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DOE OSTI2022

Charging of radioactive and environmental airborne particles

The charging of various airborne particles was investigated using single-particle levitation and charge-balance equations. Though radioactive decay and triboelectrification can induce charging, it is typically assumed that the aerosols in a radioactive plume will not carry significant charge at steady state since atmospheric particles can have their charge neutralized through the capture of adjacent counter-ions (i.e., diffusion charging). Here to assess this assumption, we directly measured the surface charge and charge density of various triboelectrically charged aerosols including radioactive uranium oxide (<1 μm), urban dust, Arizona desert dust, hydrophilic and hydrophobic silica nanoparticles, and graphene oxide powders using an electric field-assisted particle levitator in air. Of these particles, uranium oxide aerosols exhibited the highest surface charge density. Charge balance equations were employed to predict the average charge gained from radioactive decay as a function of time and to evaluate the effects of diffusion charging on triboelectrically charged radioactive and non-radioactive particles in the atmosphere. Simulation results show that particles, initially charged through triboelectrification, can be quickly discharged by diffusion charging in the absence of radioactive decay. Nevertheless, simulation results also indicate that particles can be strongly charged when they carry radionuclides. These experimental and simulation results suggest that radioactive decay can induce strong particle charging that may potentially affect atmospheric transport of airborne radionuclides.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Mitigation of Cosmic Rays-Induced Errors in Superconducting Quantum Processors

Environmental radioactivity and cosmic-rays have recently been identified as a source of decoherence in super-conducting quantum bits (qubits). In particular, the absorption of cosmic-ray muons and gamma rays emitted by naturally occurring radioactive isotopes in the qubit substrate leads to correlated errors in superconducting quantum processors, posing significant challenges to quantum error correction. To enable quantum computing to scale, it is therefore necessary the devel-opment of mitigation strategies to prevent, or keep under control, error bursts due to particle impacts in the chip. While most environmental radioactive sources can be effectively suppressed using dedicated shielding, cosmic-ray muons, with their high penetration capability, can only be mitigated by moving the entire facility in a deep underground laboratory. This work explores the potential for developing a novel class of quantum processors equipped with an active veto system to protect superconducting-based quantum computers from the detrimental effects of atmospheric muons. Such a device would enable the identification of an atmospheric muon interaction within the processor and veto all operations performed during the occurrence of such an interaction. By demonstrating high detection efficiency and negligible dead time, we aim to establish that the future of quantum processors can be envisioned in above-around facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Dose estimates and their uncertainties for use in epidemiological studies of radiation-exposed populations in the Russian Southern Urals

Many residents of the Russian Southern Urals were exposed to radioactive environmental pollution created by the operations of the Mayak Production Association in the mid- 20 th century. There were two major releases: the discharge of about 1x10 17 Bq of liquid waste into the Techa River between 1949 and 1959; and the atmospheric release of 7.4 * 10 16 Bq as a result an explosion in the radioactive waste-storage facility in 1957. The releases into the Techa River resulted in the exposure of more than 30,000 people who lived in riverside villages between 1950 and 1961. The 1957 accident contaminated a larger area with the highest exposure levels in an area that is called the East Urals Radioactive Trace (EURT). Current epidemiologic studies of the exposed populations are based on dose estimates obtained using a Monte-Carlo dosimetry system (TRDS-2016MC) that provides multiple realizations of the annual doses for each cohort member. These dose realizations provide a central estimate of the individual dose and information on the uncertainty of these dose estimates. In addition, the correlation of individual annual doses over realizations provides important information on shared uncertainties that can be used to assess the impact of shared dose uncertainties on risk estimate uncertainty.This paper considers dose uncertainties in the TRDS-2016MC. Individual doses from external and internal radiation sources were reconstructed for 48,036 people based on environmental contamination patterns, residential histories, individual 90 Sr body-burden measurements and dietary intakes. Dietary intake of 90 Sr resulted in doses accumulated in active bone marrow (or simply, marrow) that were an order of magnitude greater than those in soft tissues. About 84% of the marrow dose and 50% of the stomach dose was associated with internal exposures. The lognormal distribution is well-fitted to the individual dose realizations, which, therefore, could be expressed and easily operated in terms of geometric mean (GM) and geometric standard deviation (GSD). Cohort average GM for marrow and stomach cumulative doses are 0.21 and 0.03 Gy, respectively. Cohort average dose uncertainties in terms of GSD are as follows: for marrow it is 2.93 (90%CI: 2.02–4.34); for stomach and the other non-calcified tissues it is 2.32 (90% CI: 1.78–2.9).

61 RADIATION PROTECTION AND DOSIMETRY↗

DOE OSTI1992

Nuclear Safety [Vol. 33, No. 1, January-March 1992]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 Technical Note: A New Approach to Fission Reactor Safety, Yu. V. Petrov; 5 Erratum; ACCIDENT ANALYSIS: 6 Analysis and Modeling of Fission Product Release from Various Uranium-Aluminum Plate-Type Reactor Fuels, R. P. Taleyarkhan; CONTROL AND INSTRUMENTATION: 23 Applications of a Surveillance and Diagnostics Methodology Using Neutron Noise From a Pressurized-Water Reactor, R. T. Wood, L. F. Miller, and R. B. Perez; DESIGN FEATURES: 36 Westinghouse Advanced Passive 600 Plant, B. A. McIntyre and R. K. Beck; 47 System 80+™ PWR Safety Design, C. W. Bagnal, R. A. Matzie, and R. S. Turk; ENVIRONMENTAL EFFECTS: 58 The MATS Experiments—Mesoscale Atmospheric Transport Studies at the Savannah River Site, A. H. Weber, S. Berman, R. J. Kurzeja, and R. P. Addis; 75 Book Review: Environmental Radioactivity in the European Community 1984-1985-1986, C. A. Little; WASTE AND SPENT FUEL MANAGEMENT: 76 Activities Related to Waste and Spent Fuel Management, M. D. Muhlheim and E. G. Silver; OPERATING EXPERIENCES: 87 Aging Assessment of BWR Control Rod Drive Systems, R. H. Greene; 100 Reactor Shutdown Experience, Compiled by J. W. Cletcher; 103 Selected Safety-Related Events, Compiled by G. A. Murphy; 110 Operating U.S. Power Reactors, Compiled by M. D. Muhlheim and E. G. Silver; RECENT DEVELOPMENTS: 129 General Administrative Activities, Compiled by M. D. Muhlheim and E. G. Silver; 139 Reports, Standards, and Safety Guides, D. S. Queener; 143 Proposed Rule Changes as of Sept. 30 1991; ANNOUNCEMENTS: 128 Harvard School of Public Health Announces Short Courses; 128 16th Biennial ANS Topical Meeting on Reactor Operating Experience: Present and Future Technologies—Applying Lessons Learned (Call for Papers); 147 The Authors; 150 Indexes to Nuclear Safety, Volume 32; 154 Errata.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI1992

Nuclear Safety [Vol. 33, No. 1, January-March 1992]

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Expected sensitivity to 128 Te neutrinoless double beta decay with the CUORE TeO 2 cryogenic bolometers

The CUORE experiment is a ton-scale array of TeO 2 cryogenic bolometers located at the underground Laboratori Nazionali del Gran Sasso of Istituto Nazionale di Fisica Nucleare (INFN), in Italy. The CUORE detector consists of 988 crystals operated as source and detector at a base temperature of ~ 10 mK. Such cryogenic temperature is reached and maintained by means of a custom built cryogen-free dilution cryostat, designed with the aim of minimizing the vibrational noise and the environmental radioactivity. The primary goal of CUORE is the search for neutrinoless double beta decay of 130 Te , but thanks to its large target mass and ultra-low background it is suitable for the study of other rare processes as well, such as the neutrinoless double beta decay of 128 Te. This tellurium isotope is an attractive candidate for the search of this process, due to its high natural isotopic abundance of 31.75%. The transition energy at (866.7 ± 0.7) keV lies in a highly populated region of the energy spectrum, dominated by the contribution of the two-neutrino double beta decay of 130 Te. As the first ton-scale infrastructure operating cryogenic TeO 2 bolometers in stable conditions, CUORE is able to achieve a factor > 10 higher sensitivity to the neutrinoless double beta decay of this isotope with respect to past direct experiments.

128-Te↗

DOE OSTI2022

Ultra-low-level measurements of airborne fission products from the Fukushima Daiichi reactor accident using high volume collection systems at Savannah River National Laboratory

For this study, ultra-low-level measurements of radionuclides in air have been conducted at the Savannah River National Laboratory (SRNL) to determine the atmospheric concentration of fission products released following the Fukushima Daiichi reactor accident on March 11, 2011. Air filter samples were acquired from two high-volume collection systems (a traditional filter-based system and an electrostatic precipitator-based system) to monitor airborne radionuclide concentrations in the period covering from 2 weeks to 3 years after the disaster. The world-wide spread of low-level concentrations of airborne fission products from the Fukushima event provided a unique opportunity to demonstrate SRNL's electrostatic particle collection technology and other improvements in environmental monitoring developed at the Savannah River Site (SRS). Detecting and analyzing the release allowed a comprehensive test of SRS systems for monitoring environmental radioactivity. Gamma-ray-emitting fission products ( 131,132 I, 134,136,137 Cs, and 129,132 Te) and cosmogenic isotopes ( 7 Be and 22 Na) in air were detected and quantified by high-resolution gamma-ray spectroscopy at concentrations as low as 0.07 μBq per standard cubic meter (SCM) (50 mBq total 137 Cs), while plutonium content was quantified by thermal ionization mass spectrometry (TIMS) at concentrations as low as 6.5 × 10 –21 g/SCM (3.0 fg 239+240 Pu). Isotope concentrations measured at SRNL from gamma-ray spectroscopy were compared to independent measurements from Chapel Hill, NC, located approximately 370 km (230 mi) NE of SRNL. Meteorological modeling was also used to predict radionuclide transport from the location of release to both measurement locations.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

DOE OSTI2022

Permanent Foam Fixatives for Radioactive Contamination Control: Environmental Chamber Testing

The Department of Energy (DOE) Office of Environmental Management (EM) is tasked with closing cleanup sites throughout the DOE-EM complex. A major component of successfully closing the sites is the deactivation and decommissioning (D&D) of radioactively contaminated buildings in nuclear facilities. Deactivation consists of the process of placing a contaminated facility in stable condition in order to minimize any risks that could affect workers, the public, and the environment. Successful deactivation and decommissioning consists of leaving the buildings in an agreed upon end state to provide future protection against hazards. Hazards include radiation but can also include asbestos, polychlorinated biphenyls, and other environmental and physical hazards.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Environmental evaluation of radioactivity levels and associated radiation hazards in groundwater around the WIPP site

Groundwater may contain radioactive substances which can be dangerous to human health. Concentrations of natural radionuclides polonium (Po), thorium (Th), uranium (U), and radium (Ra) isotopes were measured in groundwater samples collected from different locations in the vicinity of the Waste Isolation Pilot Plant (WIPP) site in Carlsbad, New Mexico. The average values of gross activity concentrations of 210 Po, 228 Th, 238 U, 234 U, 226 Ra and 228 Ra isotopes were determined to be 1.62 Bq L -1 in shallow groundwater and 5.88 Bq L -1 in deep groundwater, respectively. The total radioactivity in deep groundwater was higher than that in shallow groundwater, and most of the radioactivity in the water is from 226 Ra. Furthermore, the effective doses for ingestion of natural radionuclides were about 0.333 mSv y–1 for shallow groundwater and about 1.338 mSv y –1 for deep groundwater samples, which are higher than the World Health Organization (WHO, 2017) guideline level (0.1 mSv y –1 ) for drinking water. Ra dominated the total ingestion dose, contributing 93.06 % and 75.40 % of the total effective doses to the deep and shallow groundwater, respectively. The ingrowth and decay of natural radionuclides suggested that 228 Ra/ 226 Ra ratio can be a useful indicator of the source of radioactive contamination. The radioactivity data obtained from the investigated groundwater samples can be used to establish a baseline for radioactivity levels in groundwater around the WIPP site.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

NASA NTRS1998

Retrospective dosimetry related to chronic environmental exposure

Radioactive contamination of the environment occurred in the early fifties as a result of the releases from the Mayak plutonium production complex (Southern Urals, Russia). The releases of liquid wastes into the Techa river resulted in chronic exposure of 30,000 residents of the riverside communities. Since 1951 90Sr body burdens have been measured for over half of this cohort. This paper presents the analysis of data on 90Sr in humans and describes the reconstruction of internal doses for these people.

NASA Discipline Radiation Health↗

DOE OSTI2022

Meta-Study of Particulate Detection Losses on Radioactive Air Sample Filters

Several mathematical relationships between air sample filter mass loading and the correlated analytical self-absorption factor were developed using data from other published research in this meta-study. Gross-alpha and -beta applications are addressed for this research. As filter media becomes loaded with particulate matter, there is potential for measurement losses due to self-absorption by mass loading. Components contributing to absorption include particulate dust, radioactive particulates, and filter material. Standards indicate a correction factor should be used when the penetration of radioactive material into the collection media or self-absorption of radiation by the material collected would reduce the detection rate by more than 5%. Previously, losses due to self-absorption have been reported up to 100% over a range up to ~10 mg∙cm -2 mass loading. These absorption losses then can be used to determine a correction factor for sample results. For low mass loadings (e.g., ≤0.1 mg∙cm -2 ) corrections factors in the 0.85 - 1 range have been recommended and used, while at higher mass loadings nearer to 10 mg∙cm -2 correction factors closer to 0 (representing near 100% losses) are used. Based on data from published studies, the different methods for relating percent loss due to self-absorption to mass loading include linear, exponential, quadratic, and trinomial derived functions. Where applicable, both forced zero and non-forced zero results were evaluated. From the derived functions evaluated, the trinomial function provided the best fit. Once the sample filter mass loading is known, the trinomial function can be applied to estimate losses and the corresponding self-absorption factor. When applied to routine operating conditions for radiological facility stacks monitored at the Pacific Northwest National Laboratory for an average sample filter mass loading of 0.09 ± 0.12 (2σ) mg∙cm -2 (excluding negative values and outliers) and a range from 0 - 0.24 mg∙cm -2 , the estimated trinomial function nominal self-absorption losses are less than 5% at 0.09 mg∙cm -2 and less than 10% at 0.24 mg∙cm -2 . The trinomial function is one method that may be used to adjust the activity results of an air sample when the sample-specific mass loading is determined. The application of no correction factor when the ANSI/HPS N13.1-2021 guidance of a 5% threshold for loss is not reached with typical stack sample mass loadings may be reasonable in high-efficiency particulate air filtered systems. For simplicity, it would be conservative in assigning the self-absorption correction factor at the 5% threshold (i.e., 0.95) for general uses but in cases of heavy mass loading to calculate the factor.

air sampling↗

DOE OSTI2022

Identification, isolation, and characterization of a novel type of Fukushima-derived microparticle

Abstract In the course of the Fukushima nuclear accident, radionuclides were released in various forms, including so-called radiocesium-bearing microparticles (CsMP). So far, four types of CsMP were described: Type A is smaller in size (< 10 μm), Types B, C, and D are larger (> 100 μm). In this work, we present a novel type of CsMP (proclaimed Type E). Three particles of Type E were extracted from a contaminated blade of grass that was sampled 1.5 km from the Fukushima Daiichi nuclear power plant in late 2011. They were located using autoradiography, isolated using an optical microscope and micromanipulator, and characterized using scanning electron microscopy, energy dispersive x-ray spectroscopy, and low-level gamma-ray spectrometry. Type E CsMPs are 10–20 μm in size and exhibit an unusually low and barely detectable 137 Cs activity of only ≤ 10 mBq per particle. Their brittle and fragile character may indicate a high surface tension.

137Cs↗

DOE OSTI2024

Application of machine learning to discover new intermetallic catalysts for the hydrogen evolution and the oxygen reduction reactions

The adsorption energies for hydrogen, oxygen, and hydroxyl were calculated by means of density functional theory on the lowest energy surface of 24 pure metals and 332 binary intermetallic compounds with stoichiometries AB, A 2 B, and A 3 B taking into account the effect of biaxial elastic strains. This information was used to train two random forest regression models, one for the hydrogen adsorption and another for the oxygen and hydroxyl adsorption, based on 9 descriptors that characterized the geometrical and chemical features of the adsorption site as well as the applied strain. All the descriptors for each compound in the models could be obtained from physico-chemical databases. The random forest models were used to predict the adsorption energy for hydrogen, oxygen, and hydroxyl of ≈2700 binary intermetallic compounds with stoichiometries AB, A 2 B, and A 3 B made of metallic elements, excluding those that were environmentally hazardous, radioactive, or toxic. This information was used to search for potential good catalysts for the HER and ORR from the criteria that their adsorption energy for H and O/OH, respectively, should be close to that of Pt. Further, this investigation shows that the suitably trained machine learning models can predict adsorption energies with an accuracy not far away from density functional theory calculations with minimum computational cost from descriptors that are readily available in physico-chemical databases for any compound. Moreover, the strategy presented in this paper can be easily extended to other compounds and catalytic reactions, and is expected to foster the use of ML methods in catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Applied Multi-Objective Modelling & Optimization [Slides]

Multi-objective modelling and the associated optimization are powerful tools to find solutions to complex applied problems. By finding multiple optimal solutions, we retain flexibility in later potential implementation and may choose tradeoffs from best options. Quantum-inspired and realized quantum annealing systems present interesting avenues in current and future research into the state-of-the-art in optimization.

42 ENGINEERING↗

DOE OSTI2024

Studying microbially induced corrosion on glass using ToF-SIMS

Microbially induced corrosion (MIC) is an emerging topic that has huge environmental impacts, such as long-term evaluation of microbial interactions with radioactive waste glass, environmental cleanup and disposal of radioactive material, and weathering effects of microbes. Time-of-flight secondary ion mass spectrometry (ToF-SIMS), a powerful mass spectral imaging technique with high surface sensitivity, mass resolution, and mass accuracy, can be used to study biofilm effects on different substrates. Understanding how to prepare biofilms on MIC susceptible substrates is critical for proper analysis via ToF-SIMS. We present here a step-by-step protocol for preparing bacterial biofilms for ToF-SIMS analysis, comparing three biofilm preparation techniques: no desalination, centrifugal spinning (CS), and water submersion (WS). Comparisons of two desalinating methods, CS and WS, show a decrease in the media peaks up to 99% using CS and 55% using WS, respectively. Proper desalination methods also can increase biological signals by over four times for fatty acids using WS, for example. ToF-SIMS spectral results show chemical compositional changes of the glass exposed in a Paenibacillus polymyxa SCE2 biofilm, indicating its capability to probe microbiologically induced corrosion of solid surfaces. This represents the proper desalination technique to use without significantly altering biofilm structure and substrate for ToF-SIMS analysis. ToF-SIMS spectral results showed chemical compositional changes of the glass exposed by a Paenibacillus bacterial biofilm over 3-month inoculation. Finally, possible MIC products include various phosphate phase molecules not observed in any control samples with the highest percent increases when experimental samples were compared with biofilm control samples.

36 MATERIALS SCIENCE↗

DOE OSTI2022

NEVADA NATIONAL SECURITY SITE 2021 WASTE MANAGEMENT MONITORING REPORT AREA 3 AND AREA 5 RADIOACTIVE WASTE MANAGEMENT SITES

Environmental monitoring data are collected at and around the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) within the Nevada National Security Site (NNSS). This report summarizes the 2021 environmental data to provide an overall evaluation of RWMS performance and to support environmental compliance and performance assessment (PA) activities.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

EMP, Attachment 1: Sampling and Analysis Plan (Rev.1)

This Sampling and Analysis Plan (SAP) is written for the Environmental Radiation Task activities related to radioactive air emissions (stack) monitoring and environmental radiological ambient air surveillance of Pacific Northwest National Laboratory (PNNL) operations at the PNNL-Richland campus and PNNL-Sequim campus. PNNL is a U.S. Department of Energy Office of Science laboratory in Richland, Washington. This plan is an attachment to PNNL’s Environmental Radiological Air Monitoring Plan (EMP) (PNNL-20919) and addresses a discrete, vital subject area that is subject to revision independent of the main text of the EMP document. This SAP provides the requirements for planning sampling events and the requirements imposed on the services provided by the analytical laboratory to the PNNL Environmental Radiation Task.

40 CFR 61 Subpart H↗

DOE OSTI2025

Replacement of Fly Ash with Natural Pozzolans in Cementitious Waste Forms: Progress Report

The Department of Energy Environmental Management (DOE EM) Office is currently responsible for treating radioactive and mixed waste, environmental restoration, and closing contaminated tanks and facilities resulting from radioactive isotope production for defense applications during the Cold War. Cementitious reagents are the most widely used materials for (1) chemically stabilizing and encapsulating radionuclides and hazardous metals contaminated with radionuclides and Resource Conservation and Recovery Act (RCRA) hazardous metals and (2) solidifying radioactive and mixed wastewater for final disposal. Cementitious grouts and flowable concretes are also the most widely used materials for DOE waste tank and facility closures.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗