III) to Am(VI). This solution was then pumped through a filter and into the four-stage centrifugal contactor setup. The organic phase solvent formulation was 1 M diethylhexylbutyramide (DEHBA)/dodecane. The test showed that Am(VI) was produced by bismuthate oxidation and the residual oxidant was successfully filtered without back pressure buildup. Sixty-four percent of Am was extracted in the contactors using DEHBA. Both Am and Ce were quantitatively stripped by 0.1 M H2O2. Successful demonstration of the utility of small, printable contactors suggests that hot testing of separations concepts can now be conducted more often, since it is cheaper, generates less waste, and entails much less radcon risk than previous testing. Am(VI) stability: A rigorous examination of reagents was conducted to determine if contaminants could interfere with Am oxidation and extraction. An series of DAm measurements showed that bismuthate particle size, water source, acid quality, and DAAP batch or pre-treatment had little effect on extraction efficiency, with a mean distribution ratio of 3.74 ± 0.5, using 1 M DAAP extraction. Additionally, the purposeful addition of millimolar amounts of nitrite or H2O2 to bismuthate-treated Am solutions did not prevent oxidation, as long as residual solid bismuthate was present. Finally, a series of irradiation experiments using a Nordion Gammacell 220E 60Co source was performed, and kinetic data for the radiolytic reduction of Am(VI) were obtained. Unsurprisingly, it was found that radiolysis reduces Am(VI), but that the presence of Ce(IV) acts as a radioprotection agent, to scavenge radiolytically-produced reducing agents, thereby enhancing the stability of the higher Am oxidation state. Alternative oxidants: To date, sodium bismuthate is the only practical oxidant for Am with utility in solvent extraction. While successful oxidation has been demonstrated with sodium peroxydisulfate, it is impractical for solvent extraction because it is only useful in dilute acid and it introduces sulfate into the process. Oxidation has been demonstrated using silver and cobalt catalyzed ozone, however, reduction upon contact with an organic phase is instantaneous. Oxidation is successful using Cu(III) periodate, and marginally successful in initial testing using DAAP extraction. However, the distribution ratios for the oxidized Am are marginal, because Cu(III) is also rapidly reduced by the organic phase. The possibility may exist that this can be optimized.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Cerium-iron-based magnetic compounds

New magnetic materials containing cerium, iron, and small additions of a third element are disclosed. These materials comprise compounds Ce(Fe.sub.12-xM.sub.x) where x=1-4, having the ThMn.sub.12 tetragonal crystal structure (space group I4/mmm, #139). Compounds with M=B, Al, Si, P, S, Sc, Co, Ni, Zn, Ga, Ge, Zr, Nb, Hf, Ta, and W are identified theoretically, and one class of compounds based on M=Si has been synthesized. The Si cognates are characterized by large magnetic moments (4.pi.M.sub.s greater than 1.27 Tesla) and high Curie temperatures (264.ltoreq.T.sub.c.ltoreq.305.degree. C.). The Ce(Fe.sub.12-xM.sub.x) compound may contain one or more of Ti, V, Cr, and Mo in combination with an M element. Further enhancement in T.sub.c is obtained by nitriding the Ce compounds through heat treatment in N.sub.2 gas while retaining the ThMn.sub.12 tetragonal crystal structure; for example CeFe.sub.10Si.sub.2N.sub.1.29 has T.sub.c=426.degree. C.

36 MATERIALS SCIENCE↗

Oxidation and extraction of Am(VI) using a monoamidic extractant in 3D printed centrifugal contactors

In this study, a series of tests were performed using centrifugal contactors to evaluate the separation of Am(VI) from cerium, as well as to determine the efficiency of the contactors. All experiments were performed using 2-cm, acrylic 3D-printed centrifugal contactors. Solvent extraction tests were performed using 1 M N,N-di(2-ethylhexyl)butyramide (DEHBA)/dodecane and a nitric acid feed solution spiked with 243 Am and 139 Ce and oxidized with 60 mg mL -1 sodium bismuthate. Approximately 72 % of the Am was extracted with a single contactor stage. Co-stripping of Am and Ce was demonstrated but attempts at selective stripping were not successful. Lastly, successful recycle of the used organic phase was demonstrated. Contactor efficiencies of 95-100% were obtained.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The Study of (n, 2n) Reaction Cross Sections for Ce and Nd Isotopes up to 20 MeV

Neutron cross section calculations for {sup 136}Ce(n, 2n){sup 135}Ce, {sup 138}Ce(n, 2n){sup 137}Ce, {sup 140}Ce(n, 2n){sup 139}Ce, {sup 142}Ce(n, 2n){sup 141}Ce, {sup 142}Nd(n, 2n){sup 141}Nd, {sup 144}Nd(n, 2n){sup 143}Nd, {sup 146}Nd(n, 2n){sup 145}Nd, {sup 148}Nd(n, 2n){sup 147}Nd, and {sup 150}Nd(n, 2n){sup 149}Nd were done in the incident energy range from 10 to 20 MeV. The calculations were performed using three codes TALYS-1.6 for two-component Exciton model, EMPIRE-3.2 Malta for Exciton model, and ALICE/ASH for the Geometry-Dependent Hybrid (GDH) model. The results of model calculations were compared with the available experimental data and also with the evaluated data in the TENDL-2015 (based on the modified TALYS code), ENDF/B-VII.1 libraries. The calculated cross section data were compared with the available experimental data obtained from EXFOR and also compared with semiempirical formulas around 14–15 MeV. The results of model calculation were found to be in good agreement with the experimental data given in literature and semiempirical data around 14–15MeV.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗