Nuclear fuels fission products

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]. 

Calculational methods used to determine the neutron multiplication should be validated, preferably against applicable measured data (see Appendix VII). For irradiated nuclear fuel this vahdation should include comparison with measured radionuclide data. The results of this validation should be included in determining the uncertainties and biases normally associated with the calculated neutron multiplication. Fission product cross-sections can be important in criticality safety analyses for irradiated nuclear fuel. Fission product cross-section measurements and evaluations over broad energy ranges have not been emphasized to the extent that actinide cross-sections have. Therefore, the adequacy of fission product cross-sections used in the assessment should be considered and justified by the safety analyst. 

Uranium is converted by CIF, BiF, and BrP to UF. The recovery of uranium from irradiated fuels has been the subject of numerous and extensive investigations sponsored by atomic energy agencies in a number of countries (55—63). The fluorides of the nuclear fission products are nonvolatile hence the volatile UF can be removed by distiUation (see Nuclearreactors Uraniumand uranium compounds). 

Spent nuclear fuel has fission products, uranium, and transuranic elements. Plans call for permanent disposal in underground repositories. Geological studies are in progress at the Yucca Mountain site in Nevada. Until a repository is completed, spent fuel must be stored in water pools or in dry storage casks at nuclear plant sites. 

Spent fuel can be stored or disposed of intact, in a once-through mode of operation, practiced by the U.S. commercial nuclear power industry. Alternatively, spent fuel can be reprocessed, ie, treated to separate the uranium, plutonium, and fission products, for re-use of the fuels (see Nuclear REACTORS, CHEMICAL reprocessing). In the United States reprocessing is carried out only for fuel from naval reactors. In the nuclear programs of some other countries, especially France and Japan, reprocessing is routine. 

Water as coolant in a nuclear reactor is rendered radioactive by neutron irradiation of corrosion products of materials used in reactor constmction. Key nucHdes and the half-Hves in addition to cobalt-60 are nickel-63 [13981 -37-8] (100 yr), niobium-94 [14681-63-1] (2.4 x 10 yr), and nickel-59 [14336-70-0] (7.6 x lO" yr). Occasionally small leaks in fuel rods allow fission products to enter the cooling water. Cleanup of the water results in LLW. Another source of waste is the residue from appHcations of radionucHdes in medical diagnosis, treatment, research, and industry. Many of these radionucHdes are produced in nuclear reactors, especially in Canada. 

Spent Fuel Treatment. Spent fuel assembhes from nuclear power reactors are highly radioactive because they contain fission products. Relatively few options are available for the treatment of spent fuel. The tubes and the fuel matrix provide considerable containment against attack and release of nucHdes. To minimi2e the volume of spent fuel that must be shipped or disposed of, consoHdation of rods in assembhes into compact bundles of fuel rods has been successfully tested. Alternatively, intact assembhes can be encased in metal containers. 

Approximately 25—30% of a reactor s fuel is removed and replaced during plaimed refueling outages, which normally occur every 12 to 18 months. Spent fuel is highly radioactive because it contains by-products from nuclear fission created during reactor operation. A characteristic of these radioactive materials is that they gradually decay, losing their radioactive properties at a set rate. Each radioactive component has a different rate of decay known as its half-life, which is the time it takes for a material to lose half of its radioactivity. The radioactive components in spent nuclear fuel include cobalt-60 (5-yr half-Hfe), cesium-137 (30-yr half-Hfe), and plutonium-239 (24,400-yr half-Hfe). 

During the operation of nuclear power reactors, which are fuelled with ceramic UO2 fuel rods, the fission of the nuclei leads to die formation of fission products which are isotopes of elements in all of tire Groups of the Periodic Table. The major fission products, present in 1-10% abundance, fall into five groups divided according to the chemical interaction of each product with the fuel ... 

It is also invaluable in separating U from Pu and other fission products during nuclear fuel reprocessing, since Pu reacts only to give the (involatile) PUF4 and most fission products... 

Many of the fission products formed in a nuclear reactor are themselves strong neutron absorbers (i.e. poisons ) and so will stop the chain reaction before all the (and Pu which has also been formed) has been consumed. If this wastage is to be avoided the irradiated fuel elements must be removed periodically and the fission products separated from the remaining uranium and the plutonijjm. Such reprocessing is of course inherent in the operation of fast-breeder reactors, but whether or not it is used for thermal reactors depends on economic and political factors. Reprocessing is currently undertaken in the UK, France and Russia but is not considered to be economic in the USA. 

Figure 31.3 Flow diagram for the reprocessing of nuclear fuel [FP = fission products TBP = (Bu"0)3PO).

The main drawback to nuclear power is the production of radioactive waste. Spent fuel from a nuclear reactor is considered a high-level radioactive waste, and remains radioactive for a veiy long time. Spent fuel consists of fission products from the U-235 and Pu-239 fission process, and also from unspent U-238, Pu-240, and other heavy metals produced during the fuel cycle. That is why special programs exist for the handling and disposal of nuclear waste. 

Besides fission products, the various forms of known but newly formed elements in the spent nuclear fuel, there is a small but significant amount of fissionable, or fissile, material in the SNF. This is quite important. There is some unused, unfissioned U-235 that has become too dilute to use. Like natural uranium ores in which chain reactions do not... 

Chemistry is the key to the safe use of nuclear power. It is used in the preparation of the fuel itself, the recovery of important fission products, and the safe disposal or utilization of nuclear waste. 

Fluidized-bed CVD was developed in the late 1950s for a specific application the coating of nuclear-fuel particles for high temperature gas-cooled reactors. PI The particles are uranium-thorium carbide coated with pyrolytic carbon and silicon carbide for the purpose of containing the products of nuclear fission. The carbon is obtained from the decomposition of propane (C3H8) or propylene... 

The effect of irradiation on the extractability of sulfoxides towards plutonium, uranium and some fission products were studied by Subramanian and coworkers . They studied mainly the effect of irradiation on dihexyl sulfoxide (DHSO) and found that irradiation did not change the distribution coefficient for Ru, Eu and Ce but increases the distribution coefficient for Zr and Pu. When comparing DHSO and tributyl phosphate (TBP), the usual solvent for the recovery and purification of plutonium and uranium from spent nuclear fuels, the effect of irradiation to deteriorate the extraction capability is much larger in TBP. Lan and coworkers studied diphenyl sulfoxides as protectors for the gamma radiolysis of TBP. It was found that diphenyl sulfoxide can accept energy from two different kinds of excited TBP and thus inhibits the decomposition of the latter. 

Nuclear fuel reprocessing was first undertaken with the sole purpose of recovering plutonium, for weapons use, from uranium irradiated in nuclear reactors. These reactors, called the production reactors, were dedicated to transmuting as much of the uranium as possible to plutonium. From its original scope of recovering exclusively plutonium, with no attempts to either recover or recycle uranium, nuclear fuel reprocessing has since grown into a much more sophisticated and complex operation with expanded scope. It is now called upon to separate uranium and plutonium from the fission products, and to purify these elements to levels at which these fissile materials can be conveniently recycled for reuse. The present scope also extends to fission products separation and concentration. 

The fact that spent fuel reprocessing and recycle are essential components ofgood nuclear non-proliferation and radioactive waste management practices. These actions are needed so that more efficient use can be made offissionablc materials, and unwanted radioactive fission products can be disposed of without need for permanent safeguards. In addition, potential weapons usable materials are destroyed through beneficial use. 

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