Introducing DEPDOSE, a Tool to Calculate Dose Coefficients to Members of the Public for Radioactive Aerosols.

ABSTRACT: This paper presents DEPDOSE, an open-source computer application that combines the KDEP respiratory tract deposition fractions for inhaled aerosols with DC_PAK committed equivalent dose coefficients for a unit deposition in each region of the respiratory tract. DEPDOSE allows the user to rapidly produce tables of dose coefficients for workers and members of the public inhaling precisely defined, user-specified aerosols using the ICRP Publication 60 methodology. Combined with a plume dispersion modeling system, such as the Quick Urban & Industrial Complex (QUIC) Dispersion Modeling System, this makes it possible to predict radiation doses downstream from an accidental or intentional release of radioactive materials. For this work, a radioactive plume was calculated to members of the public downstream from a dirty bomb in Chicago. DEPDOSE is published under an open source license, and can be downloaded at https://github.com/lanl/DEPDOSE .

Chelation Modeling of a Plutonium-238 Inhalation Incident Treated with Delayed DTPA.

This work describes an analysis, using a previously established chelation model, of the bioassay data collected from a worker who received delayed chelation therapy following a plutonium-238 inhalation. The details of the case have already been described in two publications. The individual was treated with Ca-DTPA via multiple intravenous injections and then nebulizations beginning several months after the intake and continuing for four years. The exact date and circumstances of the intake are unknown. However, interviews with the worker suggested that the intake occurred via inhalation of a soluble plutonium compound. The worker provided daily urine and fecal bioassay samples throughout the chelation treatment protocol, including samples collected before, during, and after the administration of Ca-DTPA. Unlike the previous two publications presenting this case, the current analysis explicitly models the combined biokinetics of the plutonium-DTPA chelate. Using the previously established chelation model, it was possible to fit the data through optimizing only the intake (day and magnitude), solubility, and absorbed fraction of nebulized Ca-DTPA. This work supports the hypothesis that the efficacy of the delayed chelation treatment observed in this case results mainly from chelation of cell-internalized plutonium by Ca-DTPA (intracellular chelation). It also demonstrates the validity of the previously established chelation model. As the bioassay data were modified to ensure data anonymization, the calculation of the "true" committed effective dose was not possible. However, the treatment-induced dose inhibition (in percentage) was calculated.

Modified human respiratory tract model to describe the retention of plutonium in scar tissues.

The Human Respiratory Tract Model described in Publication 130 of the International Commission on Radiological Protection provides some mechanisms to account for retention of material that can be subject to little to no mechanical transport or absorption into the blood. One of these mechanisms is 'binding', which refers to a process by which a fraction ('bound fraction') of the dissolved material chemically binds to the tissue of the airway wall. The value of the bound fraction can have a significant impact on the radiation doses imparted to different parts of the respiratory tract. To properly evaluate-and quantify-bound fraction for an element, one would need information on long-term retention of the element in individual compartments of the respiratory tract. Such data on regional retention of plutonium in the respiratory tract of four workers-who had inhaled materials with solubility ranging from soluble nitrate to very insoluble high-fired oxides-were obtained at the United States Transuranium and Uranium Registries. An assumption of bound fraction alone was found to be inconsistent with this dataset and also with a review of the literature. Several studies show evidence of retention of a large amount of Pu activity in the scar tissues of humans and experimental animals, and accordingly, a model structure with scar-tissue compartments was proposed. The transfer rates to these compartments were determined using Markov Chain Monte Carlo analysis of the bioassay and post-mortem data, considering the uncertainties associated with deposition, dissolution and particle clearance parameters. The models predicted that a significant amount-between 20 and 100% for the cases analyzed-of plutonium retained in the respiratory tract was sequestered in the scar tissues. Unlike chemically-bound Pu that irradiates sensitive epithelial cells, Pu in scar tissues may not be dosimetrically significant because the scar tissues absorb most, if not all, of the energy from alpha emissions.

Chelation Model Validation: Modeling of a Plutonium-238 Inhalation Incident Treated with DTPA at Los Alamos National Laboratory.

ABSTRACT: Accidental inhalation of plutonium at the workplace is a non-negligible risk, even when rigorous safety standards are in place. The intake and retention of plutonium in the human body may be a source of concern. Thus, if there is a suspicion of a significant intake of plutonium, medical countermeasures such as chelation treatment may be administered to the worker. The present work aimed to interpret the bioassay data of a worker involved in an inhalation incident due to a glovebox breach at Los Alamos National Laboratory's plutonium facility. The worker was treated with intravenous injections of calcium salts of diethylenetriaminepentaacetic acid (DTPA) in an attempt to reduce the amount of plutonium from the body and therefore reduce the internal radiation dose. It is well known in the internal dosimetry field that the administration of chelation treatment poses additional challenges to the dose assessment. Hence, a recently developed chelation model was used for the modeling of the bioassay data. The objectives of this work are to describe the incident, model the chelation-affected and non-affected bioassay data, estimate the plutonium intake, and assess the internal radiation dose.

Dose Assessment Following a 238 Pu Inhalation Incident at Los Alamos National Laboratory.

ABSTRACT: A glovebox breach at the plutonium facility at Los Alamos National Laboratory potentially exposed 15 individuals to 238 Pu aerosols. One of the individuals (P0) received two 1-g intravenous DTPA treatments, one on the day of the intake and another the following day. Several urine samples were collected from the individuals involved in the incident. Particle size analysis on the PPE and solubility analysis of the particles on a filter sample were conducted in vitro. The applicability of the results from the in vitro studies for dose assessment was questionable because of the effect of the cloth mask the workers were wearing for COVID-related protection. Based on several considerations, including the effect of cloth masks on the "effective" particle size inhaled and the analysis of fecal-to-urine ratio, the default Type M 1 µm AMAD model was used to estimate intakes and doses. Using the urinary excretion data collected after 100 d post last chelation treatment, the committed effective dose, E(50), for P0 was calculated to be 5.2 mSv. For all others, the bioassay data were consistent with no intakes or very small intakes [corresponding to E(50) less than 0.1 mSv].

Side Effects and Complications Associated with Treating Plutonium Intakes: A Retrospective Review of the Medical Records of LANL Employees Treated for Plutonium Intakes, with Supplementary Interviews.

ABSTRACT: Anecdotal evidence indicates there may be unpublished physical and psychological events associated with the medical treatment of plutonium intakes. A thorough review was conducted of the medical and bioassay records of current and previous Los Alamos National Laboratory (LANL) employees who had experienced plutonium intakes via wound or inhalation. After finding relatively incomplete information in the medical records, the research team interviewed current LANL employees who had undergone chelation therapy and/or surgical excision. Although the dataset is not large enough to reach statistically significant conclusions, it was observed that adverse events associated with treatment appear to be more frequent and more severe than previously reported.

Public health response and medical management of internal contamination in past radiological or nuclear incidents: A narrative review.

Following a radiological or nuclear emergency, workers, responders and the public may be internally contaminated with radionuclides. Screening, monitoring and assessing any internal contamination and providing necessary medical treatment, especially when a large number of individuals are involved, is challenging. Experience gained and lessons learned from the management of previous incidents would help to identify gaps in knowledge and capabilities on preparedness for and response to radiation emergencies. In this paper, eight large-scale and five workplace radiological and nuclear incidents are reviewed cross 14 technical areas, under the broader topics of emergency preparedness, emergency response and recovery processes. The review findings suggest that 1) new strategies, algorithms and technologies are explored for rapid screening of large populations; 2) exposure assessment and dose estimation in emergency response and dose reconstruction in recovery process are supported by complementary sources of information, including 'citizen science'; 3) surge capacity for monitoring and dose assessment is coordinated through national and international laboratory networks; 4) evidence-based guidelines for medical management and follow-up of internal contamination are urgently needed; 5) mechanisms for international and regional access to medical countermeasures are investigated and implemented; 6) long-term health and medical follow up programs are designed and justified; and 7) capabilities and capacity developed for emergency response are sustained through adequate resource allocation, routine non-emergency use of technical skills in regular exercises, training, and continuous improvement.

Dose Coefficients for Internal Dose Assessments for Exposure to Radioactive Fallout.

ABSTRACT: This paper presents values as well as the bases for calculating internal dose coefficients suitable for estimating organ doses from the exposure to radioactive fallout that could result from the detonation of a nuclear fission device. The 34 radionuclides discussed are the same as those given in a priority list of radionuclides for fallout dose assessments presented in a companion overview paper. The radionuclides discussed are those that are believed to account for a preponderance of the organ doses that might be received by intake by persons of all ages (including in utero and via breast feeding for infants) following exposure to radioactive fallout. The presented dose coefficients for ingestion account for age and include modifications for variations in solubility with distance as discussed previously in the literature, and those for inhalation similarly account for age, solubility, and particle sizes that would be relevant at various distances of exposure as discussed in a companion paper on ingestion dose methods. The proposed modifications peculiar to radioactive fallout account for systematic changes in solubility and particle sizes with distance from the site of detonation, termed here as the region of "local fallout" and the region "beyond local fallout." Brief definitions of these regions are provided here with more detailed discussion in a companion paper on estimating deposition of fallout radionuclides. This paper provides the dose coefficients for ingestion and inhalation (for particle sizes of 1 µm, 5 µm, 10 µm, and 20 µm) for the region "local fallout." These dose coefficients for "local fallout" are specific for particles formed in a nuclear explosion that can be large and have radionuclides, particularly the more refractory ones, distributed throughout the volume where the radionuclide has reduced solubility. The dose coefficients for the region "beyond local fallout" are assumed to be the ones published by the International Commission on Radiological Protection (ICRP) in 1995. Comparisons of the presented dose coefficients are made with values published by the ICRP.

MODELING THE LONG-TERM RETENTION OF PLUTONIUM IN THE HUMAN RESPIRATORY TRACT USING SCAR-TISSUE COMPARTMENTS.

The respiratory tract tissues of four former nuclear workers with plutonium intakes were radiochemically analyzed post mortem by the United States Transuranium and Uranium Registries. Plutonium activities in the upper respiratory tract of these individuals were found to be higher than those predicted using the most recent biokinetic models described in publications of the International Commission on Radiological Protection. Modification of the model parameters, including the bound fraction, was not able to explain the data in one of the four individuals who had inhaled insoluble form of plutonium. Literature review points to the presence of-and a significant retention of-plutonium in the scar tissues of the lungs. Accordingly, an alternate model with scar-tissue compartments corresponding to larynx, bronchi, bronchioles, alveolar-interstitium and thoracic lymph nodes was proposed. The rates of transfer to the scar tissue compartments were determined using Markov Chain Monte Carlo analysis of data on urinary excretion, lung counts and post-mortem measurements of liver, skeleton and individual respiratory tract compartments, as available. The posterior models predicted that 20-100%-depending on the solubility of the material inhaled-of the activities retained in the respiratory tract were sequestered in the scar tissues.

Long-term Retention of Plutonium in the Respiratory Tracts of Two Acutely-exposed Workers: Estimation of Bound Fraction.

ABSTRACT: Inhalation of plutonium is a significant contributor of occupational doses in plutonium production, nuclear fuel reprocessing, and cleanup operations. Accurate assessment of the residence time of plutonium in the lungs is important to properly characterize dose and, consequently, the risk from inhalation of plutonium aerosols. This paper discusses the long-term retention of plutonium in different parts of the respiratory tract of two workers who donated their bodies to the US Transuranium and Uranium Registries. The post-mortem tissue radiochemical analysis results, along with the urine bioassay data, were interpreted using Markov Chain Monte Carlo and the latest biokinetic models presented in the Occupational Intakes of Radionuclides series of ICRP publications. The materials inhaled by both workers were found to have solubility between that of plutonium nitrates and oxides. The long-term solubility was also confirmed by comparison of the activity concentration in the lungs and the thoracic lymph nodes. The data from the two individuals can be explained by assuming a bound fraction (fraction of plutonium deposited in the respiratory tract that becomes bound to lung tissue after dissolution) of 1% and 4%, respectively, without having to significantly alter the particle clearance parameters. Effects of different assumptions about the bound fraction on radiation doses to different target regions was also investigated. For inhalation of soluble materials, an assumption of fb of 1%, compared to the ICRP default of 0.2%, increases the dose to the most sensitive target region of the respiratory tract by 258% and that to the total lung by 116%. Some possible alternate methods of explaining higher-than-expected long-term retention of plutonium in the upper respiratory tract of these individuals-such as physical sequestration of material into the scar tissues and possible uptake by lungs-are also briefly discussed.

Modelling of long-term retention of high-fired plutonium oxide in the human respiratory tract: importance of scar-tissue compartments.

The U.S. Transuranium and Uranium Registries whole-body tissue donor Case 0407 had an acute intake of 'high-fired' plutonium oxide resulting from a glove-box fire in a fabrication plant at a nuclear defence facility. The respiratory tract of this individual was dissected into five regions (larynx, bronchi, bronchioles, alveolar-interstitial, and thoracic lymph nodes) and analysed for plutonium content. The activities in certain compartments of the respiratory tract were found to be higher than expected from the default models described in publications of the International Commission on Radiological Protection. Because of the extremely slow rate of dissolution of the material inhaled, the presence of bound fraction is incapable of explaining the higher-than-expected retention. A plausible hypothesis-encapsulation of plutonium in scar tissues-is supported by the review of literature. Therefore, scar-tissue compartments corresponding to the larynx, bronchi, bronchioles and alveolar-interstitial regions were added to the existing human respiratory tract model structure. The transfer rates between these compartments were determined using Markov Chain Monte Carlo analysis of data on urinary excretion, lung counts and post-mortem measurements of the liver, skeleton and regional retention in the respiratory tract. Modelling of the data showed that approximately 30% of plutonium activity in the lung was sequestered in scar tissues. The dose consequence of such sequestration is qualitatively compared against that of chemical binding.

Dose Assessment Following a 238Pu-contaminated Wound Case with Chelation and Excision.

The urinary excretion and wound retention data collected after a Pu-contaminated wound were analyzed using Markov Chain Monte Carlo (MCMC) to obtain the posterior distribution of the intakes and doses. An empirical approach was used to model the effects of medical treatments (chelation and excision) on the reduction of doses. It was calculated that DTPA enhanced the urinary excretion, on average, by a factor of 17. The empirical analysis also allowed calculation of the efficacies of the medical treatments-excision and chelation averted approximately 76% and 5.5%, respectively, of the doses that would have been if there were no medical treatment. All bioassay data are provided in the appendix for independent analysis and to facilitate the compartmental modeling approaches being developed by the health physics community.

Response to a Skin Puncture Contaminated with 238Pu at Los Alamos National Laboratory.

The three principal pathways for intakes of plutonium are ingestion, inhalation, and contaminated wounds. In August 2018, a glovebox worker at Los Alamos National Laboratory (LANL) sustained a puncture from a thread of a braided steel cable contaminated with Pu. The puncture produced no pain, no blood, and little or no visible mark. As a result, the potential for a contaminated wound was not immediately recognized, and a wound count was not conducted until elevated urine bioassay results were received 12 d after the incident. This paper discusses the circumstances of the incident, along with the medical response and dose assessment, and a discussion of the risks and benefits of the medical interventions.

Development of a New Chelation Model: Bioassay Data Interpretation and Dose Assessment after Plutonium Intake via Wound and Treatment with DTPA.

The administration of chelation therapy to treat significant intakes of actinides, such as plutonium, affects the actinide's normal biokinetics. In particular, it enhances the actinide's rate of excretion, such that the standard biokinetic models cannot be applied directly to the chelation-affected bioassay data in order to estimate the intake and assess the radiation dose. The present study proposes a new chelation model that can be applied to the chelation-affected bioassay data after plutonium intake via wound and treatment with DTPA. In the proposed model, chelation is assumed to occur in the blood, liver, and parts of the skeleton. Ten datasets, consisting of measurements of C-DTPA, Pu, and Pu involving humans given radiolabeled DTPA and humans occupationally exposed to plutonium via wound and treated with chelation therapy, were used for model development. The combined dataset consisted of daily and cumulative excretion (urine and feces), wound counts, measurements of excised tissue, blood, and post-mortem tissue analyses of liver and skeleton. The combined data were simultaneously fit using the chelation model linked with a plutonium systemic model, which was linked to an ad hoc wound model. The proposed chelation model was used for dose assessment of the wound cases used in this study.

Chelation Modeling: The Use of Ad Hoc Models and Approaches to Overcome a Dose Assessment Challenge.

Chelating agents are administered to treat significant intakes of radioactive elements such as plutonium, americium, and curium. These drugs may be used as a medical countermeasure after radiological accidents and terrorist acts. The administration of a chelating agent, such as Ca-DTPA or Zn-DTPA, affects the actinide's normal biokinetics. It enhances the actinide's rate of excretion, posing a dose assessment challenge. Thus, the standard biokinetic models cannot be directly applied to the chelation-affected bioassay data in order to assess the radiation dose. The present study reviews the scientific literature, from the early 1970s until the present, on the different studies that focused on developing new chelation models and/or modeling of bioassay data affected by chelation treatment. Although scientific progress has been achieved, there is currently no consensus chelation model available, even after almost 50 y of research. This review acknowledges the efforts made by different research groups, highlighting the different methodology used in some of these studies. Finally, this study puts into perspective where we were, where we are, and where we are heading in regards to chelation modeling.

Biokinetics of 238Pu oxides: inferences from bioassay data.

The bioassay data collected from several workers involved in 238Pu inhalation incidents have been analysed using the most recent biokinetic models described in the Occupational Intakes of Radionuclides (OIR) series of publications. Although all exposures were thought to be to 238Pu oxides, the observed urinary excretion patterns differed in different inhalation incidents. The urinary excretion from individuals involved in one of the incidents increased steadily with time, peaking around two to three years before decreasing. This pattern is described in Part 4 of the OIR series using the '238PuO2, ceramic' model. This non-monotonic behaviour, explained as being due to fragmentation and dissolution, was not specific to the incident, but observed in other incidents. The urinary excretion data collected from individuals involved in another incident showed dissolution behaviour between Type M and Type S. Finally, the bioassay data from yet another incident showed a pattern that appears to represent behaviour more insoluble than Type S, which is possibly a result of self-heating due to the decay heat from 238Pu. The urinary excretion patterns and corresponding dose coefficients have been calculated and compared.

Mitigating the Psychological Harm from Actinide Intakes.

Investigations into possible actinide intakes, as well as the intakes themselves, may result in significant psychological harm that should be mitigated by the internal dosimetrist. Many aspects of this psychological impact are unique to actinide intakes and have not been discussed in the literature. This paper discusses some of these unique considerations and describes how the Internal Dosimetry Team at Los Alamos National Laboratory (LANL) has, with input and guidance from LANL psychologists, tried to address them. We feel that much of the psychological harm can be mitigated by educating employees specifically about internal dosimetry and internal doses, and by improving communication with radiation workers.

Some Considerations for Chelation Treatment and Surgical Excision Following Incorporation of Plutonium in Wounds.

After a plutonium-contaminated wound, the role of an internal dosimetrist is to inform the patient and the physician of the dosimetric considerations. The doses averted due to medical treatments (excision or chelation) are higher if the treatments are administered early; therefore, the internal dosimetrist needs to rely on limited information on wound counts and process knowledge for advising the physician. Several wound cases in the literature were reviewed to obtain estimates of the efficacies of surgical excision and chelation treatment after plutonium-contaminated wounds. The dose coefficients calculated by coupling the NCRP 156 wound model with the systemic model were used to derive the decision guidelines that may indicate medical treatment based on 1) the concept of saved doses proposed by the NCRP 156 wound model, 2) the limits recommended by the CEC/DOE guidebook, and 3) the Clinical Decision Guidelines proposed in NCRP Report No. 161. These guidelines by themselves, however, are of limited use for several reasons, including 1) large uncertainties associated with wound measurements, 2) exposure to forms of radionuclides that cannot be assigned to a single category in the NCRP 156 framework, 3) inability of the NCRP 156 model to explain some of the wound cases in the literature, 4) neglect of the local doses to the wound site and the pathophysiological response of the tissue, 5) poorly understood relationship between effective doses and risks of late health effects, and 6) disregard of the psychological aspects of radionuclide intake.

ANALYSIS OF URINARY EXCRETION DATA FROM THREE PLUTONIUM-CONTAMINATED WOUNDS AT LOS ALAMOS NATIONAL LABORATORY.

The National Council on Radiation Protection (NCRP)-156 Report proposes seven different biokinetic models for wound cases depending on the physicochemistry of the contaminant. Because the models were heavily based on experimental animal data, the authors of the report encouraged application and validation of the models using bioassay data from actual human exposures. Each of the wound models was applied to three plutonium-contaminated wounds, and the models resulted in a good agreement to only one of the cases. We then applied a simpler biokinetic model structure to the bioassay data and showed that fitting the transfer rates from this model structure yielded better agreement with the data than does the best-fitting NCRP-156 model. Because the biokinetics of radioactive material in each wound is different, it is impractical to propose a discrete set of model parameters to describe the biokinetics of radionuclides in all wounds, and thus each wound should be treated empirically.

Bayesian Analysis of Plutonium Bioassay Data at Los Alamos National Laboratory.

The main concern of operational internal dosimetry is to detect intakes and estimate doses to the worker from a series of bioassay measurements. Although several methods are available, the inverse problem of internal dosimetry-i.e., determination of time, amount, and types of intake given a set of bioassay data-is well suited to a Bayesian approach. This paper summarizes the Bayesian methodology used at Los Alamos National Laboratory to detect intakes and estimate doses from plutonium bioassay measurements. Some advantages and disadvantages of the method are also discussed. The successful application of Bayesian methods for several years at Los Alamos National Laboratory, which monitors thousands of workers annually for plutonium, indicates that the methods can be extended to other facilities.