Renal and Intestinal Excretion of 90Y and 166Ho After Transarterial Radioembolization of Liver Tumors.

OBJECTIVE. The aim of this study was to evaluate the amount of free radioactivity in renal and intestinal excretions during the first 48 hours after transarterial radioembolization (TARE) procedures on the liver. SUBJECTS AND METHODS. Urinary, intestinal, and biliary excretions of patients who underwent TARE with three different types of microspheres were collected during a postinterventional period of 48 hours (divided into two 24-hour intervals). Radioactivity measurements were performed. The detected amounts of activity were correlated to clinical and procedural characteristics, times of excretion, and microsphere types. RESULTS. Twenty-four patients were evaluated, 10 treated with 90Y-glass, 10 with 90Y-resin, and four with 166Ho-poly-L-lactic acid (PLLA) microspheres. Activity excretion occurred in all cases. The highest total excretion proportions of the injected activities were 0.011% for 90Y-glass, 0.119% for 90Y-resin, and 0.005% for 166Ho-PLLA microspheres. Intestinal excretion was markedly less than renal excretion (p < 0.001). Excretion after TARE with 90Y-resin was statistically significantly higher than with 90Y-glass or 166Ho-PLLA micro-spheres (p = 0.002). For each microsphere type, the excreted activity was independent of the activity of the injected microspheres. CONCLUSION. Renal and intestinal excretion of radioactivity after TARE is low but not negligible. The radiation risk for individuals interacting with patients can be minimized if contact with urine and bile is avoided, particularly during the first 24 hours after the procedure.

Bioassay and alpha spectrometry in indirect monitoring of Spanish workers exposed to enriched uranium.

Workers at risk of exposure to uranium compounds should be monitored and their internal exposure quantified in terms of committed effective dose E(50) in mSv. In vitro bioassay methods can quantify uranium in urine and faeces at low activity levels. Alpha spectrometry (AS) is the most common method used for monitoring alpha-emitting radionuclides in internal dosimetry services. It provides isotopic information and low minimum detectable activity (MDA) values (≤0.50 mBq per sample). This study reports the results of a five-year monitoring of workers exposed to uranium at a Spanish Juzbado facility, which produces nuclear fuel elements enriched with up to 5 % of 235U. Monitoring included about 100 workers per year, most of whom had worked at the facility for more than 10 years before the individual monitoring programme was established. We analysed nearly 550 samples of more than 200 workers over five years. The obtained results indicate that workers were adequately protected from uranium exposure through inhalation and had an acceptably low chronic intake at the facility.

Simultaneous Determination of Uranium and Depleted Uranium Isotopic Ratio Using Inductively Coupled Mass Spectrometry.

We have developed and validated a method for the simultaneous quantitative measurement of total uranium (TU) and uranium 235 U/238 U isotopic ratio (UIR) in urine by inductively coupled plasma mass spectrometry (ICP-MS) using a Thermo Scientific iCAP-Q instrument. The performance characteristics of the assay were determined to be in compliance with clinical laboratory standards. The assay was linear in the concentration range of 1.0 to 500.0 ng/liter TU. The method was precise and accurate with limits of detection of 2.5 ng/liter for TU and 9.8 ng/liter for UIR. The accuracy was >93% and the coefficient of variation (% CV) was <5.0% for both TU and UIR. All results were within established guidelines and agreed-upon criteria, and the results fell within the certified range for the reference controls. The method has thus been shown to be effective as a simple, precise, and sensitive analytical technique for testing urine samples. © 2018 by John Wiley & Sons, Inc.

Evaluation of in vivo and in vitro dose detection limits for different radionuclides and measurement techniques.

Personal monitoring programs for workers handling radioactive materials are influenced by numerous factors as the measurements of radioactivity in tissues or/and in excreta can be carried out using different techniques. This paper summaries the basic procedures needed for accurate and fast measurement of different radionuclides like (235)U, (234)U, (238)U, (226)Ra, (210)Po, (131)I, (99m)Tc, (134)Cs, (137)Cs, (57)Co, (58)Co, and (60)Co. Overviews of in vitro and in vivo monitoring methods are provided as well as methods used to calculate detection limits and internal radiation dose. For the radionuclides of interest, in vivo and in vitro detection limits were converted into committed effective doses to evaluate the applicability and limitations of the systems used at the laboratory. The results proved that the systems' sensitivity is suitable for use in routine monitoring of workers subject to risk of internal exposure from such radionuclides. Consequently, monitoring programs suggested by the Syrian internal dosimetry laboratory are suitable to detect committed effective doses even below 1mSv in most cases.

Excreta Sampling as an Alternative to In Vivo Measurements at the Hanford Site.

The capabilities of indirect radiobioassay by urine and fecal sample analysis were compared with the direct radiobioassay methods of whole body counting and lung counting for the most common radionuclides and inhalation exposure scenarios encountered by Hanford workers. Radionuclides addressed by in vivo measurement included 137Cs, 60Co, 154Eu, and 241Am as an indicator for plutonium mixtures. The same radionuclides were addressed using gamma energy analysis of urine samples, augmented by radiochemistry and alpha spectrometry methods for plutonium in urine and fecal samples. It was concluded that in vivo whole body counting and lung counting capability should be maintained at the Hanford Site for the foreseeable future, however, urine and fecal sample analysis could provide adequate, though degraded, monitoring capability for workers as a short-term alternative, should in vivo capability be lost due to planned or unplanned circumstances.

Determination of 234U/238U, 235U/238U and 236U/238U isotope ratios in urine using sector field inductively coupled plasma mass spectrometry.

Quantification of the isotopic composition of uranium in urine at low levels of concentration is important for assessing both military and civilian populations' exposures to uranium. However, until now there has been no convenient, precise method established for rapid determination of multiple uranium isotope ratios. Here, the authors report a new method to measure (234)U/(238)U, (235)U/(238)U and (236)U/(238)U. It uses solid-phase chelation extraction (via TRU columns) of actinides from the urine matrix, followed by measurement using a magnetic sector field inductively coupled plasma mass spectrometer (SF-ICP-MS-Thermo Element XR) equipped with a high-efficiency nebulizer (Apex PFA microflow) and coupled with a membrane desolvating nebulizer system (Aridus II™). This method provides rapid and reliable results and has been used successfully to analyse Certified Reference Materials.

[Interest and limits of inductively coupled plasma mass spectrometry (ICP-MS) for urinary diagnosis of radionuclide internal contamination]. / Intérêt et limites du couplage plasma induit par haute fréquence - spectrométrie de masse (ICP-MS) pour le diagnostic urinaire d'une contamination interne par un radionucléide.

After a review of radiometric reference methods used in radiotoxicology, analytical performance of inductively coupled plasma mass spectrometry (ICP-MS) for the workplace urinary diagnosis of internal contamination by radionuclides are evaluated. A literature review (covering the period from 2000 to 2012) is performed to identify the different applications of ICP-MS in radiotoxicology for urine analysis. The limits of detection are compared to the recommendations of the International commission on radiological protection (ICRP 78: "Individual monitoring for internal exposure of workers"). Except one publication describing the determination of strontium-90 (ß emitter), all methods using ICP-MS reported in the literature concern actinides (α emitters). For radionuclides with a radioactive period higher than 10(4) years, limits of detection are most often in compliance with ICRP publication 78 and frequently lower than radiometric methods. ICP-MS allows the specific determination of plutonium-239 + 240 isotopes which cannot be discriminated by α spectrometry. High resolution ICP-MS can also measure uranium isotopic ratios in urine for total uranium concentrations lower than 20 ng/L. The interest of ICP-MS in radiotoxicology concerns essentially the urinary measurement of long radioactive period actinides, particularly for uranium isotope ratio determination and 239 and 240 plutonium isotopes discrimination. Radiometric methods remain the most efficient for the majority of other radionuclides.

Toxicity of irradiated advanced heavy water reactor fuels.

The good neutron economy and online refueling capability of the CANDU® heavy water moderated reactor (HWR) enable it to use many different fuels such as low enriched uranium (LEU), plutonium, or thorium, in addition to its traditional natural uranium (NU) fuel. The toxicity and radiological protection methods for these proposed fuels, unlike those for NU, are not well established. This study uses software to compare the fuel composition and toxicity of irradiated NU fuel against those of two irradiated advanced HWR fuel bundles as a function of post-irradiation time. The first bundle investigated is a CANFLEX® low void reactor fuel (LVRF), of which only the dysprosium-poisoned central element, and not the outer 42 LEU elements, is specifically analyzed. The second bundle investigated is a heterogeneous high-burnup (LEU,Th)O(2) fuelled bundle, whose two components (LEU in the outer 35 elements and thorium in the central eight elements) are analyzed separately. The LVRF central element was estimated to have a much lower toxicity than that of NU at all times after shutdown. Both the high burnup LEU and the thorium fuel had similar toxicity to NU at shutdown, but due to the creation of such inhalation hazards as (238)Pu, (240)Pu, (242)Am, (242)Cm, and (244)Cm (in high burnup LEU), and (232)U and (228)Th (in irradiated thorium), the toxicity of these fuels was almost double that of irradiated NU after 2,700 d of cooling. New urine bioassay methods for higher actinoids and the analysis of thorium in fecal samples are recommended to assess the internal dose from these two fuels.

Reliability of a new biokinetic model of zirconium in internal dosimetry: part I, parameter uncertainty analysis.

The reliability of biokinetic models is essential in internal dose assessments and radiation risk analysis for the public, occupational workers, and patients exposed to radionuclides. In this paper, a method for assessing the reliability of biokinetic models by means of uncertainty and sensitivity analysis was developed. The paper is divided into two parts. In the first part of the study published here, the uncertainty sources of the model parameters for zirconium (Zr), developed by the International Commission on Radiological Protection (ICRP), were identified and analyzed. Furthermore, the uncertainty of the biokinetic experimental measurement performed at the Helmholtz Zentrum München-German Research Center for Environmental Health (HMGU) for developing a new biokinetic model of Zr was analyzed according to the Guide to the Expression of Uncertainty in Measurement, published by the International Organization for Standardization. The confidence interval and distribution of model parameters of the ICRP and HMGU Zr biokinetic models were evaluated. As a result of computer biokinetic modelings, the mean, standard uncertainty, and confidence interval of model prediction calculated based on the model parameter uncertainty were presented and compared to the plasma clearance and urinary excretion measured after intravenous administration. It was shown that for the most important compartment, the plasma, the uncertainty evaluated for the HMGU model was much smaller than that for the ICRP model; that phenomenon was observed for other organs and tissues as well. The uncertainty of the integral of the radioactivity of Zr up to 50 y calculated by the HMGU model after ingestion by adult members of the public was shown to be smaller by a factor of two than that of the ICRP model. It was also shown that the distribution type of the model parameter strongly influences the model prediction, and the correlation of the model input parameters affects the model prediction to a certain extent depending on the strength of the correlation. In the case of model prediction, the qualitative comparison of the model predictions with the measured plasma and urinary data showed the HMGU model to be more reliable than the ICRP model; quantitatively, the uncertainty model prediction by the HMGU systemic biokinetic model is smaller than that of the ICRP model. The uncertainty information on the model parameters analyzed in this study was used in the second part of the paper regarding a sensitivity analysis of the Zr biokinetic models.

PROCORAD's proficiency tests as a means of analyzing capacities in emergency situations.

Beyond the metrological evaluation indispensable to prove objectively the capability of a medical laboratory to perform analysis, the comparison of analytical performances regarding the specificity, rapidity and trueness of the available methods is a real interest of international comparison exercises. The objective of this paper is to present and discuss the main results of proficiency testing organized by PROCORAD in the radiobioassay field illustrated by exercises for in vitro "surprise" analysis when no information is available on the nuclides involved, which can be the case in an emergency situation.

Laboratory evaluation of a SpectraMax microplate reader and test strips for field measurement of creatinine in spot urine samples in the event of a radiological accident.

The fear that terrorists might use radiological or nuclear (RN) devices to attack others is a new but growing phenomenon, arising mainly from the events of 11 September 2001. Research on rapid analytical methods that can allow analyses of large numbers of people who may become internally contaminated with radionuclides due to a RN accident is still limited. To contribute to this bioassay capacity for emergency response, the Radiation Protection Bureau of Health Canada has identified and evaluated two new portable SpectraMax plate readers (model 250 and Plus 384) and one brand of dry reagent strips for rapid measurement of creatinine in spot urine samples. Concentrations of creatinine in spot urine samples provide a means of adjusting or normalizing urine collections to 24 h, upon which accurate internal dose assessments due to the radionuclides can be made. Preliminary test results of the devices showed the two SpectraMax plate readers and the TECO dry creatinine reagent strips were portable, rapid and reliable for urinary creatinine measurements in spot samples, suggesting they can be used in rapid dose screening of people.

Analysis of urine for pure beta emitters: methods and application.

Bioassay for individual radionuclides is an essential and first step in estimation of radiation risk to nuclear facilities workers and people who are exposed to the contaminated environment in the event of a nuclear accident or radiological attack. Urine is a frequently used biological sample for this purpose. Tritium and (14)C are important radionuclides for workers in nuclear reactors and radiopharmaceutical laboratories. A method for the determination of tritium and (14)C in organic and inorganic forms in urine has been developed. It involves activated charcoal absorption of organic matter followed by combustion to separate tritiated water from organically-bound tritium. Inorganic (14)C from organically-bound (14)C, the separated tritium and (14)C were measured using liquid scintillation counting. Iodine-129, a long-lived beta emitter, is normally released to the atmosphere during the operation of nuclear facilities, especially in reprocessing plants. The high concentration of iodine in the thyroid makes this radionuclide an important source of exposure to exposed populations. A simple method has been developed in this work for the determination of (129)I in urine by anion exchange preconcentration, extraction purification and liquid scintillation counting. Using accelerator mass spectrometry, urine samples can be analyzed for low level (129)I in both organic and inorganic forms after active charcoal adsorption and solvent extraction separation. Condensed water collected daily from the reactor hall in a Danish research reactor and monthly urine samples from the staff working in the reactor building were collected from 2003-2010 and analyzed using this method, and the results are presented and discussed.

Rapid urinary output normalization method using specific gravity.

Spot urine samples are often taken for emergency radiobioassay to provide a quick dose assessment for contaminated individuals. The subsequent dosimetric analysis requires a urinary output normalization method to adjust spot sampling to daily urine excretion. A rapid specific gravity method that was developed for 24-h urinary output correction is described. Spot urine samples were collected from volunteers of different race, gender, and age to validate the normalization method. Results show that a specific gravity test is a fast, easy and robust method to correct the urine excretion in the event of a radiation emergency.

Investigation of magnetic nanoparticles for the rapid extraction and assay of alpha-emitting radionuclides from urine: demonstration of a novel radiobioassay method.

In the event of an accidental or intentional release of radionuclides into a populated area, massive numbers of people may require radiobioassay screening as triage for dose-reduction therapy or identification for longer-term follow-up. If the event released significant levels of beta- or alpha-emitting radionuclides, in vivo assays would be ineffective. Therefore, highly efficient and rapid analytical methods for radionuclide detection from submitted spot urine samples (≤50 mL) would be required. At present, the quantitative determination of alpha-emitting radionuclides from urine samples is highly labor intensive and requires significant time to prepare and analyze samples. Sorbent materials that provide effective collection and enable rapid assay could significantly streamline the radioanalytical process. The authors have demonstrated the use of magnetic nanoparticles as a novel method of extracting media for four alpha-emitting radionuclides of concern (polonium, radium, uranium and americium) from chemically-unmodified and pH-2 human urine. Herein, the initial experimental sorption results are presented along with a novel method that uses magnetic nanoparticles to extract radionuclides from unmodified human urine and then collect the magnetic field-induced particles for subsequent alpha-counting-source preparation. Additionally, a versatile human dose model is constructed that determines the detector count times required to estimate dose at specific protective-action thresholds. The model provides a means to assess a method's detection capabilities and uses fundamental health physics parameters and actual experimental data as core variables. The modeling shows that, with effective sorbent materials, rapid screening for alpha-emitters is possible with a 50-mL urine sample collected within 1 wk of exposure/intake.

Rapid methods for the isolation of actinides Sr, Tc and Po from raw urine.

Rapid methods for the isolation and analysis of individual actinides (Th, U, Pu, Am/Cm) and Sr, Tc and Po from small volumes of raw urine have been developed. The methods involve acidification of the sample and the addition of aluminum nitrate or aluminum chloride salting-out agent prior to isolation of the desired analyte using a tandem combination of prefilter material and extraction chromatographic resin. The method has been applied to the separation of individual analytes from spiked urine samples. Analytes were recovered in high yield and radionuclide purity with separation times as low as 30 min. The chemistry employed is compatible with automation on the ARSIIe instrument.

Evaluating the performance of the ORTEC® Detective™ for emergency urine bioassay.

The performance of the ORTEC(®) Detective™ as a field deployable tool for emergency urine bioassay of (137)Cs, (60)Co, (192)Ir, (169)Yb and (75)Se was evaluated against ANSI N13.30. The tested activity levels represent 10 % RL (reference level) and 1 % RL defined by [Li C., Vlahovich S., Dai X., Richardson R. B., Daka J. N. and Kramer G. H. Requirements for radiation emergency urine bioassay techniques for the public and first responders. Health Phys (in press, 99(5), 702-707 (2010)]. The tests were conducted for both single radionuclide and mixed radionuclides at two geometries, one conventional geometry (CG) and one improved geometry (IG) which improved the MDAs (minimum detectable amounts) by a factor of 1.6-2.7. The most challenging radionuclide was (169)Yb. The measurement of the mixture radionuclides for (169)Yb at the CG did not satisfy the ANSI N13.30 requirements even at 10 % RL. At 1 % RL, (169)Yb and (192)Ir were not detectable at either geometry, while the measurement of (60)Co in the mixed radionuclides satisfied the ANSI N13.30 requirements only at the IG.

A mobile bioassay laboratory for the assessment of internal doses based on in vivo and in vitro measurements.

Internal exposures may occur in nuclear power plants, radioisotope production, and in medicine and research laboratories. Such practices require quick response in case of accidents of a wide range of magnitudes. This work presents the design and calibration of a mobile laboratory for the assessment of accidents involving workers and the population as well as for routine monitoring. The system was set up in a truck with internal dimensions of 3.30 m × 1.60 m × 1.70 m and can identify photon emitters in the energy range of 100-3,000 keV in the whole body, organs, and in urine. A thyroid monitor consisting of a lead-collimated NaI(Tl)3" × 3" (7.62 × 7.62 cm) detector was calibrated with a neck-thyroid phantom developed at the IRD (Instituto de Radioproteção e Dosimetria). Whole body measurements were performed with a NaI(Tl)8" × 4" (20.32 × 10.16 cm) detector calibrated with a plastic-bottle phantom. Urine samples were measured with another NaI(Tl) 3" × 3" (7.62 × 7.62 cm) detector set up in a steel support. Standard solutions were provided by the National Laboratory for Metrology of Ionizing Radiation of the IRD. Urine measurements are based on a calibration of efficiency vs. energy for standard volumes. Detection limits were converted to minimum committed effective doses for the radionuclides of interest using standard biokinetic and dosimetric models in order to evaluate the applicability and limitations of the system. Sensitivities for high-energy activation and fission products show that the system is suitable for use in emergency and routine monitoring of individuals under risk of internal exposure by such radionuclides.

Urinary excretion of radionuclides from Marshallese exposed to fallout from the 1954 Bravo nuclear test.

Soon after the Bravo nuclear test at Bikini Atoll in the Marshall Islands on 1 March 1954, urine samples were collected for analysis of excreted radioactivity from native residents exposed to radioactive fallout on two atolls as well as from U.S. military personnel on a third atoll. The earliest acquired samples, obtained by the Los Alamos Scientific Laboratory (LASL), were assayed for various radionuclides and provided the first known measurements of (131)I in urine following exposure to fallout from a nuclear test. Over the course of 1954, many additional samples were collected by the LASL, as well as by the Atomic Energy Commission New York Operations Office's Health and Safety Laboratory and the Naval Radiological Defense Laboratory. Collectively, the groups sampled included Marshallese exposed on Rongelap and Ailinginae Atolls, American military weather observers temporarily resident on Rongerik Atoll, and sailors from the Japanese fishing vessel, the Lucky Dragon. While the bioassay measurement data and individual urine volumes have been crucial to various attempts to assess intakes of radioactivity and the related internal radiation doses among the Marshallese, those data have never been published in any peer-reviewed journal, but have been restricted to agency memoranda, laboratory reports, and summaries in some publications and book chapters. Reconstructions of internal doses to Marshallese in 1954 and in later years have depended on these data and, hence, they have considerable historical importance as well as importance to ongoing health risk projections for Marshallese. This paper presents much of the original data on urine volumes and radioactivity from the various assays of urine for radionuclides, and compares estimates of (131)I intakes made in 1954, 1985, 1987, and 2008.

Physical aspects of scintigraphy-based dosimetry for nuclear medicine therapy.

In nuclear medicine therapy the treatment of tumours by radiation exposure from internally deposited labelled antibodies or labelled peptides is currently an active field of investigation. To permit the efficient delivery of high amounts of radiation dose to tumours while limiting the radiation dose to critical organs dosimetry calculations have to be performed. These are relying on scintigraphic data being input to the well known MIRD formalism. This paper focuses on the methods and the difficulties associated with the scintigraphic determination of organ kinetics. The physical properties of the well-known scintigraphic imaging modalities, PET, SPECT and planar scintigraphy, are discussed thereby taking into account the properties of the appropriate radionuclides currently being available for therapy and dosimetry. Several arguments are given and disputed for the limited clinical use of PET and SPECT in dosimetry and the ongoing preference of planar whole-body imaging as the method of choice. The quantitative restrictions still inherent to this method are also discussed in detail. Procedural recommendations are proposed covering all processes related to data acquisition, data correction and data analysis which finally lead to reliable estimations of organ dose.

Population monitoring for acute exposure to 210Po.

OBJECTIVE: To investigate the feasibility of using single void urine samples to monitor internal radiation exposure of first responders and large populations int he event of a radiological incident involving the intentional dispersal of 210Po. METHODS: Urinary excretion of 210Po was evaluated and organ absorbed and effective doses were calculated subsequent to an acute unit intake of 210Po. RESULTS: 210Po can be detected in single void urine samples at levels sufficient to detect effective dose below recommended limits. Minimum intakes of 210Po that would result in clinically significant effects were estimated. CONCLUSIONS: Collection and analysis of single void urine samples is adequate to identify persons who may be exposed in the event of a radiological emergency involving 210Po. Also, the first responder limit appears to be sufficiently protective to prevent clinically significant deterministic effects.