Neutron Activation Analysis Of Thorium-230*

INTRODUCTION The radiological health significance of thorium-230 stems from its tendency to separate from the uranium238 parent, concentrate in bone tissues, and to subsequently irradiate the radiosensitive tissues lining the bone surfaces and the bone marrow. Indeed, thorium-230 may be the radionuclide which contributes the major dose following intake of natural uranium (Hartley and Pasternack 1979). This is reflected by the most recent recommendations of the International Commission on Radiological Protection, which specify the limits shown in Table I for the annual intake of radionuclides by occupationally exposed workers (ICRP 1979). TABLE 1. Occupational Annual Intake Limits (microcuries per year) for Selected Uranium Nuclides and Daughters (ICRP 79) [Radionuclide Ingestion Inhalation] [Uranium-238 200 0.05 Uranium-235 200 0.05 Uranium-234 200 0.03 Thorium-234 300 200 Thorium-230 3 0.02 Radium-226 2 0.5] Clearly, the relatively low annual limit of intake for thorium-230 shows it to be of greater radiological concern than its parent radionuclides. Because of the greater toxicity and different metabolism of thorium-230, monitoring only for uranium-238 does not satisfactorily identify the possible hazard from thorium-230 nor does it provide any real indication of the metabolism or biodynamics of these two radionuclides. Thorium-230 has a half-life of 80,000 years and can be detected by direct counting of the alpha particles or photons emitted during its transformation to radium-226. The 4.69 and 4.62 MeV alpha particles are distinctive and specific indicators of thorium-230 and are emitted with abundances of 76% and 24%, respectively. The principal photon, a 68 keV gamma ray, is emitted in only 0.37% of the transformations and is, therefore, not useful for low level measurements. The other photons emitted have even lower yields, or, in the case of radium L x-rays, are non-specific and, hence, useless for quantification. High sensitivity measurements of thorium-230 currently are usually accomplished by wet washing of the sample substrate, quantitative chemical separation of thorium atoms, and, finally, direct measurement of the alpha particles emitted from a massless deposition. This procedure is complicated, expensive, and time-consuming, and subject to interferences from uranium, other actinides, and other thorium isotopes. Recently, the feasibility of low-level measurement of thorium-230 by neutron activation analysis (NAA) was demonstrated (Kathren, Desrosiers and Church 1980). Two principal variations of the NAA method were used in this study: 1) instrumental NAA technique and 2) post-irradiation radiochemical separations (RCS). Instrumental NAA procedure is a nondestrucive technique which is preferred because of its simplicity. The procedure is as follows: after irradiation with a known neutron fluence, the samples are transferred to a clean container and quantitative gamma spectroscopy performed. With the radiochemical separations procedure, the sample is initially treated as in the instrumental technique. However, after irradiation, a known amount of "carrier" is added to the sample. The element(s) of interest are then separated from the rest of the matrix by distillation, precipitation and extraction techniques. The resulting sample, now free of interferring elements, is then ready for gamma-ray analysis. The use of a "carrier" is to determine the loss of element-of-interest during the chemical separations process. The neutron activation cross section of thorium-230 has an epicadmium resonance value of 1,010 barns (Mughahghab and Garber 1976) and a thermal neutron cross section of 23 barns. The 25.52 hr thorium-231 produced releases two photons of significance: an 84 keV complex, (6.5% yield) and 25.6 keV (15% yield) (Lederer and Shirley 1978). The 84 keV complex is particularly useful for quantification since neither natural uranium, thorium, their daughters, or activation products emit photons in this region. However, the higher yield of the 25.6 keV photon may result in increased sensitivity if there are no other photons of similar energy emitted by other radionuclides in the sample. PRELIMINARY STUDIES Thorium-230 standard stock solution was prepared from a pure sample of the oxide purchased from Oak Ridge National Laboratory. From this stock solution a series of samples were prepared for irradiation in the TRIGA Mark I reactor at Reed College. Various dilutions were prepared as well as thorium-230 spiked urine samples. Irradiation times varied from 1 to 54 minutes in a neutron fluence rate of 1.84 x 1012 n/ cu m-sec. The neutron spectrum was abundant in thermal neutrons, having a Cd ratio of approximately 10. Treated urine samples were also analyzed by the NAA instrumental method. Analysis of untreated urine samples was not possible due to the high background