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

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 ( s s , 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 (UO 2 ) and triuranium octoxide (U 3 O 8 ). The second individual worked at the conversion workshop where multiple compounds, including uranium hexafluoride (UF 6 ), uranium dioxide (UO 2 ), ammonium uranyl carbonate, and AUC [UO 2 CO 3 ·2(NH 4 ) 2 CO 3 ], 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 ( f r ,), rapid dissolution rate ( s r , d -1 ), and slow dissolution rate ( s s , d -1 ) and alimentary tract transfer factor ( f A ) 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 ( s s = 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 (A 0 )] fast compartment with a clearance half-time of 1.3 ± 0.4 d ( s r = 0.5 d -1 ) and a minor (7% of A 0 ) slow compartment with a half-time of 394 ± 241 d ( s s = 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, f r = 0.32, s r = 27 d -1 , s s = 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, f r = 0.008, s r = 12 d -1 , f A = 0.00019) from our previous dissolution studies with the slow rate parameter step-wise optimized to urine-data ( s s = 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, UF 6 ) and relatively insoluble aerosol (e.g., UO 2 ) can be assumed. For the subject retired from work at the pelletizing workshop, which involved exposure to relatively insoluble aerosols (UO 2 and U 3 O 8 ), a considerably higher s s than obtained in dissolution studies provided a better representation of the urinary data and was comparable to reported s s values for UO 2 and U 3 O 8 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.

Particle Size Dependent Dissolution of Uranium Aerosols in Simulated Gastrointestinal Fluids.

ABSTRACT: Uranium aerosol exposure can be a health risk factor for workers in the nuclear fuel industry. Good knowledge about aerosol dissolution and absorption characteristics in the gastrointestinal tract is imperative for solid dose assessments and risk management. In this study, an in vitro dissolution model of the GI tract was used to experimentally study solubility of size-fractionated aerosols. The aerosols were collected from four major workshops in a nuclear fuel fabrication plant where uranium compounds such as uranium hexafluoride (UF 6 ), uranium dioxide (UO 2 ), ammonium uranyl carbonate, AUC [UO 2 CO 3 ·2(NH 4 ) 2 CO 3 ] and triuranium octoxide (U 3 O 8 ) are present. The alimentary tract transfer factor, f A , was estimated for the aerosols sampled in the study. The transfer factor was derived from the dissolution in the small intestine in combination with data on absorption of soluble uranium. Results from the conversion workshop indicated a f A in line with what is recommended (0.004) by the ICRP for inhalation exposure to Type M materials. Obtained transfer factors, f A , for the powder preparation and pelletizing workshops where UO 2 and U 3 O 8 are handled are lower for inhalation and much lower for ingestion than those recommended by the ICRP for Type M/S materials f A = 0.00029 and 0.00016 vs. 0.0006 and 0.002, respectively. The results for ingestion and inhalation f A indicate that ICRP's conservative recommendation of f A for inhalation exposure is applicable to both ingestion and inhalation of insoluble material in this study. The dissolution- and subsequent absorption-dependence on particle size showed correlation only for one of the workshops (pelletizing). The absence of correlation at the other workshops may be an effect of multiple chemical compounds with different size distribution and/or the reported presence of agglomerated particles at higher cut points having more impact on the dissolution than particle size. The impact on dose coefficients [committed effective dose (CED) per Bq] of using experimental f A vs. using default f A recommended by the ICRP for the uranium compounds of interest for inhalation exposure was not significant for any of the workshops. However, a significant impact on CED for ingestion exposure was observed for all workshops when comparing with CED estimated for insoluble material using ICRP default f A . This indicates that the use of experimentally derived site-specific f A can improve dose assessments. It is essential to acquire site-specific estimates of the dissolution and absorption of uranium aerosols as this provides more realistic and accurate dose- and risk-estimates of worker exposure. In this study, the results indicate that ICRP's recommendations for ingestion of insoluble material might overestimate absorption and that the lower f A found for inhalation could be more realistic for both inhalation and ingestion of insoluble material.

Particle Size-dependent Dissolution of Uranium Aerosols in Simulated Lung Fluid: A Case Study in a Nuclear Fuel Fabrication Plant.

ABSTRACT: Inhalation exposure to uranium aerosols can be a concern in nuclear fuel fabrication. The ICRP provides default absorption parameters for various uranium compounds but also recommends determination of material-specific absorption parameters to improve dose calculations for individuals exposed to airborne radioactivity. Aerosol particle size influences internal dosimetry calculations in two potentially significant ways: the efficiency of particle deposition in the various regions of the respiratory tract is dependent on aerodynamic particle size, and the dissolution rate of deposited materials can vary according to particle size, shape, and porosity because smaller particles tend to have higher surface-to-volume ratios than larger particles. However, the ICRP model assumes that deposited particles of a given material dissolve at the same rate regardless of size and that uptake to blood of dissolved material normally occurs instantaneously in all parts of the lung (except the anterior portion of the nasal region, where zero absorption is assumed). In the present work, the effect of particle size on dissolution in simulated lung fluid was studied for uranium aerosols collected at the plant, and its influence on internal dosimetry calculations was evaluated. Size fractionated uranium aerosols were sampled at a nuclear fuel fabrication plant using portable cascade impactors. Absorption parameters, describing dissolution of material according to the ICRP Human Respiratory Tract Model, were determined in vitro for different size fractions using simulated lung fluid. Samples were collected at 16 time-points over a 100-d period. Uranium content of samples was determined using inductively coupled plasma mass spectrometry and alpha spectrometry. In addition, supplementary experiments to study the effect of pH drift and uranium adsorption on filter holders were conducted as they could potentially influence the derived absorption parameters. The undissolved fraction over time was observed to vary with impaction stage cut-point at the four main workshops at the plant. A larger fraction of the particle activity tended to dissolve for small cut-points, but exceptions were noted. Absorption parameters (rapid fraction, rapid rate, and slow rate), derived from the undissolved fraction over time, were generally in fair agreement with the ICRP default recommendations for uranium compounds. Differences in absorption parameters were noted across the four main workshops at the plant (i.e., where the aerosol characteristics are expected to vary). The pelletizing workshop was associated with the most insoluble material and the conversion workshop with the most soluble material. The correlation between derived lung absorption parameters and aerodynamic particle size (impactor stage cut-point) was weak. For example, the mean absorption parameters derived from impaction stages with low (taken to be <5 µm) and large (≥5 µm) cut-points did not differ significantly. Drift of pH and adsorption on filter holders appeared to be of secondary importance, but it was found that particle leakage can occur. Undissolved fractions and to some degree derived lung absorption parameters were observed to vary depending on the aerodynamic size fraction studied, suggesting that size fractionation (e.g., using cascade impactors) is appropriate prior to conducting in vitro dissolution rate experiments. The 0.01-0.02 µm and 1-2 µm size ranges are of particular interest as they correspond to alveolar deposition maxima in the Human Respiratory Tract Model (HRTM). In the present work, however, the dependency on aerodynamic size appeared to be of minor importance, but it cannot be ruled out that particle bounce obscured the results for late impaction stages. In addition, it was noted that the time over which simulated lung fluid samples are collected (100 d in our case) influences the curve-fitting procedure used to determine the lung absorption parameters, in particular the slow rate that increased if fewer samples were considered.

Uranium Aerosol Activity Size Distributions at a Nuclear Fuel Fabrication Plant.

Inhalation of uranium aerosols is a concern in nuclear fuel fabrication. Determination of committed effective doses and lung equivalent doses following inhalation intake requires knowledge about aerosol characteristics; e.g., the activity median aerodynamic diameter (AMAD). Cascade impactor sampling of uranium aerosols in the breathing zone of nuclear operators was carried out at a nuclear fuel fabrication plant producing uranium dioxide via ammonium uranyl carbonate. Complementary static sampling was carried out at key process steps. Uranium on impaction substrates was measured using gross alpha counting and alpha spectrometry. Activity size distributions were evaluated for both unimodal and bimodal distributions. When a unimodal distribution was assumed, the average AMAD in the operator breathing zone at the workshops was 12.9-19.3 µm, which is larger than found in previous studies. Certain sampling occasions showed variable isotope ratios (U/U) at different impactor stages, indicating more than one population of particles; i.e., a multimodal activity size distribution. When a bimodal distribution (coarse and fine fraction) was assumed, 75-88% of the activity was associated with an AMAD of 15.2-18.9 µm (coarse fraction). Quantification of the AMAD of the fine fraction was associated with large uncertainties. Values of 1.7-7.1 µm were obtained. Static sampling at key process steps in the workshops showed AMADs of 4.9-17.2 µm, generally lower than obtained by breathing zone sampling, when a unimodal distribution was assumed. When a bimodal distribution was assumed, a smaller fraction of the activity was associated with the coarse fraction compared to breathing zone sampling. This might be due to impactor positioning during sampling and sedimentation of large particles. The average committed effective dose coefficient for breathing zone sampling and a bimodal distribution was 1.6-2.6 µSv Bq for U when Type M/S absorption parameters were assumed (5.0 µSv Bq for an AMAD of 5 µm). The corresponding lung equivalent dose coefficient was 3.6-10.7 µSv Bq (29.9 µSv Bq for an AMAD of 5 µm). The predicted urinary excretion level 100 d after inhalation intake was found to be 13-34% of that corresponding to an AMAD of 5 µm. Uranium aerosols generated at a nuclear fuel fabrication plant using ammonium uranyl carbonate route of conversion were associated with larger AMADs compared to previous work, especially when sampling of aerosols was carried out in the operator breathing zone. A bimodal activity size distribution can be used in calculations of committed effective doses and lung equivalent doses, but parameters associated with the fine fraction must be interpreted with care due to large uncertainties.