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At least 19 records

International challenge to predict the impact of radioxenon releases from medical isotope production on a comprehensive nuclear test ban treaty sampling station

Abstract The International Monitoring System (IMS) is part of the verification regime for the Comprehensive Nuclear-Test-Ban-Treaty Organization (CTBTO). At entry-into-force, half of the 80 radionuclide stations will be able to measure concentrations of several radioactive xenon isotopes produced in nuclear explosions, and then the full network may be populated with xenon monitoring afterward (Bowyer et al., 2013). Fission-based production of 99Mo for medical purposes also releases radioxenon isotopes to the atmosphere (Saey, 2009). One of the ways to mitigate the effect of emissions from medical isotope production is the use of stack monitoring data, if it were available, so that the effect of radioactive xenon emissions could be subtracted from the effect from a presumed nuclear explosion, when detected at an IMS station location. To date, no studies have addressed the impacts the time resolution or data accuracy of stack monitoring data have on predicted concentrations at an IMS station location. Recently, participants from seven nations used atmospheric transport modeling to predict the time-history of 133Xe concentration measurements at an IMS station in Germany using stack monitoring data from a medical isotope production facility in Belgium. Participants received only stack monitoring data and used the atmospheric transport model and meteorological data of their choice. Some of the models predicted the highest measured concentrations quite well (a high composite statistical model comparison rank or a small mean square error with the measured values). The results suggest release data on a 15 min time spacing is best. The model comparison rank and ensemble analysis suggests that combining multiple models may provide more accurate predicted concentrations than any single model. Further research is needed to identify optimal methods for selecting ensemble members and those methods may depend on the specific transport problem. None of the submissions based only on the stack monitoring data predicted the small measured concentrations very well. The one submission that best predicted small concentrations also included releases from nuclear power plants. Modeling of sources by other nuclear facilities with smaller releases than medical isotope production facilities may be important in discriminating those releases from releases from a nuclear explosion.

133Xe↗

Optimization of LANSCE proton beam performance for isotope production

The LANSCE Isotope Production Facility (IPF) utilizes a 100-MeV proton beam with average power of 23 kW for isotope production in the fields of medicine, nuclear physics, national security, environmental science and industry. Typical tolerable fractional beam loss in the 100-MeV beamline is 4 x 10 -3 . Experimental beam study was made to minimize the beam losses. Adjustments to the ion source’s extraction voltage resulted in the removal of tails in phase space. Beam based steering in beamlines led to the reduction of beam emittance growth. Readjustment of the 100-MeV quadrupole transport resulted in the elimination of excessive beam envelope oscillations and removed significant parts of the beam halo at the target. Careful beam matching in the drift tube linac (DTL) provided high beam capture (75%) in the DTL. Finally, after improvements, beam losses in the 100-MeV beamline were reduced by an order of magnitude and reached the fractional level of 5 x 10 -4 .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Novel design and diagnostics improvements for increased production capacity and improved reliability at the Los Alamos Isotope Production Facility

The Isotope Production Facility (IPF) at Los Alamos National Laboratory (LANL) is used to produce an array of isotopes for medical, global security, and research applications with an intense beam of protons supplied by the linear accelerator at the Los Alamos Neutron Science Center (LANSCE). An Accelerator Improvement Project (AIP) was recently conducted at IPF to improve facility reliability and reduce programmatic risk while increasing general isotope production capacity and flexibility. This was accomplished through the installation of an improved beam window assembly, more robust beam diagnostics, an active and adjustable collimator, and a new beam rastering system. This paper will highlight the four exciting innovations and how they were designed, validated, and installed in parallel as well as the significant operational advantages they provide to IPF. Key experiments and the increased currents achieved in routine production runs demonstrating the enhanced capability from the AIP will be presented. As a result, the most notable capability enhancements include irradiations with beam currents ranging from 100 nA experimental runs up to 300 μA on routine production targets and utilization of a range of cylindrical target diameters.

100 MeV protons↗

SRF Resonators for a bi-directional Energy Ramping Upgrade of the Isotope Production Facility Beamline at LANL

The LANL Isotope Production Facility (IPF) is one of the two high-current proton linear accelerators operated under the auspices of the DOE Office of Nuclear Physics Isotope Development and Production for Research Applications Program. The IPF beamline operates with a fixed 100-MeV energy proton beam, diverted from the LANSCE accelerator and guided towards the isotope production target station. The fixed beam energy limits the number of isotopes that can be produced at IPF, and adversely affects the purity of isotopes produced at non-optimal energies. In particular, the IPF program is receiving increasing numbers of requests for high purity isotopes such as Np-236 (national security applications) and Re-186 (medical therapy). These are typically produced via (p,n) and (p,2n) nuclear reactions, requiring very tight control of the incident energies on the production targets to ensure an end product with a high radionuclidic purity. It is well known that this level of energy control cannot be achieved when a 100 MeV beam of mono-energetic protons is degraded to the required energies, typically below 30 MeV, as too much energy spread is acquired. Operating the IPF beamline at lower, mono-energetic beam energies such as at 40 MeV will allow the required tight energy control in target assemblies to ensure a high purity product. In addition, NP has requested a LANL/BNL/ORNL collaboration focus on establishing a national large-scale production capability for the therapy isotope Ac-225. Recent nuclear cross section measurements done at LANL show that due to a steep rise in production cross section towards higher proton energies (See Figure 2), proton beams at energies substantially greater than 100 MeV will be highly beneficial for Ac-225 production [AC255]. Such higher-energy beams cannot be delivered to IPF at present. Lower-energy beams (70 MeV and 40 MeV) can be delivered but only in sole-use mode; all other LANSCE users must be offline during 70 MeV or 40 MeV operation.

07 ISOTOPE AND RADIATION SOURCES↗

Development of experimental and computational frameworks to predict subcooled flow boiling in the LANL Isotope Production Facility

Cooling is crucial to maintain the integrity of target systems in isotope production facilities. At Los Alamos National Laboratory (LANL)’s Isotope Production Facility (IPF), multiple encapsulated targets are stacked and irradiated in tandem with a 100 MeV, ~250μA proton beam. To facilitate effective heat removal, these stacked targets are separated and cooled via a series of water channels. At these beam currents, this high-energy proton beam heats the target system, likely initiating subcooled flow boiling in the cooling channels. However, in-beam monitoring of the IPF target system is not possible due to the extreme radiation environment, and the necessarily significant shielding. To better understand high-power target performance, we developed ex-situ experimental and computational frameworks to predict the behavior of subcooled flow boiling at IPF. Subcooled flow boiling experiments on Inconel 625 samples under IPF conditions (2 bar pressure, 10 GPM flow rate (i.e., 2249 kg/m 2 /s), 85 K subcooling) revealed that IPF's average operating power is at the early stage of boiling with a heat transfer coefficient of 48,000 W/m 2 /s. The proposed modeling framework enables us to predict a complete boiling curve, i.e., single-phase heat transfer, onset of nucleate boiling, two-phase heat transfer, and critical heat flux (CHF), with specification of input boiling parameters up to intermediate heat flux levels. The estimated CHF under IPF conditions is 5.2 MW/m 2 . Experimental data under reduced conditions (2 bar pressure, 1.5 GPM flow rate (i.e., 337 kg/m 2 /s), 45 K subcooling) served as validation cases for the computational modeling. This computational model can be further extended to more complicated systems replicating the real IPF configuration, for instance, to study void distribution as a function of the incident proton beam profile and coolant velocity profile of multiple cooling channels. Finally, the proposed experimental and computational frameworks provide a means to better understand cooling systems in the isotope production facilities at different accelerators, where in-beam monitoring of the cooling process is not available.

07 ISOTOPE AND RADIATION SOURCES↗

Medical Isotope Production Analyses In KIPT Neutron Source Facility

Medical isotope production analyses in Kharkov Institute of Physics and Technology (KIPT) neutron source facility were performed to include the details of the irradiation cassette and the self-shielding effect. An updated detailed model of the facility was used for the analyses. The facility consists of an accelerator-driven system (ADS), which has a subcritical assembly using low-enriched uranium fuel elements with a beryllium-graphite reflector. The beryllium assemblies of the reflector have the same outer geometry as the fuel elements, which permits loading the subcritical assembly with different number of fuel elements without impacting the reflector performance. The subcritical assembly is driven by an external neutron source generated from the interaction of 100-kW electron beam with a tungsten target. The facility construction was completed at the end of 2015, and it is planned to start the operation during the year of 2016. It is the first ADS in the world, which has a coolant system for removing the generated fission power. Argonne National Laboratory has developed the design concept and performed extensive design analyses for the facility including its utilization for the production of different radioactive medical isotopes. 99 Mo is the parent isotope of 99m Tc, which is the most commonly used medical radioactive isotope. Detailed analyses were performed to define the optimal sample irradiation location and the generated activity, for several radioactive medical isotopes, as a function of the irradiation time.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Source Term Estimates of Radioxenon Released from the BaTek Medical Isotope Production Facility Using External Measured Air Concentrations

Abstract Batan Teknologi (BaTek) operates an isotope production facility in Serpong, Indonesia that supplies 99mTc for use in medical procedures. Atmospheric releases of Xe-133 in the production process at BaTek are known to influence the measurements taken at the closest stations of the International Monitoring System (IMS). The purpose of the IMS is to detect evidence of nuclear explosions, including atmospheric releases of radionuclides. The xenon isotopes released from BaTek are the same as those produced in a nuclear explosion, but the isotopic ratios are different. Knowledge of the magnitude of releases from the isotope production facility helps inform analysts trying to decide whether a specific measurement result came from a nuclear explosion. A stack monitor deployed at BaTek in 2013 measured releases to the atmosphere for several isotopes. The facility operates on a weekly cycle, and the stack data for June 15-21, 2013 show a release of 1.84E13 Bq of Xe-133. Concentrations of Xe-133 in the air are available at the same time from a xenon sampler located 14 km from BaTek. An optimization process using atmospheric transport modeling and the sampler air concentrations produced a release estimate of 1.88E13 Bq. The same optimization process yielded a release estimate of 1.70E13 Bq for a different week in 2012. The stack release value and the two optimized estimates are all within 10 percent of each other. Weekly release estimates of 1.8E13 Bq and a 40 percent facility operation rate yields a rough annual release estimate of 3.7E13 Bq of Xe-133. This value is consistent with previously published estimates of annual releases for this facility, which are based on measurements at three IMS stations. These multiple lines of evidence cross-validate the stack release estimates and the release estimates from atmospheric samplers.

atmospheric modeling↗

Search for New Isotope Production Pathways

The isotope group at Jefferson Lab is carrying out R&D for producing medically interesting radioisotopes, especially those with theranostic (therapeutic and diagnostic) attributes. Here the search for viable production mechanisms has been expanded to multi-step reactions where a daughter is produced from the target and decays into a medically interesting granddaughter radioisotope. It is difficult to find efficient production routes when investigating both the initial excitation reaction as well as the decay routes leading to medically interesting isotopes. The overall goal of this project is to create a structured code in Python to find these decay routes by automatically exploring the large number of isotopes and their possible decay modes. The program structure is described, and preliminary results are presented.

Dabill, L.↗

Isotope Production Education and Research via a Systematic Study of Photo-nuclear Reaction Yields and Excitation Functions

A new collaboration between the New Mexico Institute of Mining and Technology, Idaho State University, and Idaho National Laboratory builds the domestic workforce in isotope production and related science and technologies by conducting research and education programs related to photo-nuclear reactions. Workforce development was identified by the Department of Energy’s Office of Science in the Reaching a New Energy Sciences Workforce (RENEW) program that seeks to engage underrepresented university students in isotope production activities. This collaboration includes coursework development, student training, and isotope production research utilizing photo-nuclear reactions at electron linear accelerators. Bremsstrahlung-weighted excitation functions and cross-sections will be measured and the use of nanomaterials to exploit kinematic recoil reactions will be investigated. Students will be hosted at the Idaho National Laboratory where mentors will provide opportunities to explore careers in nuclear science and technology. This presentation regards the ongoing progress of the research and education objectives of the collaboration that was performed under the Office of Science Isotopes Program under award number D000-22-2765.

07 ISOTOPE AND RADIATION SOURCES↗

Characterizing secondary neutrons at BLIP for isotope production applications

Fast secondary neutrons created at the Brookhaven Linac Isotope Producer (BLIP) facility following proton irradiation were characterized by the foil activation technique and compared with FLUKA Monte Carlo simulations. The FLUKA-simulated neutron flux was spectrally adjusted following the maximum entropy formalism using the International Reactor Dosimetry and Fusion File (IRDFF-II), with predictions agreeing with experimental measurements to within 9 % following the adjustment procedure. Here, a multitude of degrader configurations were simulated to assess the feasibility of improving the fast (E n > 20 MeV) secondary neutron yield at the proposed neutron target position (“N-slot”). A configuration where the N-slot is closest to the proton degrader produced the highest fast neutron yield, with tungsten degraders achieving the best performance. Assuming the optimized target-degrader configuration proposed in this work, we discuss potential isotope production opportunities with secondary neutrons. In most cases the yields are in the order of several mCi.

07 ISOTOPE AND RADIATION SOURCES↗

Sensitivity Studies and Experimental Evaluation for Optimizing Transcurium Isotope Production

This work applies to recent initiatives at the Radiochemical Engineering Development Center at Oak Ridge National Laboratory to optimize the production of transcurium isotopes in the High Flux Isotope Reactor in such a way as to prolong the use of high quality heavy curium feedstock. By studying the sensitivity of fission and transmutation reaction rates to the neutron flux spectrum a means of increasing the fraction of (n,γ) reactions per neutron absorption is explored. Filter materials which preferentially absorb neutrons at energies considered detrimental to optimal transcurium production are identified and transmutation rates are examined with high energy resolution. Experimental capsules are irradiated employing filter materials and the resulting fission and activation products studied to validate the filtering methodology. Improvement is seen in the production efficiency of heavier curium isotopes in 244 Cm and 245 Cm targets, and potentially in production of 252 Cf from mixed californium targets. Finally, further analysis is recommended to evaluate longer duration irradiations more representative of typical transcurium production.

07 ISOTOPE AND RADIATION SOURCES↗

Electron linac for medical isotope production with improved energy efficiency and isotope recovery

A method and isotope linac system are provided for producing radio-isotopes and for recovering isotopes. The isotope linac is an energy recovery linac (ERL) with an electron beam being transmitted through an isotope-producing target. The electron beam energy is recollected and re-injected into an accelerating structure. The ERL provides improved efficiency with reduced power requirements and provides improved thermal management of an isotope target and an electron-to-x-ray converter.

07 ISOTOPE AND RADIATION SOURCES↗

Isotope Production for UK PhD Student Visit [Slides]

Overview of INL isotope production work, including organizational structures, the current work and future plans of plutonium fuel supplies, cobalt-60 production, and BRR cask shipping.

07 ISOTOPE AND RADIATION SOURCES↗

Real-time Stack Monitoring at the BaTek Medical Isotope Production Facility

Radioxenon emissions from radiopharmaceutical production are a major source of background concentrations affecting the radioxenon detection systems of the International Monitoring System (IMS). Collection of real-time emissions data from production facilities makes it possible to screen out some medical isotope signatures from the IMS radioxenon data sets. This paper describes an effort to obtain and analyze real-time stack emissions data with the design, construction and installation of a small stack monitoring system developed by a joint CTBTO-IDC, BATAN, and PNNL team at the BaTek medical isotope production facility near Jakarta, Indonesia.

CTBTO↗

Short-lived photofission product yields from 238 U and 232 Th at Bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV for nuclear forensics isotope production applications

The existing photofission product yield data sets are often based on nuclear models, and limited experimental measurements of these fission product yields have been performed. These experiments resulted in measured cumulative fission product yields (CFPYs) for 238 U and 232 Th for the bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV. The half-lives of the reported fission products range from 1.07–40.8 s. This work is motivated by a demonstrated need for novel isotope production methods for nuclear forensics and improved nuclear data to support the nonproliferation community. A high-purity germanium detector and a pneumatic transfer system were employed for measurements of short-lived fission products, collecting data between cycles of accelerator irradiation and measurement.

07 ISOTOPE AND RADIATION SOURCES↗

Production of 230 Pa by proton irradiation of 232 Th at the LANL isotope production facility: Precursor of 230 U for targeted alpha therapy

Uranium-230 ( t 1/2 = 20.8 d) is an alpha-emitting radionuclide that has potential application in targeted alpha therapy (TAT) of cancer. Its parent isotope 230 Pa ( t 1/2 = 17.4 d), can be produced by proton irradiation of thorium metal targets. Preliminary 230 Pa production runs were performed at the Los Alamos National Laboratory Isotope Production Facility (LANL-IPF) using thin thorium metal targets and a proton beam energy of 15–30 MeV, followed by radiochemical separation of 230 Pa from the irradiated target matrix. The measured 230 Pa production yields were found to exceed the predicted values in most of the experiments that were performed. Furthermore, this data will inform further production efforts for providing 230 Pa/ 230 U for clinical trials.

07 ISOTOPE AND RADIATION SOURCES↗