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Title: Physicochemical Characterization of Capstone Depleted Uranium Aerosols II: Particle Size Distributions as a Function of Time

Abstract

The Capstone Depleted Uranium (DU) Aerosol Study, which generated and characterized aerosols containing depleted uranium from perforation of armored vehicles with large-caliber DU penetrators, incorporated a sampling protocol to evaluated particle size distributions. Aerosol particle size distribution is an important parameter that influences aerosol transport and deposition processes as well as the dosimetry of the inhaled particles. These aerosols were collected on cascade impactor substrates using a pre-established time sequence following the firing event to analyze the uranium concentration and particle size of the aerosols as a function of time. The impactor substrates were analyzed using beta spectrometry, and the derived uranium content of each served as input to the evaluation of particle size distributions. Activity median aerodynamic diameters (AMADs) of the particle size distributions were evaluated using unimodal and bimodal models. The particle size data from the impactor measurements was quite variable. Most size distributions measured in the test based on activity had bimodal size distributions with a small particle size mode in the range of between 0.2 and 1.2 um and a large size mode between 2 and 15 um. In general, the evolution of particle size over time showed an overall decrease of average particle size frommore » AMADs of 5 to 10 um shortly after perforation to around 1 um at the end of the 2-hr sampling period. The AMADs generally decreased over time because of settling. Additionally, the median diameter of the larger size mode decreased with time. These results were used to estimate the dosimetry of inhaled DU particles.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
949878
Report Number(s):
PNNL-SA-64971
Journal ID: ISSN 0017-9078; HLTPAO; TRN: US0901913
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Health Physics, 96(3):266-275; Journal Volume: 96; Journal Issue: 3
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; AERODYNAMICS; AEROSOLS; BETA SPECTROSCOPY; CASCADE IMPACTORS; DEPLETED URANIUM; DEPOSITION; DISTRIBUTION; DOSIMETRY; EVALUATION; PARTICLE SIZE; PENETRATORS; SAMPLING; SUBSTRATES; TRANSPORT; URANIUM; aerosols; environmental contamination; depleted uranium; airborne radioactivity

Citation Formats

Cheng, Yung-Sung, Kenoyer, Judson L., Guilmette, Raymond A., and Parkhurst, MaryAnn. Physicochemical Characterization of Capstone Depleted Uranium Aerosols II: Particle Size Distributions as a Function of Time. United States: N. p., 2009. Web. doi:10.1097/01.HP.0000290613.41486.cb.
Cheng, Yung-Sung, Kenoyer, Judson L., Guilmette, Raymond A., & Parkhurst, MaryAnn. Physicochemical Characterization of Capstone Depleted Uranium Aerosols II: Particle Size Distributions as a Function of Time. United States. doi:10.1097/01.HP.0000290613.41486.cb.
Cheng, Yung-Sung, Kenoyer, Judson L., Guilmette, Raymond A., and Parkhurst, MaryAnn. 2009. "Physicochemical Characterization of Capstone Depleted Uranium Aerosols II: Particle Size Distributions as a Function of Time". United States. doi:10.1097/01.HP.0000290613.41486.cb.
@article{osti_949878,
title = {Physicochemical Characterization of Capstone Depleted Uranium Aerosols II: Particle Size Distributions as a Function of Time},
author = {Cheng, Yung-Sung and Kenoyer, Judson L. and Guilmette, Raymond A. and Parkhurst, MaryAnn},
abstractNote = {The Capstone Depleted Uranium (DU) Aerosol Study, which generated and characterized aerosols containing depleted uranium from perforation of armored vehicles with large-caliber DU penetrators, incorporated a sampling protocol to evaluated particle size distributions. Aerosol particle size distribution is an important parameter that influences aerosol transport and deposition processes as well as the dosimetry of the inhaled particles. These aerosols were collected on cascade impactor substrates using a pre-established time sequence following the firing event to analyze the uranium concentration and particle size of the aerosols as a function of time. The impactor substrates were analyzed using beta spectrometry, and the derived uranium content of each served as input to the evaluation of particle size distributions. Activity median aerodynamic diameters (AMADs) of the particle size distributions were evaluated using unimodal and bimodal models. The particle size data from the impactor measurements was quite variable. Most size distributions measured in the test based on activity had bimodal size distributions with a small particle size mode in the range of between 0.2 and 1.2 um and a large size mode between 2 and 15 um. In general, the evolution of particle size over time showed an overall decrease of average particle size from AMADs of 5 to 10 um shortly after perforation to around 1 um at the end of the 2-hr sampling period. The AMADs generally decreased over time because of settling. Additionally, the median diameter of the larger size mode decreased with time. These results were used to estimate the dosimetry of inhaled DU particles.},
doi = {10.1097/01.HP.0000290613.41486.cb},
journal = {Health Physics, 96(3):266-275},
number = 3,
volume = 96,
place = {United States},
year = 2009,
month = 3
}
  • During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing depleted uranium were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols weremore » evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time particularly within the first minute after the shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% 30 min after perforation. In the Bradley vehicle, the initial (and maximum) uranium concentration was lower than those observed in the Abrams tank and decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in the cyclone samplers, which collected aerosol continuously for 2 h post perforation. The percentages of uranium mass in the cyclone separator stages from the Abrams tank tests ranged from 38% to 72% and, in most cases, varied with particle size, typically with less uranium associated with the smaller particle sizes. Results with the Bradley vehicle ranged from 18% to 29% and were not specifically correlated with particle size.« less
  • The impact of depleted uranium (DU) penetrators against an armored target causes erosion and fragmentation of the penetrators, the extent of which is dependent on the thickness and material composition of the target. Vigorous oxidation of the DU particles and fragments creates an aerosol of DU oxide particles and DU particle agglomerations combined with target materials. Aerosols from the Capstone DU aerosol study, in which vehicles were perforated by DU penetrators, were evaluated for their oxidation states using X-ray diffraction (XRD) and particle morphologies using scanning electron microscopy/energy dispersive spectrometry (SEM/EDS). The oxidation state of a DU aerosol is importantmore » as it offers a clue to its solubility in lung fluids. The XRD analysis showed that the aerosols evaluated were a combination primarily of U3O8 (insoluble) and UO3 (relatively more soluble) phases, though intermediate phases resembling U4O9 and other oxides were prominent in some samples. Analysis of particle residues in the micrometer-size range by SEM/EDS provided microstructural information such as phase composition and distribution, fracture morphology, size distribution, and material homogeneity. Observations from SEM analysis show a wide variability in the shapes of the DU particles. Some of the larger particles appear to have been fractured (perhaps as a result of abrasion and comminution); others were spherical, occasionally with dendritic or lobed surface structures. Amorphous conglomerates containing metals other than uranium were also common, especially with the smallest particle sizes. A few samples seemed to contain small chunks of nearly pure uranium metal, which were verified by EDS to have a higher uranium content exceeding that expected for uranium oxides. Results of the XRD and SEM/EDS analyses were used in other studies described in this issue of The Journal of Health Physics to interpret the results of lung solubility studies and in selecting input parameters for dose assessments.« less
  • The Capstone Depleted Uranium (DU) Aerosol Characterization and Risk Assessment Study was conducted to generate data about DU aerosols generated during the perforation of armored combat vehicles with large-caliber DU penetrators, and to apply the data in assessments of human health risks to personnel exposed to these aerosols, primarily through inhalation, during the 1991 Gulf War or in future military operations. The Capstone study consisted of two components: 1) generating, sampling and characterizing DU aerosols by firing at and perforating combat vehicles and 2) applying the source-term quantities and characteristics of the aerosols to the evaluation of doses and risks.more » This paper reviews the background of the study including the bases for the study, previous reviews of DU particles and health assessments from DU used by the U.S. military, the objectives of the study components, the participants and oversight teams, and the types of exposures it was intended to evaluate. It then discusses exposure scenarios used in the dose and risk assessment and provides an overview of how the field tests and dose and risk assessments were conducted.« less
  • Assessment of the health risk from exposure to aerosols of depleted uranium (DU) is an important outcome of the Capstone aerosol studies that established exposure ranges to personnel in armored combat vehicles perforated by DU munitions. Although the radiation exposure from DU is low, there is concern that DU deposited in the body may increase cancer rates. Radiation doses to various organs of the body resulting from the inhalation of DU aerosols measured in the Capstone studies were calculated using International Commission on Radiological Protection (ICRP) models. Organs and tissues with the highest calculated committed equivalent 50-yr doses were lungmore » and extrathoracic tissues (nose and nasal passages, pharynx, larynx, mouth and thoracic lymph nodes). Doses to the bone surface and kidney were about 5 to 10% of the doses to the extrathoracic tissues. The methodologies of the ICRP International Steering Committee on Radiation Standards (ISCORS) were used for determining the whole body cancer risk. Organ-specific risks were estimated using ICRP and U.S. Environmental Protection Agency (EPA) methodologies. Risks for crewmembers and first responders were determined for selected scenarios based on the time interval of exposure and for vehicle and armor type. The lung was the organ with the highest cancer mortality risk, accounting for about 97% of the risks summed from all organs. The highest mean lifetime risk for lung cancer for the scenario with the longest exposure time interval (2 h) was 0.42%. This risk is low compared with the natural or background risk of 7.35%. These risks can be significantly reduced by using an existing ventilation system (if operable) and by reducing personnel time in the vehicle immediately after perforation.« less
  • The methods used to calculate radiological and toxicological doses to hypothetical persons inside either a United States Army Abrams tank or Bradley Fighting Vehicle that has been perforated by depleted uranium munitions is described. Data from time- and particle-size-resolved measurements of depleted uranium aerosol as well as particle-size resolved measurements of aerosol solubility in lung fluids for aerosol produced in the breathing zones of the hypothetical occupants were used. The aerosol was approximated as a mixture of nine monodisperse (single particle size) components corresponding to particle size increments measured by the eight stages plus backup filter of the cascade impactorsmore » used. A Markov Chain Monte Carlo Bayesian analysis technique was employed, which straightforwardly calculates the uncertainties in doses. Extensive quality control checking of the various computer codes used is described.« less