Uranium Body Clearance Kinetics—A Long-term Follow-up Study of Retired Nuclear Fuel Workers

Abstract

Abstract Nuclear industry workers exposed to uranium aerosols may risk kidney damage and radiation-induced cancer. This warrants the need for well-established dose and risk assessments, which can be greatly improved by using material-specific absorption parameters in the ICRP Human Respiratory Tract Model. The present study focuses on the evaluation of the slow dissolution rate (ss , d−1), a parameter that is difficult to quantify with in vitro dissolution studies, especially for more insoluble uranium compounds. A long-term follow-up of urinary excretion after the cessation of chronic inhalation exposure can provide a better estimate of the slow-rate dissolution. In this study, two workers, previously working for >20 y at a nuclear fuel fabrication plant, provided urine samples regularly for up to 6 y. One individual had worked at the pelletizing workshop with the known presence of uranium dioxide (UO2) and triuranium octoxide (U3O8). The second individual worked at the conversion workshop where multiple compounds, including uranium hexafluoride (UF6), uranium dioxide (UO2), ammonium uranyl carbonate, and AUC [UO2CO3·2(NH4)2CO3], are present. Data on uranium concentration in urine during working years were also available for both workers. The daily excretion of uranium by urine was characterized by applying non-linear least square regression fitting to the urinary data. Material-specific parameters, such as the activity median aerodynamic diameter (AMAD), the respiratory tract absorption parameters, rapid fraction (fr ,), rapid dissolution rate (sr , d−1), and slow dissolution rate (ss , d−1) and alimentary tract transfer factor (fA ) acquired from previous work along with default absorption types, were applied to urine data, and the goodness of fit was evaluated. Thereafter intake estimates and dose calculations were performed. For the ex-pelletizing worker, a one-compartment model with a clearance half-time of 662 ± 100 d (ss = 0.0010 d−1) best represented the urinary data. For the ex-conversion worker, a two-compartment model with a major [93% of the initial urinary excretion (A0)] fast compartment with a clearance half-time of 1.3 ± 0.4 d (sr = 0.5 d−1) and a minor (7% of A0) slow compartment with a half-time of 394 ± 241 d (ss = 0.002 d−1) provided the best fit. The results from the data-fitting of urinary data to biokinetic models for the ex-conversion worker demonstrated that in vitro derived experimental parameters (AMAD = 20 μm, fr = 0.32, sr = 27 d−1, ss = 0.0008 d−1, f A = 0.005) from our previous work best represented the urinary data. This resulted in an estimated intake rate of 0.66 Bq d−1. The results from the data-fitting of urinary data to biokinetic models for the ex-pelletizing worker indicated that the experimental parameters (AMAD = 10 μm and 20 μm, fr = 0.008, sr = 12 d−1, fA = 0.00019) from our previous dissolution studies with the slow rate parameter step-wise optimized to urine-data (ss = 0.0008 d−1) gave the best fit. This resulted in an estimated intake rate of 5 Bq d−1. Experimental parameters derived from in vitro dissolution studies provided the best fit for the subject retired from work at the conversion workshop, where inhalation exposure to a mix of soluble (e.g., AUC, UF6) and relatively insoluble aerosol (e.g., UO2) can be assumed. For the subject retired from work at the pelletizing workshop, which involved exposure to relatively insoluble aerosols (UO2 and U3O8), a considerably higher ss than obtained in dissolution studies provided a better representation of the urinary data and was comparable to reported ss values for UO2 and U3O8 in other studies. This implies that in vitro dissolution studies of insoluble material can be uncertain. When evaluating the results from the retrospective fitting of urine data, it is evident that the urine samples acquired after cessation of exposure provide less fluctuation. Long-term follow-up of uranium excretion after cessation of exposure is a good alternative for determining absorption parameters and can be considered the most viable way for determining the slow rate for more insoluble material.