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Aging of Concrete for the Evaluation of Repair Materials to Protect the Walls of the HCAEX Tunnel at Savannah River - 20301

H-Canyon, located in the Savannah River site, is a unique facility for chemical reprocessing of plutonium, highly-enriched uranium, and other radioactive materials. The exhaust gases of the H-Canyon are sent through the H-Canyon Exhaust (HCAEX) tunnel for contamination removal. Robotic inspections of the tunnel revealed significant degradation of the reinforced concrete structure that was associated with acid attack, and could compromise the structural stability of the tunnel. Thus, the identification and evaluation of potential repair materials that could be applied on the degraded walls to mitigate and prevent further degradation is of significant interest to the Department of Energy and the Savannah River representatives. This research effort has been divided into two phases: 1) Development and evaluation of aged concrete under accelerated aging conditions (which is the focus of this paper) and 2) Evaluation of potential repair materials applied on aged and non-aged concrete under simulated aggressive conditions. In order to develop and evaluate concrete samples exposed to accelerated aging conditions in simulated aggressive environments, a literature review of the HCAEX tunnel was conducted that included 1) characterization and extent of the concrete damage, 2) environmental conditions inside the tunnel and 3) primary deterioration mechanisms. In addition, potential coatings and/or repair materials for degraded concrete surfaces exposed to aggressive environments (primarily acidic) were selected from the literature review and the most common testing and measurements for evaluating acid attack phenomena, erosion, etc. were reviewed. From the literature review findings, a preliminary bench-scale test plan for the concrete aging was developed, including accelerated aging tests with aggressive conditions (acid fumes, humidity, etc.). Concrete samples were exposed to the aging accelerated conditions (e.g. immersion in acid solutions) and visual inspection, mass loss and pH change (acid solution) were recorded over time. Correlations between the visual inspection, mass loss and pH changes results and the aging time or the aging conditions were developed. Specimens submitted to the highest acid concentration showed the fastest and most intense degradation. The type of coarse aggregate (limestone) used for the concrete seemed to be the cause of the fastest aging observed, compared to the cement paste. The research findings created the foundation for the ongoing investigation, in which new concrete samples with a mix design similar to the HCAEX tunnel will be tested and will serve as the substrate for testing the selected coatings and /or repair materials. In this paper, the literature review and preliminary results from the aging tests are provided. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Microstructure of In-Core Molten Salt Corrosion Hastelloy N{sup R} and 316 Stainless Steel

Since 2011, many materials have been discussed for potential application in Fluoride salt-cooled High-temperature nuclear Reactors (FHRs), which are emerging as leading reactor concept for the next generation of nuclear reactors thanks to the benefits of a high degree of passive safety, high thermal efficiency, and low spent fuel volume. Among these discussed materials, Hastelloy N{sup R} and 316L stainless steel have been selected as the most likely candidate alloys for FHRs. To provide direct experience in integrating a real system using molten FLiBe salt for reactor operation, these two candidate alloys were experimentally tested in Li-7 enriched Li{sub 2}BeF{sub 4} (FLiBe) molten salt in the core of MIT Research Reactor (MITR) at 700 deg. C for 1000 hours. After in-core corrosion testing, some basic post-irradiation examinations (PIE) including weight change per unit area and surface profile as well as surface morphology were conducted in the MIT Nuclear Reactor Laboratory (NRL) and compared with out-of-reactor corrosion samples. The deep understanding of these alloys in high-temperature molten salt with strong neutron irradiation requires further microstructural analysis such as electron microscopy and energy dispersive spectroscopy on the surface and cross-section of the in-core corrosion tested samples. The challenge in the microstructural analysis is due to the high radioactivity from the gamma emitting isotopes formed in alloys during neutron irradiation. Additionally, the facilities that are authorized for radioactive materials are very limited on campus. In this study, the microstructure of the in-core corrosion tested Hastelloy N{sup R} and 316L stainless steel specimen was analyzed by using the facilities at the Center for Advanced Energy Studies (CAES) at Idaho National Laboratory (INL) through the Nuclear Science User Facilities (NSUF) Rapid Turnaround Experiment (RTE) program.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Project 57 Air Monitoring Report: (Jan 1 - Dec 31 2018)

During the late 1950s, the Atomic Energy Commission (AEC) (now the U.S. Department of Energy [DOE]) conducted a series of safety experiments to determine if a nuclear device subjected to a large conventional explosives detonation would result in a nuclear yield. The AEC obtained temporary use of a large portion of western Emigrant Valley from the U.S. Department of Defense (DOD) for one of these experiments: Project 57. Following the Project 57 safety experiment, the AEC fenced the contaminated area and returned control of the surrounding land to the DOD. Emigrant Valley is part of the Nevada Test and Training Range (NTTR). For safety and security reasons, access to the NTTR is controlled using both physical (i.e., fences) and administrative (e.g., signs and postings) controls. Therefore, the public cannot access the Project 57 site and there are no known human receptors that routinely access the site. Project 57 was detonated on April 24, 1957, in Emigrant Valley approximately 13 mi (21 km) northeast of the north end of Yucca Flat. This test was undertaken to develop: (1) a means of estimating immediate distribution and long-term redistribution of plutonium dispersed during a nonnuclear detonation; (2) biomedical evaluation techniques for use in likely plutonium-laden environments; (3) methods of decontaminating ground areas, pavements, and building materials; and (4) alpha survey instruments and field monitoring procedures to promptly estimate contaminant deposition. Although the test did not result in the fission of nuclear materials, it did disseminate plutonium across the ground surface. Various radiological surveys have been performed in the area since Project 57 was conducted. The AEC delineated the area containing radioactive material based on radioactivity surveys performed shortly after the test was conducted. A designated Contamination Area (CA), marked by a fence, was established later. The distribution of americium-241 (Am-241) in the area was determined again in a 1997 flyover, which showed Am-241 ranging from as much as 70,000 counts per second (cps) at ground zero to background (<70 cps). This survey also documented Am-241 radioactivity on the ground surface beyond the east side CA fence at levels of up to 150 cps. In 2007, the DOE expanded the CA by posting “Contamination Area” signs 200 ft to 400 ft (60 m to 120 m) beyond the original fence, which formed a new CA boundary.

54 ENVIRONMENTAL SCIENCES↗

Radiation Leakage and the Precision of Characterizing Nuclear Material Using Calorimetric Assay - 19233

For measuring a waste drum containing multi-nuclide radioactive material calorimetric assay is often combined with gamma ray and neutron measurements. To reduce the methodological uncertainties of the inventory determination in a multi-nuclide matrix, the escaping radiation must be quantized as much as the encapsulated gamma-rays and α-, β-, n- particles depositing radiological heat inside the drum. To differentiate the possible variety of heat sources in a radioactive waste drum, Monte Carlo simulations are utilized resembling the waste drum and the calorimeter in both, their geometries as well as the material compositions. MCNP6-based numerical imaging of the Large Volume Calorimeter (LVC) designed by KEP Nuclear(France) allows simulating various scenarios for different particles types, energies and source locations to accompany and support the interpretation of calorimetric KEP-LVC measurements anticipated within the CHANCE project. For the analyses, the particle flux and energy deposition in each layer of the calorimeter are displayed. The results yield that a significant part of the emitted radiation leaves the system and does not contribute to the heat deposited inside the drum. As an example, the particle flux study of a 200 L mock-up drum placed inside the KEP-LVC calorimeter is discussed. A tally 4 with mesh option for both gamma and neutrons up to 5 MeV simulates the mean flux in each cell and for various source location and source distribution patterns. The expected energy deposition is cumulated for each layer, and over the whole energy range it reveals that actually a small but well known fraction of particles escapes the LVC calorimeter. This makes it a very suitable apparatus for the anticipated experiments on large and heterogeneous waste drums. The results suggest that the most interesting cases would be polyethylene, bitumen and concrete matrices [3, 5]. However, it must be kept in mind that the high-energy part of the gamma and neutron radiation flux can reach the reference chamber of the calorimeter and deposit some energy there, which may compromise the calibration and cause double-bias. The simulations showed that, depending on source location and power, neutron and high-energy gamma radiation leakage can influence the heat measurements differently. In general, part of the simulation results suggest that for waste drums with a high emission rate the accuracy of calorimetric assay can be decreased due to radiation escape. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Mixed-layered bismuth-oxygen-iodine materials for capture and waste disposal of radioactive iodine

Materials and methods of synthesizing mixed-layered bismuth oxy-iodine materials, which can be synthesized in the presence of aqueous radioactive iodine species found in caustic solutions (e.g. NaOH or KOH). This technology provides a one-step process for both iodine sequestration and storage from nuclear fuel cycles. It results in materials that will be durable for repository conditions much like those found in Waste Isolation Pilot Plant (WIPP) and estimated for Yucca Mountain (YMP). By controlled reactant concentrations, optimized compositions of these mixed-layered bismuth oxy-iodine inorganic materials are produced that have both a high iodine weight percentage and a low solubility in groundwater environments.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Response of the REWARD detection system to the presence of a Radiological Dispersal Device

In recent years an increased international concern has emerged about the radiological and nuclear (RN) threats associated with the illicit trafficking of nuclear and radioactive materials that could be potentially used for terrorist attacks. The objective of the REWARD (Real Time Wide Area Radiation Surveillance System) project, co-funded by the European Union 7. Framework Programme Security, consisted in building a mobile system for real time, wide area radiation surveillance, using a CdZnTe detector for gamma radiation and a neutron detector based on novel silicon technologies. The sensing unit includes a GPS system and a wireless communication interface to send the data remotely to a monitoring base station, where it will be analyzed in real time and correlated with historical data from the tag location, in order to generate an alarm when an abnormal situation is detected. Due to its portability and accuracy, the system will be extremely useful in many different scenarios such as nuclear terrorism, lost radioactive sources, radioactive contamination or nuclear accidents. This paper shortly introduces the REWARD detection system, depicts some terrorist threat scenarios involving radioactive sources and special nuclear materials and summarizes the simulation work undertaken during the past three years in the framework of the REWARD project. The main objective consisted in making predictions regarding the behavior of the REWARD system in the presence of a Radiological Dispersion Device (RDD), one of the reference scenarios foreseen for REWARD, using the Monte Carlo simulation program MCNP6. The reference scenario is characterized in detail, from the i) radiological protection, ii) radiation detection requirements and iii) communications points of view. Experimental tests were performed at the Fire Brigades Facilities in Rome and at the Naples Fire Brigades, and the results, which validate the simulation work, are presented and analyzed. The response of the REWARD detection system to the presence of an RDD is predicted and discussed. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Results from the third Galaxy Serpent tabletop exercise demonstrating the utility of nuclear forensics libraries in support of an investigation

Galaxy Serpent is a virtual, web-based international ongoing series of tabletop exercises designed to mature the concept of National Nuclear Forensics Libraries (NNFL) and illustrate their utility in answering investigative questions or providing investigative leads as part of an investigation involving nuclear or other radioactive material (R/N) out of regulatory control (MORC). Two prior versions of the exercise have been conducted; the first utilizing surrogate data for spent nuclear fuel as the material of interest, and the second using synthetic sealed radioactive source data. Teams participating in the recently concluded third version of the exercise were provided with synthetic uranium ore concentrate (UOC) data mimicking actual data characteristics (e.g. trace element concentrations), which was used to compile a model NNFL. Teams decided how to organize and interpret the data they were provided, dealt with real world features such as missing data, and assessed discriminating attributes. Next, a hypothetical scenario involving three UOC samples found out of regulatory control was provided, and each team had to assess the self-consistency of the individual sources in the unknown data, and employ their model NNFL as a comparative assessment instrument to determine whether the three UOC materials in question were consistent with any of the types of materials in their library. In conclusion, the design of the exercise, methodologies utilized by participating teams, and aggregate results of the exercise will be presented, along with challenges encountered and benefits realized.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Transition in helium bubble strengthening of copper from quasi-static to dynamic deformation

Damage from low-temperature irradiation and the subsequent degradation of materials performance pose significant challenges for the storage of radioactive materials and for peripheral components in some nuclear reactor designs. Fully understanding the mechanical behavior of such materials requires test data for strain rates in both the quasi-static (< 10/s) and dynamic (>> 10/s) regimes. While dynamic testing has generally been avoided in the past for neutron irradiated (contamination concerns) and ion irradiated (insufficient volume) materials, surface-sensitive Richtmyer-Meshkov instability (RMI) tests were used in the present work to overcome these limitations. Here, nanopillar compression, nanoindentation, and RMI testing data from a helium implanted surface layer (~10 µm thick) were compiled to explore the effects of helium bubbles on the materials strength of high-purity copper at strain rates of 0.001/s – 10 8 /s. While nano-mechanical testing revealed increases in yield strength and hardness with increasing helium dose from 1000 to 4000 appm He, RMI indicated no significant changes in strength as compared to unimplanted copper. Here, this discrepancy in behavior was rationalized through a combination of recent literature and follow-on molecular dynamics (MD) simulations, leading to the conclusion that the nanoscale helium bubbles acting as dispersed barriers to dislocation motion at quasi-static strain rates collapse under shock loading and cease to be effective barriers at high strain rates.

36 MATERIALS SCIENCE↗

Solar Powered Radioactive Air Monitoring Stations

Environmental monitoring of ambient air for radioactive material is required as stipulated in the PNNL Site radioactive air license. Sampling ambient air at identified preferred locations could not be initially accomplished because utilities were not readily available. Therefore, solar powered environmental monitoring systems were considered as a possible option. PNNL purchased two 24-V DC solar powered environmental monitoring systems which consisted of solar panels, battery banks, and sampling units. During an approximate four month performance evaluation period, the solar stations operated satisfactorily at an on-site test location. They were subsequently relocated to their preferred locations in June 2012 where they continue to function adequately under the conditions found in Richland, Washington.

air sampling↗

Post-irradiation examination of legacy high burnup fuel to support safety testing

Safety/transient testing to evaluate performance under off-normal conditions is an essential pillar for both the development of Accident Tolerant Fuels (ATF) and the optimization of fuel operation economics beyond current discharge burnups. Among other factors, the successful interpretation of the transient testing results relies upon the knowledge of the initial conditions of the test, including the characteristics of the fuel system under scrutiny. When testing pre-irradiated material, the assumptions that the fuel and the cladding still have the same properties as in the pre-irradiation stage is obviously wrong and could affect the results of the test. This is particularly true the more burnup accumulates in the fuel rod and irradiation progresses. The knowledge of the initial microstructure of both fuel and cladding allows a clearer interpretation of the subsequent transient testing results, provides validation of the physical phenomena underlying the model predictions and eliminates the uncertainties related to the limited knowledge of the sample status before the test. One example is the phenomenon of fine fragmentation that occurs in Light Water reactor (LWR) fuel. During a Loss of Coolant Accident (LOCA) or Reactivity Initiated Transient (RIA) the fuel can severely fragment. During LOCA, high burnup fuel tend to finely fragment, which has raised safety concerns due to the increased likelihood of dispersal of such small particles once the cladding has burst and due to the increased fission gas release. Therefore, efforts have been devoted to the assessment of a pulverization threshold that could determine the conditions under which fine fragmentation is predominant. However, the lack of information regarding the initial conditions of the fuel, and the connections between those conditions and the pre-transient irradiation history, have hindered the development of a fully mechanistic fragmentation and pulverization criterion. The empirical relationships rely on conservative estimations, due to the lack of information on critical material properties and characteristics. More generally, experimental evidence of the irradiation-induced modifications at microstructural scale are necessary to determine the behavior of the material at the macroscopic scale, with the latter being the one of technological interest. Significant progress has been made in the last two decades in the developments of analytical materials science techniques that can be applied to highly radioactive materials, such as high burnup fuels. The availability of new techniques and the improvement of existing ones has enabled investigations previously not possible that can deepen the understanding of the fuel characteristics and properties at high burnup. The better knowledge of material behavior and irradiation-induced phenomena could help the prediction of its performance. In this context, the scope of the present work is to apply a wide portfolio of advanced characterization techniques to determine properties that are relevant for safety and performance. The results are interpreted in the context of engineering scale post-irradiation examinations and available information on the irradiation conditions.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Spent Nuclear Fuel Disposition

One interdisciplinary field devoted to achieving the end-state of used nuclear fuel (UNF) through reuse and/or permanent disposal. The reuse option aims to make use of the remaining energy content in UNF and reduce the amount of long-lived radioactive materials that require permanent disposal. The planned approach in the U.S., as well as in many other countries worldwide, is direct permanent disposal in a deep geologic repository. Used nuclear fuel is fuel that has been irradiated in a nuclear reactor to the point where it is no longer capable of sustaining operational objectives. The vast majority (by mass) of UNF is from electricity generation in commercial nuclear power reactors. Furthermore, the other main source of UNF in the U.S. is the Department of Energy’s (DOE) and other federal agencies’ operation of reactors in support of federal government missions, such as materials production, nuclear propulsion, research, testing, and training. Upon discharge from a reactor, UNF emits considerable heat from radioactive decay. Some period of active on-site cooling (e.g., 2 or more years) is typically required to facilitate efficient packaging and transportation to a disposition facility. Hence, the field of UNF disposition broadly includes storage, transportation and ultimate disposition. See also: Nuclear Fission (content/nuclear-fission/458400), Nuclear Fuels (/content/nuclear-fuels/458600), Nuclear Fuel Cycle (/content/nuclear-fuel-cycle/458500), Nuclear Fuels Reprocessing (/content/nuclear-fuels-reprocessing/458700), Nuclear Power (/content/nuclear-power/459600), Nuclear Reactor (/content/nuclear-reactor/460100), Radiation (/content/radiation/566300), and Radioactive Waste Management (/content/radioactive-waste-management/568900).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Regulatory Perspective on Potential Fuel Reconfiguration and Its Implication to High Burnup Spent Fuel Storage and Transportation - 13042

The recent experiments conducted by Argonne National Laboratory on high burnup fuel cladding material property show that the ductile to brittle transition temperature of high burnup fuel cladding is dependent on: (1) cladding material, (2) irradiation conditions, and (3) drying-storage histories (stress at maximum temperature) [1]. The experiment results also show that the ductile to brittle temperature increases as the fuel burnup increases. These results indicate that the current knowledge in cladding material property is insufficient to determine the structural performance of the cladding of high burnup fuel after it has been stored in a dry cask storage system for some time. The uncertainties in material property and the elevated ductile to brittle transition temperature impose a challenge to the storage cask and transportation packaging designs because the cask designs may not be able to rely on the structural integrity of the fuel assembly for control of fissile material, radiation source, and decay heat source distributions. The fuel may reconfigure during further storage and/or the subsequent transportation conditions. In addition, the fraction of radioactive materials available for release from spent fuel under normal condition of storage and transport may also change. The spent fuel storage and/or transportation packaging vendors, spent fuel shippers, and the regulator may need to consider this possible fuel reconfiguration and its impact on the packages' ability to meet the safety requirements of Part 72 and Part 71 of Title 10 of the Code of Federal Regulations. The United States Nuclear Regulatory Commission (NRC) is working with the scientists at Oak Ridge National Laboratory (ORNL) to assess the impact of fuel reconfiguration on the safety of the dry storage systems and transportation packages. The NRC Division of Spent Fuel Storage and Transportation has formed a task force to work on the safety and regulatory concerns in relevance to high burnup fuel storage and transportation. This paper discusses the staff's preliminary considerations on the safety implication of fuel reconfiguration with respect to nuclear safety (subcriticality control), radiation shielding, containment, the performance of the thermal functions of the packages, and the retrievability of the contents from regulatory perspective. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Formation of hydrocarbons from acid-Clay suspensions by gamma irradiation

The adsorption of certain organic compounds by clays gives rise to the transformation of the adsorbate through the action of the clays. This phenomenon can be enhanced using ionizing radiation. In this context, these kinds of reactions play an important role in many natural and industrial processes. For example, in oil and gas exploration, the source and trap of petroleum hydrocarbons is frequently clay-rich rocks. Clay-water-based muds are also seen as environmentally friendly alternatives to toxic oil-based fluids. The principal processes that occur in sediments are usually held to be of bacterial action and thermal transformation, which may include thermally induced catalytic alteration of the organic debris. On the other hand, radioactive materials are widely distributed throughout Earth. They were more abundant in the past, but are present in petroleum reservoirs. Their presence induced radioactive bombardment, which may have altered these sediments. This important subject has not been extensively studied. The aim of this work is to study the behavior of fatty acids-like behenic acid-and dicarboxylic acids-like fumaric acid-as model compounds, which are adsorbed in a clay mineral (Na-montmorillonite) and exposed to gamma radiation. The results show that the radiation-induced decomposition of the clay-acid system goes along a definitive path (oxidation), rather than following several modes of simultaneous decomposition, as happens in radiolysis without clay or by heating the system. The main radiolytic products for fatty acids are their corresponding hydrocarbons, with one C-atom less than the original acid.

36 MATERIALS SCIENCE↗

Mixed-layered bismuth--oxygen--iodine materials for capture and waste disposal of radioactive iodine

Materials and methods of synthesizing mixed-layered bismuth oxy-iodine materials, which can be synthesized in the presence of aqueous radioactive iodine species found in caustic solutions (e.g. NaOH or KOH). This technology provides a one-step process for both iodine sequestration and storage from nuclear fuel cycles. It results in materials that will be durable for repository conditions much like those found in Waste Isolation Pilot Plant (WIPP) and estimated for Yucca Mountain (YMP). By controlled reactant concentrations, optimized compositions of these mixed-layered bismuth oxy-iodine inorganic materials are produced that have both a high iodine weight percentage and a low solubility in groundwater environments.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Guidelines for Assessing the Toxic Hazard of Spacecraft Chemicals and Test Materials

This document describes the criteria and procedural guidelines used by the NASA/JSC Toxicology Office (JSCSTO), to perform toxicological evaluations. The JSCSTO is responsible for conducting toxicological assessments and assigning toxic hazard levels (THLs) for essentially all chemicals and test materials to be used in or transported to the habitable areas of U.S. spacecraft, non‐U.S. spacecraft inhabitaed by U.S. crew members or habitable areas of off‐Earth habitats where U.S. crew members would be present, including chemicals carried by visiting spacecraft(visiting vehicles) to and from the International Space Station (ISS). Biohazard assessments for biological materials used in payload experiments are performed by the NASA Biosafety Review Board. Radioactive materials are assessed by the Space Radiation Analysis Group for radiation hazards; the flammability rating on flammable materials is assessed by the JSC Materials and Processes Branch, ES4. This document will focus on the assessment of chemically‐induced toxicity hazards. The toxicological assessments, together with assessments on radioactive, biological, physical, and flammability hazards, are incorporated into a mission‐specific Hazardous Materials Summary Table (HMST).

Valerie Elizabeth Ryder↗

Advances in actinide thin films: synthesis, properties, and future directions

Actinide-based compounds exhibit unique physics due to the presence of 5f electrons, and serve in many cases as important technological materials. Targeted thin film synthesis of actinide materials has been successful in generating high-purity specimens in which to study individual physical phenomena. These films have enabled the study of the unique electron configuration, strong mass renormalization, and nuclear decay in actinide metals and compounds. The growth of these films, as well as their thermophysical, magnetic, and topological properties, have been studied in a range of chemistries, albeit far fewer than most classes of thin film systems. This relative scarcity is the result of limited source material availability and safety constraints associated with the handling of radioactive materials. Here, we review recent work on the synthesis and characterization of actinide-based thin films in detail, describing both synthesis methods and modeling techniques for these materials. Further, we review reports on pyrometallurgical, solution-based, and vapor deposition methods. We highlight the current state-of-the-art in order to construct a path forward to higher quality actinide thin films and heterostructure devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗