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Monte Carlo simulations demonstrating physics of equivalency of gamma, electron-beam, and X-ray for radiation sterilization
We report the sterilization of medical devices using the gamma rays from the decay of cobalt-60 has accumulated decades of experience of the performance of the materials and devices that are irradiated. The use of radiation using electron beams and x-rays has much less experience and this leads to questions of equivalency between these three technologies. Computer simulations were conducted to model the relevant physical processes of the interactions of each of the three forms of radiation in order to compare the spectra of electron energies at energies below 500 keV. It is predominantly the electrons below this threshold that produce the sterilization dose. No difference in energy spectra was seen between the three types of initial radiation. It is concluded that there is no energy dependent difference between gamma, e-beam, and x-ray for radiation sterilization.
Compatibility of ethylene vinyl acetate (EVA)/ethylene vinyl alcohol (EVOH)/EVA films with gamma, electron-beam, and X-ray irradiation
Many polymer-based medical devices are sterilized by gamma irradiation. To reduce the use of cobalt-60 gamma-ray sources, transition from gamma ray to alternative irradiation technologies was proposed, namely electron beam (e-beam) and X-ray. A major impediment for such a transition is the knowledge gap in material compatibility with the different radiation sources. In this study, multi-layer films consisting of ethylene vinyl acetate (EVA) and ethylene vinyl alcohol (EVOH) components were irradiated to target doses of 30, 45, and 60 kGy by gamma-ray, e-beam, and X-ray sources. Effects of irradiation were evaluated on 12 material properties, and statistical comparisons between gamma irradiation and alternative technologies were conducted using the two one-sided t-test (or “equivalence test”) and classic t-test. Melting temperature and UV absorbance below 300 nm showed dose dependencies, while other investigated properties such as discoloration and mechanical durability did not change with dose up to 60 kGy. Based on these results, there is no material compatibility issue associated with the transition from gamma to e-beam or to X-ray as source of sterilization radiation of the studied multi-layer film.
Radiation-Induced Effects on the Extraction Properties of Hexa-n-octylnitrilo-triacetamide (HONTA) Complexes of Americium and Europium
The candidate An(III)/Ln(III) separation ligand hexa-n-octylnitrilo-triacetamide (HONTA) was irradiated under envisioned SELECT (Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation) process conditions (n-dodecane/0.1 M HNO 3 ) using a solvent test loop in conjunction with cobalt-60 gamma irradiation. The extent of HONTA radiolysis and complimentary degradation product formation was quantified by HPLC-ESI-MS/MS. Further, the impact of HONTA radiolysis on process performance was evaluated by measuring the change in 243 Am and 154 Eu distribution ratios as a function of absorbed gamma dose. HONTA was found to decay exponentially with increasing dose, affording a dose coefficient of d = (4.48 ± 0.19) × 10 –3 kGy –1 . Multiple degradation products were detected by HPLC-ESI-MS/MS with dioctylamine being the dominant quantifiable species. Both 243 Am and 154 Eu distribution ratios exhibited an induction period of ~70 kGy for extraction (0.1 M HNO 3 ) and back-extraction (4.0 M HNO 3 ) conditions, after which both values decreased with absorbed dose. The decrease in distribution ratios was attributed to a combination of the destruction of HONTA and ingrowth of dioctylamine, which is capable of interfering in metal ion complexation. Furthermore, the loss of HONTA with absorbed gamma dose was predominantly attributed to its reaction with the n-dodecane radical cation (R˙ + ). These R˙ + reaction kinetics were measured for HONTA and its 241 Am and 154 Eu complexes using picosecond pulsed electron radiolysis techniques. All three second-order rate coefficients (k) were essentially diffusion limited in n-dodecane indicating a significant reaction pathway: k(HONTA + R˙ + ) = (7.6 ± 0.8) × 10 9 M –1 s –1 , k(Am(HONTA) 2 + R˙ + ) = (7.1 ± 0.7) × 10 10 M –1 s –1 , and k(Eu(HONTA) 2 + R˙ + ) = (9.5 ± 0.5) × 10 10 M –1 s –1 . HONTA-metal ion complexation afforded an order-of-magnitude increase in rate coefficient. Additional nanosecond time-resolved measurements showed that both direct and indirect HONTA radiolysis yielded the short-lived (< 100 ns) HONTA radical cation and a second long-lived (µs) species identified as the HONTA triplet excited state. The latter was confirmed by a series of oxygen quenching picosecond pulsed electron measurements, affording a quenching rate coefficient of k( 3 [HONTA]* + O 2 ) = 2.2 × 10 8 M –1 s –1 . Overall, both the HONTA radical cation and triplet excited state are important precursors to the suite of measured HONTA degradation products.
Effect of f -element complexation on the radiolysis of 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP])
A systematic study of the impact on the chemical reactivity of the oxidising n-dodecane radical cation (RH˙ + ) with f-element complexed 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) has been undertaken utilizing time-resolved electron pulse radiolysis/transient absorption spectroscopy and high-level quantum mechanical calculations. Lanthanide ion complexed species, [Ln((HEH[EHP]) 2 ) 3 ], exhibited vastly increased reactivity (over 10× faster) in comparison to the non-complexed ligand in n-dodecane solvent, whose rate coefficient was k = (4.66 ± 0.22) × 10 9 M -1 s -1 . Similar reactivity enhancement was also observed for the corresponding americium ion complex, k = (5.58 ± 0.30) × 10 10 M -1 s -1 . The vastly increased reactivity of these f-element complexes was not due to simple increased diffusion-control of these reactions; rather, enhanced hole transfer mechanisms for the complexes were calculated to become energetically more favourable. Interestingly, the observed reactivity trend with lanthanide ion size was not linear; instead, the rate coefficients showed an initial increase (Lu to Yb) followed by a decrease (Tm to Ho), followed by another increase (Dy to La). This behaviour was excellently predicted by the calculated reaction volumes of these complexes. In conclusion, complementary cobalt-60 gamma irradiations for select lanthanide complexes demonstrated that the measured kinetic differences translated to increased ligand degradation at steady-state timescales, affording ~38% increase in ligand loss of a 1:1 [La((HEH[EHP]) 2 ) 3 ]: HEH[EHP] ratio system.
Identification and time evolution of thionyl chloride (SOCl 2 ) radiolysis products
In this study, innovative solutions are needed to reduce the amount of high-level waste generated by used nuclear fuel recycling strategies to support the widespread adoption of sustainable nuclear fission energy technologies. To this end, a new sulfur chloride-based process has been developed to recycle zirconium alloy-based materials, which make up a significant fraction of high-level radioactive waste. To support the continued development of this process, we present new data on the potential reaction pathways over time of the products arising from the gamma and electron beam radiolysis of neat thionyl chloride (SOCl 2 ). Interrogation of the gamma irradiated liquid by Raman spectroscopy provided more conclusive identification of the SOCl 2 degradation products, specifically sulfur dichloride (SCl 2 ), molecular chlorine (Cl 2 ), sulfur dioxide (SO 2 ), and sulfuryl chloride (SO 2 Cl 2 ). In comparison, the high dose rate (~10 7 Gy s -1 ) electron beam irradiations formed significantly more degradation products. For both cobalt-60 gamma and electron beam irradiations, the observed degradation products were found to evolve as a function of time post-irradiation via the same reaction pathways, with indication of a solvent regeneration mechanism. These findings are fortuitous for process development, as such a mechanism would be beneficial for process longevity and cost effectiveness.
Drones for Decommissioning
The U.S. Nuclear Regulatory Commission has responsibility for regulating the safe decommissioning of facilities and sites to meet the License Termination Rule in 10 Code of Federal Regulations (CFR) Part 20, Standards for Protection Against Radiation, Subpart E “Radiological Criteria for License Termination.” Decommissioning is performed in accordance with 10 CFR Part 50, Domestic Licensing of Production and Utilization Facilities, as part of license termination (§50.82) and release of the facility or site for unrestricted use (§50.83). The guidance currently demonstrates the minimum requirements and necessary conditions for conducting radiological surveys by a person carrying a radiation detector(s). The Pacific Northwest National Laboratory (PNNL) evaluated the use of an unoccupied aerial vehicle (UAV) to conduct radiological surveys that could be used in decommissioning to potentially reduce time, cost, and worker safety compared to current survey methods. The objective of this project was to evaluate the performance and limitations of a UAV to support a decommissioning radiological survey and compare it to a radiological survey conducted by a human. The primary research questions of interest evaluated were: 1. Did observed UAV paths differ from human paths and, if so, how much? 2. Did survey path deviation affect survey results and, if so, how? 3. Were radiological measurements from human and UAV surveys significantly different? To answer these research questions, an experimental field was set up at PNNL’s 3440 test track, and it included radiological sources commonly surveyed during decommissioning: cobalt-60 (Co-60), cesium-137 (Cs-137), and americium-241 (Am-241). Nine check sources (three each of Am-241, Cs-137, and Co-60) with activities ranging from 3.54 µCi to 39.34 µCi were set over a path that also included an area for measuring background radiation. An Aurelia X6 UAV coupled with a GPS and lidar unit was used to conduct the radiological surveys. UAV and human surveys were conducted using two different NaI(Tl) scintillation radiation detectors (2 in. × 2 in. Ludlum, Inc. and 2 in. × 0.04 in. Alpha Spectra, Inc.) at a travel velocity of approximately 0.2 m/s at a low (15–40 cm median altitude) or high (87–105 cm median altitude) survey altitude. Since the survey velocity and altitude parameters were atypical for normal UAV operations, testing was done prior to conducting the radiological surveys to establish airworthiness, evaluate the navigation system, and establish flight control. Human and UAV surveys were paired according to the detector type and altitude regime to compare the survey data. The results of this proof-of-concept research determined that the UAV and human surveys followed similar survey paths and detected the radiological sources with no significant statistical difference (in 33 out of 36 surveys). However, further research is needed prior to deploying UAVs for decommissioning surveys.
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.
Radiation Aging of Cable Insulation Systems to Support Extension of Cable Electrical Assessment Techniques - CRADA 562 (Final Report)
Radiation aging (primarily gamma radiation) affects a small subset of the LV cable population based on a 40-year operation. Increasing plant operating life to 60 or 80 years will result in additional cables experiencing degradation, either from radiation or from combined thermal and radiation effects. Previous research work done by EPRI and other researchers focuses on electrical diagnostics of thermal effects. However, the electrical diagnostic response of the cable system to radiation aging is minimally understood. In order to study the electrical responses from XLPE and EPR cabling and correlate these responses with radiation dose and level of thermal exposure, gamma radiation testing was performed at Pacific Northwest National Laboratory (PNNL). This report covers the radiation testing performed at PNNL, which involved irradiation of 30-foot long cables and short witness samples. The cabling was irradiated, at room temperature, using cobalt-60 gamma-rays to intervals of 10 million rads (10 Mrads), for a maximum of 70 Mrads. The results can be used to determine cable conditions (extent of damage) more accurately and localize where the degradation exists along the length of the cable (axial location). These insights can provide operators with the options to focus repair, mitigation, or replacement efforts locally.
Effects of X-Rays, Electron Beam, and Gamma Irradiation on Chemical and Physical Properties of EVA Multilayer Films
Gamma-ray irradiation, using the cobalt-60 isotope, is the most common radiation modality used for medical device and biopharmaceutical products sterilization. Although X-ray and electron-beam (e-beam) sterilization technologies are mature and have been in use for decades, impediments remain to switching to these sterilization modalities because of lack of data on the resulting radiation effects for the associated polymers, as well as a lack of education for manufacturers and regulators on the viability of these sterilization alternatives. For this study, the compatibility of ethylene vinyl acetate (EVA) multilayer films with different ionizing radiation sterilization (X-ray, e-beam, and gamma irradiation) is determined by measuring chemical and physical film properties using high performance liquid chromatography, differential scanning calorimetry, Fourier-Transform InfraRed spectroscopy (FTIR), surface energy measurement, and electron spin resonance techniques. The results indicate that the three irradiation modalities induce no differences in thermal properties in the investigated dose range. Gamma and X-Ray irradiations generate the same level of reactive species in the EVA multilayer film, whereas e-beam generates a reduced quantity of reactive species.
Radiolytic Gas Production from Aluminum Coupons (Alloy 1100 and 6061) in Helium Environments—Assessing the Extended Storage of Aluminum Clad Spent Nuclear Fuel
Corrosion of aluminium alloy clad nuclear fuel, during reactor operation and under subsequent wet storage conditions, promotes the formation of aluminium hydroxide and oxyhydroxide layers. These hydrated mineral phases and the chemisorbed and physisorbed waters on their surfaces are susceptible to radiation-induced processes that yield molecular hydrogen gas (H 2 ), which has the potential to complicate the long-term storage and disposal of aluminium clad nuclear fuel through flammable and explosive gas mixture formation, alloy embrittlement, and pressurization. Here, we present a systematic study of the radiolytic formation of H 2 from aluminium alloy 1100 (AA1100) and 6061 (AA6061) coupons in “dry” (~0% relative humidity) and “wet” (50% relative humidity) helium environments. Cobalt-60 gamma irradiation of both aluminium alloy types promoted the formation of H 2 , which increased linearly up to ~2 MGy, and afforded G-values of 1.1 ± 0.1 and 2.9 ± 0.1 for “dry” and “wet” AA1100, and 2.7 ± 0.1 and 1.7 ± 0.1 for “dry” and “wet” AA6061. The negative correlation of H 2 production with relative humidity for AA6061 is in stark contrast to AA1100 and is attributed to differences in the extent of corrosion and varying amounts of adsorbed water in the two alloys, as characterized using optical profilometry, scanning electron microscopy, Raman spectroscopy, and X-ray diffraction techniques.
Motivation and Development of a Compact Superconducting Accelerator for X-ray Medical Device Sterilization
Fermilab is developing a compact superconducting (CSRF) accelerator as a source of a high-power, high-energy electron beam to produce an x-ray beam comparable to $\geq$ 2 MCi of cobalt-60. As part of this development, we are presently assembling a 20 kW, 1.6 MeV prototype that incorporates the four enabling technologies described below. These technologies support a heat budget that is within the capacity of commercially available cryocoolers and eliminate the need for liquid cryogens. The use of superconducting technologies promises efficiencies, wall-plug to beam, of 80% or greater. A summary of the design and progress to date will be given. In addition, we will present a review of developments within the medical device sterilization industry that are motivating the development of this technology.
Predicting Radiation-Induced Plutonium Redox Chemistry using Multi-scale Modeling Methods
Over the the last 70 years plutonium (Pu) has been integral in the development of several technologies that have changed the world, yet our fundamental understanding of its chemistry is still far from complete. This is a testament to this element’s unique and complex properties, such as its ability to coexist as multiple oxidation states in aqueous solution. Careful manipulation of plutonium oxidation states is essential in the study and utilization of its rich chemistry. To achieve this level of control, a comprehensive mechanistic understanding of radiation-induced plutonium redox chemistry is critical due to the unavoidable exposure of plutonium to ionizing radiation fields, both inherent and from in-process applications. For this reason, we have developed an experimentally evaluated multi-scale computer model for the prediction of gamma radiation-induced Pu(IV) redox chemistry in concentrated nitric acid solutions (1.0, 3.0, and 6.0 M). Under these acidic, aqueous solution conditions, cobalt-60 gamma irradiation afforded negligible net change in the steady-state oxidation state distribution of Pu(IV). Multi-scale calculations, which are in excellent agreement with experimental data, indicate that this observation is due to radiation-induced redox cycling between Pu(IV) and Pu(III), as achieved by the reduction of Pu(IV) by radiolytic nitrous acid and hydrogen peroxide, and the oxidation of Pu(III) by nitrate and hydroxyl radicals. These radiation-induced redox processes are augmented by plutonium’s inherent disproportionation reactions.
Purification Techniques for Actinide Radiolysis Studies
Our fundamental understanding of actinide radiation-induced redox chemistry is crucial due to their unavoidable exposure to ionizing radiation fields, both inherent and from in-process applications. Plutonium (Pu) and americium (Am) both possess multiple oxidation states, the careful manipulation of which are essential in the study and utilization of their rich chemistry, developing new technologies, and securing the long-term sustainability of nuclear power. However, knowledge in this area is far from complete. We have studied the radiation-induced chemistry of both Pu and Am through a variety of techniques, including gamma irradiation, in-situ alpha irradiation and pulse radiolysis experiments. However, for the collection of accurate data, thorough purification and quantification of actinide-containing solutions is required. This presentation will cover the purification and quantification techniques employed for the radiolysis experiments described in our recent publications: Kynman et al., Multiscale Modeling of Plutonium Radiation Chemistry in Nitric Acid Solutions. 1. Cobalt-60 Gamma Irradiation of Pu(IV) [https://pubs.acs.org/doi/10.1021/acs.inorgchem.4c00138] and Kynman et al., Generation and Study of Am(IV) by Temperature-Controlled Electron Pulse Radiolysis [https://doi.org/10.1039/D4DT00991F].
Dodecane Radiolysis Yields by Time-Resolved and Steady-State Methods
Liquid organic molecules are present as solvents, complexing ligands, and additives in both used nuclear fuel reprocessing solvent systems and in their subsequent nuclear waste streams. Under these extreme environments, these organic molecules are constantly exposed to ionizing radiation which promotes their radiolysis, forming a variety of short-lived, highly energetic, excited state and radical species.1-4 Here, we demonstrate new experimental results for the steady-state and time-resolved irradiations of dodecane (C12H26), a long chain, liquid, aliphatic hydrocarbon that is the prototypical solvent used for benchtop studies of aqueous-organic solvent extraction systems. When ionizing radiation interacts with neat dodecane, the energy transfer can result in molecular ionization, to give the dodecane radical cation (C12H26+•) and the solvated electron (eS–), and molecular electronic excitation (C12H26*), which rapidly produces transient carbon-centered radical fragments (CxHy•) and hydrogen atoms (H•).1-4 Studies on the initial yields of the ionization and excitation products were performed using time-resolved picosecond electron pulse radiolysis with the use of molecular probes. Using steady-state cobalt-60 gamma irradiations, the suite of products formed by dodecane radiolysis in aerated and deaerated solutions was determined. Then, using iodine as an alkyl radical scavenger, the loss of molecular iodine with dose was quantified, and by correlating with the molecular hydrogen yields of the system, the initial yields of the various carbon-centered radicals were also determined. Finally, the rates of reactions of the C12H26+• and eS– with ligands proposed for use in spent nuclear fuel reprocessing were studied as a function of temperature from 10 – 40 °C.
In-Canal Assay of High Specific Activity 60 Co at the Advanced Test Reactor
Production of high specific activity (HSA) 60 Co has recently resumed at the Advanced Test Reactor (ATR) at the Idaho National Laboratory. The technical steps of performing in-canal assay of HSA 60 Co targets at the ATR are described herein. The HSA targets are assayed on a regular basis, between cycles at the ATR, in order to assess the progress of activation. The targets are also assayed at the conclusion of the irradiation in order to provide activity estimates for the distributor and to be used for safety and shipping evaluations. These target assay activities must take place in the ATR canal to provide sufficient radiological shielding. Furthermore, a specialized assay fixture is used in conjunction with custom 60 Co radiation standards to assess the irradiated target. The specific activity of each irradiated target was determined by first measuring the 60 Co standards to determine a sensitivity factor. Then, each irradiated target was measured, and the integrated measurement was multiplied by the sensitivity factor to determine the total activity of the irradiated target. Finally, a correction factor was determined to adjust the reported activity, accounting for differences in the physical geometries of the standards and targets. These methods were used to accurately assay the gross activity of nine irradiated 60 Co targets, two of which were delivered to the distributor where confirmatory hot-cell assays were performed verifying the accuracy of the in-canal assay method.
Replacement of Cobalt in Medical Device Sterilization: Current Trends, Opportunities and Barriers to Adoption of X-ray and E-Beam Within the Medical Device Sterilization Market
Radioactive sources, specifically Co-60, are crucially important to the medical device sterilization industry; however, their benefits must be balanced against the need to ensure that the materials are secure. Accelerator-based sterilization methods, including X-ray and E-Beam, can in many cases sufficiently replace Co-60 and ethylene oxide, the dominant modalities currently in use; however, a lack of hands-on experience with accelerators, regulations, and a lack of capacity have hampered faster adoption of these technologies. The market is likely to change, however, given public pressures against ethylene oxide and concerns over the cost and long-term supply chain robustness of Co-60. This may provide an opportunity for growth for accelerator capabilities. Current research at Sandia National Laboratories and Argonne National Laboratory, on behalf of the Department of Energy’s National Nuclear Security Administration Office of Radiological Security, is focused on developing an understanding of the medical device sterilization marketplace, the different modalities that are used to sterilize goods, and the drivers that affect the actors within it. Research at Pacific Northwest National Laboratory, in conjunction with the medical device sterilization industry, has focused on expanding the industry’s understanding of the capabilities of X-ray sterilization and developing data that can inform the industry’s consideration of a transition towards accelerator-based devices.
Gamma Calibrations and 60 Co Standards for Prompt Detectors
Abstract not provided.