Search

During the dissolution of the spent nuclear fuel (SNF) some radionuclides are released to the solution simultaneously from different sources in the fuel. This is of particular importance to some radionuclides that contribute to the Instant Release Fraction (IRF), which govern the initial radiation dose during the dissolution of the SNF. In this work a model that is able to discriminate between the different contributions responsible for the total concentration of a radionuclide in solution was developed. The model permits to establish that uranium and radionuclides that dissolved congruently with the UO2 matrix came from two sources as a function of time: oxidized phases on the surface of the SNF including fines and the matrix itself. Other radionuclides such as Ru and Rh were released from metallic precipitates with dissolution rates lower than the matrix dissolution rate. In the case of radionuclides that were expected to contribute to the IRF, this work showed that Cs, Rb and Sr had initial release rates higher than uranium because a fraction of such radionuclides were segregated from the matrix during the irradiation. Actually it was calculated that the fraction of those radionuclides in the grain boundaries in a BWR SNF powder sample from the center part of a pellet (burnup 42 MWd/kgU) was 2.1%, 0.9%, and 0.6% for Cs, Rb, and Sr, respectively. In addition, the model permitted to calculate the duration of their contribution to the IRF, matrix dissolution governed the release of such radionuclides after 137 days, 75 days, and 164 days for Cs, Rb, and Sr, respectively (at these times, the contribution of the release from grain boundaries was lower than the 0.1%).

Screen-printed carbon nanofiber electrodes (SPCNFEs) represent an alternative with great acceptance due to their results, as well as their low impact on the environment. In order to improve their performance, in the present work they were modified with silver nanoparticles (Ag-NPs) and electrochemically characterized by using anodic stripping voltammetry. From the Ag-NP synthesis, silver seeds (Ag-NS) and silver nanoprisms (Ag-NPr) were obtained. The Ag-NP formation was confirmed by micrographs, where Ag-NPs with diameters of 12.20 &plusmn, 0.04 nm for Ag-NS and 20.40 &plusmn, 0.09 nm for Ag-NPr were observed. The electrodes were modified by using three different deposition methods&mdash, drop-casting, spin-coating, and in situ approaches&mdash, that offer different nanoparticle distribution and electrode modification times. It was observed that the last methodology showed a low amount of Ag-NS deposited on the electrode surface and deep alteration of this surface. Those facts suggest that the in situ synthesis methodology was not appropriate for the determination of heavy metals, and it was discarded. The incorporation of the nanoparticles by spin-coating and drop-casting strategies showed different spatial distribution on the electrode surface, as proved by scanning electron microscopy. The electrodes modified by these strategies were evaluated for the cadmium(II) and lead(II) detection using differential pulse anodic stripping voltammetry, obtaining detection limit values of 2.1 and 2.8 &micro, g&middot, L&minus, 1, respectively. The overall results showed that the incorporation route does not directly change the electrocatalytic effect of the nanoparticles, but the shape of these nanoparticles (spherical for seeds and triangular for prisms) has preferential electrocatalytic enhancement over Cd(II) or Pb(II).

This is a post-peer-review, pre-copyedit version of an article published in Journal of Radioanalytical and Nuclear Chemistry. The final authenticated version is available online at: http://dx.doi.org/10.1007/s10967-018-6217-2. This work studies the influence of epsilon particles and metallic precipitates, simulated through the deposition of Pd nanoparticles on non-irradiated UO2, on the oxidation of the spent nuclear fuel (SNF). The presence of Pd nanoparticles favored the reduction by hydrogen of oxidized uranium phases located on the UO2 surface, decreased the oxidation of the UO2 by H2O in the absence of hydrogen, and, in the presence of hydrogen and water vapor, no oxidation of the UO2 by water was detected, contrasting experiments without Pd nanoparticles.

This work determines the capacity of uranophane, one of the long-term uranyl secondary solid phases formed on the spent nuclear fuel (SNF), to retain radionuclides (cesium and strontium) released during the dissolution of the SNF. Sorption was fast in both cases, and uranophane had a high sorption capacity for both radionuclides (maximum sorption capacities of 1.53·10-5¿mol¿m-2 for cesium and 3.45·10-3¿mol¿m-2 for strontium). The high sorption capacity of uranophane highlights the importance of the formation of uranyl silicates as secondary phases during the SNF dissolution, especially in retaining the release of radionuclides not retarded by other mechanisms such as precipitation.

This work determines the capacity of uranophane, one of the long-term uranyl secondary solid phases formed on the spent nuclear fuel (SNF), to retain radionuclides (cesium and strontium) released during the dissolution of the SNF. Sorption was fast in both cases, and uranophane had a high sorption capacity for both radionuclides (maximum sorption capacities of 1.53·10

The effect of the presence of NaCl on the synthesis of Egyptian blue pigment (cuprorivaite, CaCuSi4O10) was studied through experiments in which different amounts of NaCl were introduced in the initial mixture of reactants. The solids synthesized were characterized by X-ray Diffraction, Field Emission Scanning Electron Microscopy (FE-SEM) coupled to Energy-Dispersive Spectrometry (EDS) and High Resolution Transmission Electron Microscopy (HR-TEM) coupled to EDS. The main result of the experiments was that Egyptian blue formation was inhibited in the presence of NaCl, actually, almost no cuprorivaite was found in > 10% NaCl experiments and the solids synthesized in NaCl were always green instead of the characteristic blue of the Egyptian blue pigment. The solids synthesized in the presence of NaCl, a mixture of wollastonite (CaSiO3) and a Cu-rich amorphous phase, probably corresponded to the composition of the pigment known as Egyptian green. Considering the usual presence of NaCl on some of the raw materials used for the pigment fabrication, Egyptian artisans had to be very careful on selecting the reactants for the fabrication of the pigment (quartz would be much more suitable than Egyptian sand, and ash plants than natron) or they incorporated a process of purification of the reactants in order to eliminate chlorides prior to the synthesis.