Fission-product elements radioactivity

The population of fission product elements as a function of time is changing rapidly. These may be estimated from a knowledge of the half-lives of the fission product chain members, the mass chain yield, and the independent yield distribution along the mass chains. Although there are some uncertainties in these procedures largely because of lack of data on short-lived species, and a less than perfect understanding of the charge distribution function, reasonable estimates of radioactive atom... 

Early Work. The irradiated fuel, upon discharge from the reactor, comprises the residual unbumt fuel, its protective cladding of magnesium alloy, zirconium or stainless steels, and fission products. The fission process yields over 70 fission product elements, while some of the excess neutrons produced from the fission reaction are captured by the uranium isotopes to yield a range of hew elements—neptunium, plutonium, americium, and curium. Neutrons are captured also by the cladding materials and yield a further variety of radioactive isotopes. To utilize the residual uranium and plutonium in further reactor cycles, it is necessary to remove the fission products and transuranic elements and it is usual to separate the uranium and plutonium this is the reprocessing operation. 

A second mode of production in reactors is by the fission process itself as the majority of fission products are radioactive and cover a wide range of atomic numbers of varying abundances. These radioactivities may be isolated with high specific activity in contrast to the neutron capture products. However, in fission products the isolation of any particular radioactive element can require a fairly lengthy separation from the large number of other radioactivities present we discuss this further in Chapter 21. 

Sepa.ra.tion of Plutonium. The principal problem in the purification of metallic plutonium is the separation of a small amount of plutonium (ca 200—900 ppm) from large amounts of uranium, which contain intensely radioactive fission products. The plutonium yield or recovery must be high and the plutonium relatively pure with respect to fission products and light elements, such as lithium, beryUium, or boron. The purity required depends on the intended use for the plutonium. The high yield requirement is imposed by the price or value of the metal and by industrial health considerations, which require extremely low effluent concentrations. 

The same problems of separating radioactive materials occur of course with the fission products of uranium where the task is often to separate a much larger number of different carrier-free radio-elements than occurs in normal targets. The mixture is complex and consists of elements from zinc to terbium and several hundred radioactive isotopes of varying half-life. 

The fission products contain some 50 elements located in the middle part of the periodic system. Some of the fission products are produced in considerable amounts, though their radioactivity is rather low [71], and they were therefore thought to have a potential value on the mineral market. 

The major characteristic of technetium is that it is the only element within the 29 transition metal-to-nonmetal elements that is artificially produced as a uranium-fission product in nuclear power plants. It is also the tightest (in atomic weight) of all elements with no stable isotopes. Since all of technetiums isotopes emit harmful radiation, they are stored for some time before being processed by solvent extraction and ion-exchange techniques. The two long-lived radioactive isotopes, Tc-98 and Tc-99, are relatively safe to handle in a well-equipped laboratory. 

Since transport by water is virtually the only available mechanism for escape, we will be predominantly concerned with the chemistry of aqueous solutions at the interface with inorganic solids - mainly oxides. These will be at ordinary to somewhat elevated temperatures, 20-200 C, because of the heating effects of radioactive decay during the first millennium. The elements primarily of interest (Table I) are the more persistent fission products which occur in various parts of the periodic table, and the actinides, particularly uranium and thorium and, most important of all, plutonium. 

Symbol Ce atomic number 58 atomic weight 140.115 a rare-earth metal a lanthanide series inner-transition /-block element metaUic radius (alpha form) 1.8247A(CN=12) atomic volume 20.696 cm /mol electronic configuration [Xe]4fi5di6s2 common valence states -i-3 and +4 four stable isotopes Ce-140 and Ce-142 are the two major ones, their percent abundances 88.48% and 11.07%, respectively. Ce—138 (0.25%) and Ce—136(0.193%) are minor isotopes several artificial radioactive isotopes including Ce-144, a major fission product (ti 284.5 days), are known. 

Xenon occurs in the atmosphere at trace concentrations. It also occurs in gases from certain mineral springs. Xenon also is a fission product of uranium, plutonium, and thorium isotopes induced by neutron bombardment. The radioactive fission product, xenon-135, has a very high thermal neutron cross-section. The element has been detected in Mars atmosphere. 

Apatite is being considered as a barrier that will prevent the leakage of radioactive nuclei from the radioactive waste storage. Because of the similarity in the chemical and spectral features REE have been chosen as a model of the fission products of the actinides. For this reason it is of importance to recognize whether the elements are incorporated in the bulk of the barrier, or adsorbed on the surface where they can be subjected to leaching out (Martin et al. 1996 Martin et al. 1999a Martin et al. 1999b). 

Touring the formation of radioactive fallout particles, one of the most important processes is the uptake, in the cooling nuclear fireball, of the vaporized radioactive fission products by particles of molten soil or other environmental materials. Owing to the differences in the chemical nature of the various radioactive elements, their rates of uptake vary, depending upon temperature, pressure, and substrate and vapor-phase composition. These varying rates of uptake, combined with different residence times of the substrate particles in the fireball, result in radiochemical fractionation of the fallout. This fractionation has a considerable effect on the final partition of radioactivity, exposure rate, and radionuclides between the ground surface and the atmosphere. 

There are little data available which can be used to predict the rates of uptake of the different vaporized radioactive elements or oxides. Since such data are important to the application of any fallout prediction model based on kinetics, a program has been started at this laboratory to measure the rates of uptake of a selected group of fission-product oxides under conditions approximating those found in the cooling fireball. The data from these measurements will be useful, not only as input to fallout models, but also for discovering the mechanisms which govern the rates of uptake. 

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... 

In tlie PUREX process, the spent fuel and blanket materials are dissolved in nitric acid to form nitrates of plutonium and uranium. These are separated chemically from the other fission products, including the highly radioactive actinides, and then the two nitrates are separated into tv/o streams of partially purified plutonium and uranium. Additional processing will yield whatever purity of the two elements is desired. The process yields purified plutonium, purified uranium, and high-level wastes. See also Radioactive Wastes in the entry1 on Nuclear Power Technology. Because of the yield of purified plutonium, the PUREX process is most undesirable from a nuclear weapons proliferation standpoint,... 

The third principal component of environmental radioactivity is that due to the activities of humans, the anthropogenic radionuclides. This group of nuclides includes the previously discussed cases of 3H and 14C along with the fission products and the transuranium elements. The primary sources of these nuclides are nuclear weapons tests and nuclear power plant accidents. These events and the gross nuclide releases associated with them are shown in Table 3.1. Except for 14C and... 

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