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At least 649 records · Page 36

Minor actinide separation: simplification of the DIAMEX-SANEX strategy by means of novel SANEX processes

The separation of An(III) from PUREX raffinate has previously been demonstrated by applying a DIAMEX process (i.e., co-extraction of An(III) and Ln(III) from HAR) followed by a SANEX process (i.e., selective extraction of An(III) from the DIAMEX product containing An(III) + Ln(III)). In line with process intensification issues, more compact processes have been developed: Recently, a 1c-SANEX process test was successfully performed, directly extracting An(III) from PUREX HAR. More recently, a new i-SANEX process was successfully tested. This process is based on the co-extraction of An(III) + Ln(III) into a TODGA solvent, followed by a selective back-extraction of An(III) by a water soluble complexing agent, in this case SO{sub 3}-Ph-BTP. In both cases, good recoveries were achieved, and very pure product solutions were obtained. However, both 1c-SANEX and i-SANEX used non-CHON chemicals. Nevertheless, these processes are a simplification to the DIAMEX + SANEX process as only one solvent is used. Finally, the new i-SANEX process is the most compact process. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Atalante research facility new mass limits in a unit containing plutonium and minor actinides - 14402

ATALANTE, located in Marcoule, is one of the main Nuclear Facilities of the French Alternative Energies and Atomic Energy Commission (CEA). This facility is mainly dedicated to research and development for nuclear energy related to the back end of the fuel cycle: spent fuel and final waste management. It is a large research complex housing chemistry and analytical laboratories and shielded cells (240 glove boxes and 11 shielded cells), equipped for basic studies through to demonstration experiments. Within the facility, one unit can contain plutonium and curium at the same time. In this case, nuclear criticality safety is achieved by exercising control over mass. A subcritical mass limit is defined for plutonium (280 g for {sup 239}Pu) and an exemption mass limit (3 g for {sup 245}Cm) is used for the actinide. In order to increase the maximum mass (in particular {sup 245}Cm) which can be handled in the unit, new mass control limits were studied, based on control over the sum of the mass ratio to the upper subcritical mass, noted m{sub lim}, for each nuclide (350 g for {sup 239}Pu; 34.8 g or 23 g for {sup 245}Cm) as shown in equation (1) below. m({sup 239}Pu)/ m{sub lim}({sup 239}Pu)+ m({sup 245}Cm)/m{sub lim}({sup 245}Cm)≤1 (1) To validate this criticality safety control method, a study was conducted to demonstrate that, for different masses of {sup 239}Pu and {sup 245}Cm meeting equation (1), the calculated effective multiplication factor is always lower than the effective multiplication factor corresponding to a sphere of 350 g of pure {sup 239}Pu, moderated, with 20 cm water reflection. The two pseudo fissile media are: - metallic plutonium (100% {sup 239}Pu, density 19.86), moderated with water, - metallic curium (100% {sup 245}Cm, density 13.566), moderated with water. The calculation model is a sphere of {sup 245}Cm metal positioned in a sphere of {sup 239}Pu metal, with optimum moderation for each fissile material, and a full water reflection (20 cm). The results show that, under certain conditions, the effective multiplication factor of the mixture can be higher than the effective multiplication factor of each pure fissile material when using the upper subcritical mass of 34.8 g for {sup 245}Cm. When using 23 g of {sup 245}Cm, the k{sub eff} of the mixture is always lower than the k{sub eff} of pure {sup 239}Pu. These calculations enable the safety documentation to be changed by introducing a new process operational procedure, based on equation (1). This change in procedure allows the operator to work with a larger quantity of curium in the unit. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The Miller Range 090340 and 090206 meteorites: Identification of new brachinite-like achondrites with implications for the diversity and petrogenesis of the brachinite clan

Miller Range (MIL) 090340 and MIL 090206 are olivine-rich achondrites originally classified as ureilites. We investigate their petrography, mineral compositions, olivine Cr valences, equilibration temperatures, and (for MIL 090340) oxygen isotope compositions, and compare them with ureilites and other olivine-rich achondrites. We conclude that they are brachinite-like achondrites that provide new insights into the petrogenesis of brachinite clan meteorites. MIL 090340,6 has a granoblastic texture and consists of ~97 modal % by area olivine (Fo = molar Mg/[Mg+Fe] = 71.3 ± 0.6). It also contains minor to trace augite, chromite, chlorapatite, orthopyroxene, metal, troilite, and terrestrial Fe-oxides. Approximately 80% by area of MIL 090206,5 has a granoblastic texture of olivine (Fo 72.3 ± 0.1) plus minor augite and chromite, similar to MIL 090340 but also containing minor plagioclase. The rest of the section consists of a single crystal of orthopyroxene (~11 × 3 mm), poikilitically enclosing rounded grains of olivine (Fo = 76.1 ± 0.6), augite, chromite, metal, and sulfide. Equilibration temperatures for MIL 090340 and MIL 090206, calculated from olivine-spinel, olivine-augite, and two-pyroxene thermometry range from ~800 to 930 °C. In both samples, symplectic intergrowths of Ca-poor orthopyroxene + opaque phases (Fe-oxides, sulfide, metal) occur as rims on and veins/patches within olivine. Before terrestrial weathering, the opaques were probably mostly sulfide, with minor metal. All petrologic properties of MIL 090340 and MIL 090206 are consistent with those of brachinite clan meteorites, and largely distinct from those of ureilites. Oxygen isotope compositions of olivine in MIL 090340 (δ 18 O = 5.08 ± 0.30‰, δ 17 O = 2.44 ± 0.21‰, and Δ 17 O = -0.20 ± 0.12‰) are also within the range of brachinite clan meteorites, and well distinguished from ureilites. Olivine Cr valences in MIL 090340 and the granoblastic area of MIL 090206 are 2.57 ± 0.06 and 2.59 ± 0.07, respectively, similar to those of three brachinites also analyzed here (Brachina, Hughes 026, Nova 003). They are higher than those of olivine in ureilites, even those containing chromite. The valence systematics of MIL 090340, MIL 090206, and the three analyzed brachinites (lower Fo = more oxidized Cr) are consistent with previous evidence that brachinite-like parent bodies were inherently more oxidized than the ureilite parent body. The symplectic orthopyroxene + sulfide/metal assemblages in MIL 090340, MIL 090206, and many brachinite clan meteorites have superficial similarities to characteristic “reduction rims” in ureilites. However, they differ significantly in detail. They likely formed by reaction of olivine with S-rich fluids, with only minor reduction. MIL 090340 and the granoblastic area of MIL 090206 are similar in modal mineralogy and texture to most brachinites, but have higher Fo values typical of brachinite-like achondrites. The poikilitic pyroxene area of MIL 090206 is more typical of brachinite-like achondrites. The majority of their properties suggest that MIL 090340 and MIL 090206 are residues of low-degree partial melting. The poikilitic area of MIL 090206 could be a result of limited melt migration, with trapping and recrystallization of a small volume of melt in the residual matrix. Finally, these two samples are so similar in mineral compositions, Cr valence, and cosmic ray exposure ages that they could be derived from the same lithologic unit on a common parent body.

58 GEOSCIENCES↗

Symmetric spectrum current drive due to finite radial drift effects

We report the drift surfaces of minority heated ions differ from flux surfaces due to finite poloidal gyroradius effects. As the minority poloidal gyroradius approaches radial scale lengths in the plasma, the difference between drift and flux surfaces can modify the heating and lead to a symmetric spectrum minority counter-current being driven. In response, a corresponding overall net co-current of comparable size is driven. This beneficial symmetric spectrum current drive in a tokamak is due to the parallel velocity asymmetry in the drift departure from a flux surface. As this new source of driven current is a side effect of minority heating it comes without any additional economic cost to reactor power balance. The symmetric spectrum current driven for near Maxwellian minorities is evaluated by an adjoint method and found to be modest. However, minority heating typically results in strong non-Maxwellian features on minority distributions so it may be possible to drive a significantly larger co-current. A related evaluation is performed for alpha particles in a deuterium minority heated plasma with a tritium majority. The low density of the alphas tends to keep this driven symmetric spectrum current small, but at very high heating levels a significant co-current might be driven. Other mechanisms to drive co-current with a symmetric spectrum are discussed and estimated, including asymmetric electron drag and focusing of the applied minority heating radio frequency fields.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Symmetric spectrum current drive due to finite radial drift effects

The drift surfaces of minority heated ions differ from flux surfaces due to finite poloidal gyroradius effects. As the minority poloidal gyroradius approaches radial scale lengths in the plasma the difference between drift and flux surfaces can modify the heating and lead to a symmetric spectrum minority counter-current being driven. In response, a corresponding overall net co-current of comparable size is driven. This beneficial symmetric spectrum current drive in a tokamak is due to the parallel velocity asymmetry in the drift departure from a flux surface. As this new source of driven current is a side effect of minority heating it comes without any additional economic cost to reactor power balance. The symmetric spectrum current driven for near Maxwellian minorities is evaluated by an adjoint method and found to be modest. However, minority heating typically results in strong non-Maxwellian features on minority distributions so it may be possible to drive significantly larger co-current. A related evaluation is performed for alpha particles in a deuterium minority heated plasma with a tritium majority. The low density of the alphas tends to keep this driven symmetric spectrum current small, but at very high heating levels a significant co-current might be driven. Other mechanisms to drive co-current with a symmetric spectrum are discussed and estimated, including asymmetric electron drag and focusing of the applied minority heating radio frequency fields.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Plasma heating and hot ion sustaining in mirror based hybrids

Possibilities of plasma heating and sloshing ion sustaining in mirror based hybrids are briefly reviewed. Sloshing ions, i.e. energetic ions with a velocity distribution concentrated to a certain pitch-angle, play an important role in plasma confinement and generation of fusion neutrons in mirror machines. Neutral beam injection (NBI) is first discussed as a method to generate sloshing ions. Numerical results of NBI modeling for a stellarator-mirror hybrid are analyzed. The sloshing ions could alternatively be sustained by RF heating. Fast wave heating schemes, i.e. magnetic beach, minority and second harmonic heating, are addressed and their similarities and differences are described. Characteristic features of wave propagation in mirror hybrid devices including both fundamental harmonic minority and second harmonic heating are examined. Minority heating is efficient for a wide range of minority concentration and plasma densities; it allows one to place the antenna aside from the hot ion location. A simple-design strap antenna suitable for this has good performance. However, this scenario is appropriate only for light minority ions. The second harmonic heating can be applied for the heavy ion component. Arrangements are similar for minority and second harmonic heating. The efficiency of second harmonic heating is influenced by a weaker wave damping than for minority heating. Numerical calculations show that in a hybrid reactor scaled mirror machine the deuterium sloshing ions could be heated within the minority heating scheme, while the tritium ions could be sustained by second harmonic heating.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Cesium vacancy ordering in phase-separated C s x F e 2 - y S e 2

By simultaneously displaying magnetism and superconductivity in a single phase, the iron-based superconductors provide a model system for the study of magnetism's role in superconductivity. The class of intercalated iron selenide superconductors is unique among these in having the additional property of phase separation and coexistence of two distinct phases—one majority phase with iron vacancy ordering and strong antiferromagnetism, and the other a poorly understood minority microscopic phase with a contested structure. Adding to the intrigue, the majority phase has never been found to show superconductivity on its own while the minority phase has never been successfully synthesized separate from the majority phase. In order to better understand this minority phase, a series of high-quality Cs x Fe 2–y Se 2 single crystals with (0.8 ≤ x ≤ 1;0 ≤ y ≤ 0.3) were grown and studied. Neutron and x-ray powder diffraction performed on ground crystals show that the average I4/mmm structure of the minority phase is distinctly different from the high-temperature I4/mmm parent structure. Moreover, single-crystal diffraction reveals the presence of discrete superlattice reflections that remove the degeneracy of the Cs sites in both the majority and minority phases and reduce their structural symmetries from body centered to primitive. Group theoretical analysis in conjunction with structural modeling shows that the observed superlattice reflections originate from three-dimensional Cs vacancy ordering. This model predicts a 25% vacancy of the Cs site in the minority phase which is consistent with the site's refined occupancy. Magnetization measurements performed in tandem with neutron single-crystal diffraction provide evidence that the minority phase is the host of superconductivity. Lastly, our results also reveal a superconducting dome in which the superconducting transition temperature varies as a function of the nominal valence of iron.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Investigation of Benefits from U/TRU Recycle - Quantification and Comparison to U/Pu Recycle

The recently completed comprehensive evaluation and screening of nuclear fuel cycle options identified a number of potentially promising fuel cycles for R&D that offer what could be considered by decision-makers as having the potential for significant improvement compared to the current U.S. fuel cycle. The fuel cycles that consistently performed the best were recycle fuel cycles that used self-sustaining fast reactors operating with either U/Pu or U/TRU recycle fuel and also included options where the fast reactors provided fissile materials to support operation of thermal reactors. However, based on the evaluation criteria and metrics used in the study, there was no difference in benefit between recycle of U/Pu and U/TRU (where TRU is plutonium and the minor actinides) while there were differences in the challenges for developing and deploying such fuel cycles, with U/TRU recycle being more challenging. This observation prompted the question as to the desirability of pursuing R&D on U/TRU recycle given that there may not be an increase in benefit. As a result, activities have been pursued to further investigate the performance differences between U/Pu and U/TRU recycle based on considering issues beyond those used in the evaluation and screening study to identify, if possible, areas where there are significant benefits of U/TRU recycle compared to U/Pu recycle. These new considerations focused on several areas, but especially on the impact on disposal of the HLW, which in the case of U/Pu recycle contains all of the minor actinides along with fission products, while in the case of U/TRU recycle only contains the losses of minor actinides from the reprocessing and recycle fuel fabrication operations. This difference in content has several implications. One impact is on the time dependent decay heat which can affect handling and the use of space in a geologic repository. Another impact concerns the HLW form and volume, since presence of minor actinides may adversely affect the ability to reduce HLW volume. The short-term radioactivity and long-term radiotoxicity of the HLW is also affected, which may be of more or less importance depending on the specific geologic disposal environment. To study these potential effects, a range of waste forms and disposal environments were used in the analysis, documenting to what extent the recycle of minor actinides in addition to plutonium may offer further benefit. Another area of investigation concerned the recycle fuel, for the fast reactor and for the thermal reactors they may support. Information to date indicates that U/Pu fuel may be simpler to fabricate and has a much more extensive database than U/TRU fuel, one of the reasons for the increased challenge for developing and deploying a U/TRU fuel cycle, and also indicates that heterogeneous recycle of the minor actinides may be even more difficult as compared to homogeneous recycle. This information was reviewed and updated to reflect the most recent studies for the purpose of informing on all aspects of the differences between U/Pu and U/TRU recycle. The results of all of these investigations will be presented to provide information on the findings concerning the value of U/TRU recycle.

Fast reactor recycle↗