Investigation of electrorefining of metallic alloy fuel onto solid Al cathodes

This work concerned the electrorefining of UZr and UPuZr alloys on a solid aluminium cathode, in the LiCl-KCl eutectic melt containing U3+, Pu3+, Np3+, Zr2+ or Zr 4+, Am3+, Nd3+, Y3+, Ce3+ and Gd3+ chlorides. During constant current electrolyses, the use of a cathodic cut-off potential (-1.25 V vs. Ag/AgCl) allowed to selectively deposit actinides (mainly U), while lanthanides remainedin the salt. The aim was to determine the maximal load achievable on a single aluminium electrode. The total exchange charge was 4300 C, which represents the deposition of 3.72 g of actinides in 4.17 g Al, yielding a composition of 44.6 wt% An in Al. It was shown that the melting of the cathode contributed to increase the total amount of actinides deposited on the aluminium

Modeling the actinides with disordered local moments

A first-principles disordered local moment (DLM) picture within the local-spin-density and coherent potential approximations (LSDA+CPA) of the actinides is presented. The parameter free theory gives an accurate description of bond lengths and bulk modulus. The case of $\delta$-Pu is studied in particular and the calculated density of states is compared to data from photo-electron spectroscopy. The relation between the DLM description, the dynamical mean field approach and spin-polarized magnetically ordered modeling is discussed.Comment: 6 pages, 4 figure

Predicting the optical observables for nucleon scattering on even-even actinides

Previously derived Lane consistent dispersive coupled-channel optical model for nucleon scattering on $^{232}$Th and $^{238}$U nuclei is extended to describe scattering on even-even actinides with $Z=$90--98. A soft-rotator-model (SRM) description of the low-lying nuclear structure is used, where SRM Hamiltonian parameters are adjusted to the observed collective levels of the target nucleus. SRM nuclear wave functions (mixed in $K$ quantum number) have been used to calculate coupling matrix elements of the generalized optical model. The "effective" deformations that define inter-band couplings are derived from SRM Hamiltonian parameters. Conservation of nuclear volume is enforced by introducing a dynamic monopolar term to the deformed potential leading to additional couplings between rotational bands. Fitted static deformation parameters are in very good agreement with those derived by Wang and collaborators using the Weizs\"acker-Skyrme global mass model (WS4), allowing to use the latter to predict cross section for nuclei without experimental data. A good description of scarce "optical" experimental database is achieved. SRM couplings and volume conservation allow a precise calculation of the compound-nucleus formation cross sections, which is significantly different from the one calculated with rigid-rotor potentials coupling the ground-state rotational band. Derived parameters can be used to describe both neutron and proton induced reactions.Comment: 6 pages, 4 figures, 5 table

X-ray absorption branching ratio in actinides: LDA+DMFT approach

To investigate the x-ray absorption (XAS) branching ratio from the core 4d to valence 5f states, we set up a theoretical framework by using a combination of density functional theory in the local density approximation and Dynamical Mean Field Theory (LDA+DMFT), and apply it to several actinides. The results of the LDA+DMFT reduces to the band limit for itinerant systems and to the atomic limit for localized f electrons, meaning a spectrum of 5f itinerancy can be investigated. Our results provides a consistent and unified view of the XAS branching ratio for all elemental actinides, and is in good overall agreement with experiments.Comment: 6 pages, 4 figure

Evaluation of diffusive gradients in thin-films using a Diphonix® resin for monitoring dissolved uranium in natural waters

Commercially available Diphonix® resin (TrisKem International) was evaluated as a receiving phase for use with the diffusive gradients in thin-films (DGT) passive sampler for measuring uranium. This resin has a high partition coefficient for actinides and is used in the nuclear industry. Other resins used as receiving phases with DGT for measuring uranium have been prone to saturation and significant chemical interferences. The performance of the device was evaluated in the laboratory and in field trials. In laboratory experiments uptake of uranium (all 100% efficiency) by the resin was unaffected by varying pH (4–9), ionic strength (0.01–1.00 M, as NaNO3) and varying aqueous concentrations of Ca2+ (100–500 mg L−1) and HCO3− (100–500 mg L−1). Due to the high partition coefficient of Diphonex®, several elution techniques for uranium were evaluated. The optimal eluent mixture was 1 M NaOH/1 M H2O2, eluting 90% of the uranium from the resin. Uptake of uranium was linear (R2 = 0.99) over time (5 days) in laboratory experiments using artificial freshwater showing no saturation effects of the resin. In field deployments (River Lambourn, UK) the devices quantitatively accumulated uranium for up to 7 days. In both studies uptake of uranium matched that theoretically predicted for the DGT. Similar experiments in seawater did not follow the DGT theoretical uptake and the Diphonix® appeared to be capacity limited and also affected by matrix interferences. Isotopes of uranium (U235/U238) were measured in both environments with a precision and accuracy of 1.6–2.2% and 1.2–1.4%, respectively. This initial study shows the potential of using Diphonix®-DGT for monitoring of uranium in the aquatic environment

Spallation dominated propagation of Heavy Cosmic Rays and the Local Interstellar Medium (LISM)

Measurements of ultra heavy nuclei at GeV/n energies in the galactic cosmic radiation address the question of the sources (nucleosynthetic s- and r-processes). As such, the determination of CR source abundances is a promising way to discriminate between existing nucleosynthesis models. For primary species (nuclei present and accelerated at sources), it is generally assumed that the relative propagated abundances, if they are close in mass, are not too different from their relative source abundances. Besides, the range of the correction factor associated to propagation has been estimated in weighted slab models only. Heavy CRs that are detected near Earth were accelerated from regions that are closer to us than were the light nuclei. Hence, the geometry of sources in the Solar neighbourhood, and as equally important, the geometry of gas in the same region, must be taken into account. In this paper, a two zone diffusion model is used, and as was previously investigated for radioactive species, we report here on the impact of the local interstellar medium (LISM) feature (under-dense medium over a scale ~100 pc) on primary and secondary stable nuclei propagated abundances. Going down to Fe nuclei, the connection between heavy and light abundances is also inspected. A general trend is found that decreases the UHCR source abundances relative to the HCR ones. This could have an impact on the level of r-process required to reproduce the data.Comment: 12 pages, 9 figures, accepted by A&A. Comparison with truncated weighted slab and discussion added. Figure 8 modified. New appendix on truncated weighted slab techniqu