[In Vitro] Dissolution Of Commercial Yellowcake And Comparisons With Available Human Data

INTRODUCTION If a uranium mill worker is involved in an accident, analysis of excreta for uranium content and[in vivo] counting methods are used to estimate the extent of the possible exposure and to predict the pattern of uranium distribution among tissues (Spitz, [et al]., 1980). Interpretations of urinary excretion data are based on studies of human exposures to single uranium compounds including U02, U308, U03, UF4, U02F2 and UF6 (Alexander, 1974). Refined uranium ore (yellowcake) is a variable mixture of U03-NH3-H20 adducts (ammonium diuranate, ADU) and their thermal conversion product, U308. The variability in composition of yellowcake (Kalkwarf, 1979; Eidson and Mewhinney, 1980; Dennis, Blauer and Kent, 1981) complicates the interpretation of bioassay data from individuals that might have inhaled any single yellowcake material. A test system would be useful to estimate the dissolution behavior of a particular yellowcake aerosol inhaled by a worker and aid in the interpretation of bioassay data collected before and after an accident. A series of experiments was conducted for this purpose. The objectives of these studies were to: 1) develop specific criteria for comparing [in vitro] dissolution systems and 2) use the criteria to evaluate solvents, methods and experimental temperature and pH conditions used in previous studies. Dissolution experiments were conducted using different combinations of solvents, conditions and methods with a common yellowcake sample. Because little information is available from human yellowcake inhalation exposures to evaluate the [in vitro] results, criteria for evaluation of different tests were derived from a model of yellowcake dissolution in lung constructed from a number of cases in which humans were exposed to single uranium compounds known to be in yellowcake (Mercer, 1975). MATERIALS AND METHODS Materials The powder used in the tests was taken from one lot of yellowcake obtained from a commercial uranium mill. The same powder was previously designated as Mill D in Eidson and Mewhinney, 1980 and Mill 2 in Kalkwarf, 1979. The ammonium diuranate content was measured by infrared absorption to be 25% ± 1% (Eidson and Mewhinney, 1980). Solvents The compositions of the two biological fluid simulants used are compared in Table 1. Simulated lung fluid (SLF) (Kalkwarf, 1979; Dennis, Blauer and Kent, 1981) was chosen to simulate the composition [ ] of lung fluid as closely as practical (Moss, 1979). Simulated blood serum ultrafiltrate (SUF) (Eidson and Mewhinney, 1980) was chosen because of previous successful efforts to model human urinary excretion of inhaled plutonium aerosols (Kanapilly Raabe and Boyd, 1974) and the dissolution rate of 241Am02 in Beagle dogs (Mewhinney and Griffith, 1981). Major differences are that simulated lung fluid contains Mg2+ and a higher Ca2+ concentration than SUF and that SUF contains ammonium ion. Both solvents include protein substitutes; acetate is used in SLF, while amino acids are used in SUF. Both solvents include phosphate but the chelating agent diethylenetriaminepentaacetic acid (DTPA) is included in SUF to prevent possible formation of insoluble uranyl phosphate precipitates that would result in an underestimation of solubility. In addition to the above solvents, modified solvent compositions were prepared to investigate the role of specific salts in yellowcake dissolution studies. Solutions of SUF (Table 1) were prepared without DTPA (SUF-DTPA) and without amino acids (SUF-amino acids). No solution excluded both DTPA and amino acids. The SLF solutions were prepared with DTPA (SLF + DTPA) and without phosphate