Fission products determination

The chemical identities of the fission products determine their subsequent redistribution, those elements which are in the gaseous state at the temperature of the operation migrating to the cooler exterior of the fuel rods, and die less voltile elements undergoing incorporation in the fuel rod in solid solution. Thus caesium and iodine migrate to the gas fill which sunounds the fuel rod, and elements such as the rare earths and zirconium are accommodated in solid solution in UO2 without significant migration along the fuel rod radius. Strontium and barium oxidize to form separate islands which can be seen under the microscope. 

An extraction process for separating actinide elements (principally uranium, U, and plutonium, Pu) from fission products in an aqueous solution of spent fuel rods is illustrated in Figure 5.31. The extraction solvent is 30% tributyl phosphate (TBP) in kerosene. The most extractable of the fission products are zirconium, niobium and ruthenium. Zirconium, Zr, is used herein to represent the fission products. Determine the number of stages required in the wash section and in the extraction section. Determine the percentage of the Pu in the feed which is recovered in the extract product. V denotes the relative volumetric flowrate. 

The throwaway fuel cycle does not recover the energy values present ia the irradiated fuel. Instead, all of the long-Hved actinides are routed to the final waste repository along with the fission products. Whether or not this is a desirable alternative is determined largely by the scope of the evaluation study. For instance, when only the value of the recovered yellow cake and SWU equivalents are considered, the world market values for these commodities do not fully cover the cost of reprocessing (2). However, when costs attributable to the disposal of large quantities of actinides are considered, the classical fuel cycle has been the choice of virtually all countries except the United States. 

An accident sequence source term requires calculating temperatures, pressures, and fluid flow rates in the reactor coolant system and the containment to determine the chemical environment to which fission products are exposed to determine the rates of fission product release and deposition and to assess the performance of the containment. All of these features are addressed in the... 

Computer sensitivity studies show that hole size strongly affects the fraction of fission products released from the containment. The failure location determines mitigation due to release into another building in which condensation and particulate removal occur. The quantity released depends on the time of containment fails relative to reactor vessel failure. If containment integrity is maintained for several hours after core melt, then natural and engineered mechanisms (e.g., deposition, condensation, and filtration) can significantly reduce the quantity and radioactivity of the aerosols released to the atmosphere. 

In addition to the aforementioned methods, TLC in combination with other instrumental techniques have also been used for quantification of inorganic species. For example, two-dimensional TLC coupled with HPLC has been utilized for the separation and quantification of REEs in nuclear fuel fission products using silaiuzed silica gel as layer material [60]. In another interesting method, REEs in geological samples have been determined by ICP-AAS after their preconcentration by TLC on Fixion plates [32]. TLC in combination with neutron activation has been used to determine REE in rock samples on Eixion 50 x 8 layers with the sensitivity limit of 0.5 to 10 pg/g for 10- to 30-mg samples [41]. A combination of TLC and A AS has been utilized for the isolation and determination of zinc in forensic samples [27]. 

A radiochemical procedure is proposed for the determination of technetium activities from mixed fission products of uranium and thorium. The chief decontamination step is the extraction of TcO into a tetrapropylammonium hydroxide-bromoform mixture from 4.0 M NaOH solutions. Decontamination factors of 10 with chemical yields of 50-70% have been obtained. 

A method has been developed for the determination of technetium-99 in mixed fission products by neutron activation analysis Tc is separated from most fission products by a cyclohexanone extraction from carbonate solution, the stripping into water by addition of CCI4 to the cylohexanone phase, and the adsorption on an anion exchange column. Induced Tc radioactivity is determined using X-ray spectrometry to measure the 540 and 591 keV lines. The sensitivity of the analysis under these conditions is approximately 5 ng. The method has been successfully applied to reactor fuel solutions. 

Suitable conditions for the quantitative polarographic determination of technetium as pertechnetate are given by Miller et al. who propose a 0.1 M KCl solution of pH 10 or a phosphate buffer solution of pH 7. Since in pH 7 buffer the current is directly proportional to the concentration of technetium over the range of 0.1 to 1.1 ppm, this medium has been used for the determination of low concentrations of technetium in solutions of fission products by the standard addition technique. The half-wave potential of the used wave is —0.68 V vs. SCE. The reaction appears to be irreversible (Fig. 13). It has been found that neither rhenium, ruthenium nor other fission products interfere. However, tetraphenyl-arsonium chloride is reduced at a more positive potential than is pertechnetate therefore, (QH5) AsCl, if present, must be separated. 

For the rapid determination of Tc in a mixture of uranium fission products. Love and Greendale have used the method of amalgam polarography. It consists in a selective reduction of technetium at a dropping mercury electrode at a potential of —1.55 V vs. SCE in a medium of 1 M sodium citrate and 0.1 M NaOH. Under these conditions, technetium is reduced to an oxidation state which is soluble in mercury. The amalgam is removed from the solution of fission fragments and the amount of Tc determined in nitric acid solution of the amalgam by a y count. For Tc the measurement accuracy is within 1 %, and the decontamination factor from other fission products 10 . 

The quasi-simultaneous separation and determination of lanthanides and actinides by ion chromatography inductively coupled plasma mass spectrometry combined with the isotope dilution technique and the further use of ion chromatography for the determination of fission products and actinides in nuclear applications are described by Betti et ul.10 48 68... 

Gross dissolution of the waste can be measured from the loss of weight of the sample or by determination of the appearance in the leaching medium of the major matrix constituent e.g. glass). However, the selective leaching of important fission product elements has been observed in this work to be significantly different from that of the bulk waste matrix. The units normally used to describe leach rates, g/cm day, appear to imply... 

Concern about fission-product release from coated reactor fuel particles and fission-product sorption by fallout particles has provided stimulus to understand diffusion. In a fallout program mathematics of diffusion with simple boundary conditions have been used as a basis for (1) an experimental method of determining diffusion coefficients of volatile solutes and (2) a calculational method for estimating diffusion profiles with time dependent sources and. time dependent diffusion coefficients. The latter method has been used to estimate the distribution of fission products in fallout. In a fission-product release program, a numerical model which calculates diffusion profiles in multi-coated spherical particles has been programmed, and a parametric study based on coating and kernel properties has provided an understanding of fission product release. 

The retention of fission product iodine and xenon by unirradiated and irradiated pyrolytic-carbon-coated (Th,U)C2 fuel particles has been studied in annealing experiments and has been compared with similar studies of the release (or retention) of barium and strontium. The objective was to study the effects of irradiation on the retention of the two types of fission products and to determine the mechanism of release which could account for the observed behaviors. In both unirradiated and irradiated particles, iodine and xenon were found to be retained highly by the impervious isotropic pyrolytic coating which was unaffected by the irradiation. In contrast, the fuel kernel which controls the release of the metallic species is damaged severely by the irradiation, resulting in a marked decrease in its ability to retain the metals. 

Tihe atmosphere contains many radionuclides which result from nuclear weapons testing and from natural processes. The nuclear weapons-produced radionuclides include both fission products and activation products from the construction materials of the device. The natural radionuclides include the decay products of radon and thoron, the natural radionuclides in the airborne dust, and the cosmic-ray-produced radionuclides which result from spallation reactions in the atmosphere. Through the determination of the absolute and relative concentrations of this wide spectrum of radionuclides, it should be possible to define the rates of both the long term stratospheric processes and the shorter term tropospheric processes. At the beginning of 1962 a ground-level... 

The character of the radioactive debris from a land surface explosion is determined largely by the extent of mixing between the extraneous debris injected into the cloud and the fission product radioactivities. Within the early cloud there is a well developed toroidal circulation (5), which is clearly evident in the case of air bursts and large yield surface bursts. In low yield surface explosions it may be obscured quickly by the dirt cloud and by rapid damping of a systematic circulation. 

The differences in condensation history of the three alkaline-earth element fission products allows examination of their radioactivity ratio as a method for determining fractionation. The recent atmospheric... 

Figure 11.1 suggests fission proceeds in two steps, the ascent to the saddle point and the passage through the scission point. We shall present our discussion of fission from this point of view. We shall assert that like chemical reactions, the reaction probability is determined by the passage through the transition state. We shall also assert, more controversially, that the distribution of fission product energies, masses, and so forth is determined at or near the scission point. 

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