Nuclear Data for Advanced Reactors and Security Applications [Slides]
Abstract not provided.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
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Irradiation Results of Commercial Neutron and Gamma Sensors at the Ohio State University Research Reactor
This report serves to present the evaluation results of commercial radiation detectors (SPNDs) with the potential to accomplish the data objectives—having sufficient gamma and fast neutron sensitivity—at temperatures near 650°C. The detectors chosen for evaluation are gamma ion chambers from Exosens (previously known as Photonis) models CRGA11 and CRGE32 and tantalum-based self-powered neutron detectors (Ta-SPND) from Mirion. The evaluation was performed in a series of heat irradiations from ambient to 850°C in the 9.5-inch dry tube furnace at the Ohio State University Research Reactor (OSURR). Ion chamber counting curves were measured to evaluate sensor operability at temperature. Detector sensitivity to reactor power and temperature were measured and presented in curve fit parameters. The curve fit equations were used to identify the suggested operational temperatures based on reactor power. Overall, it was evaluated that the CRGA11 was not significantly affected by temperatures up to 650°C and is operable—with higher temperature-contributed signals—up to 700°C. The CRGE32 was more affected by the high temperatures compared to the CRGA11. As a result of increasing temperature, the leakage current was a dominating factor. While the detector can operate up to 600°C and 700°C with lowered high voltage, it is not recommended unless a suitably strong gamma flux field is present. Finally, Ta SPND did not demonstrate good performance beyond 350°C due to the presence of an unknown phenomenon at changing temperatures. The study of the phenomenon is an active research topic outside the scope of this project.
21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
First-of-a-Kind Fuel-bearing Molten Chloride Irradiation Experiment
Molten salt reactors (MSRs) have garnered increasing attention recently with several demonstration efforts on the way. A key challenge to the licensing basis for these reactors is the lack of experimental data on fueled salts. This is expected to be crucial to the safety evaluation and licensing basis of reactors of this type deployed in the future. While capability for irradiating molten salts has been reestablished in the recent decade, no enriched fuel irradiation capability has been developed and tested as of yet. A new experiment vehicle under development at Idaho National Laboratory (INL) is presented here. The Molten-salt Research Temperature-controlled Irradiation (MRTI) experiment was developed to host enriched uranium bearing salt samples to be irradiated at a test reactor within the lab complex. One of the key scientific objectives is to provide irradiated salt samples for post-irradiation examination (PIE) to study the impact of fission product generation and neutron/gamma radioactivity on the salt solution and salt-facing wall material. This paper provides a detailed overview of the mechanical design of the experiment, followed by an overview of the fabrication and assembly of an initial prototype vehicle (with non-fuel-bearing salt). A summary of the key analyses conducted as a part of the performance and safety evaluation is then provided. Lastly, an overview of the test conducted in prototypic out-of-pile (non-neutron) environment are shown. These evaluations provide the foundation for a planned irradiation of an enriched uranium-bearing chloride salt sample in the near term. The upcoming irradiation will contain 13 cm3 of UCl3-NaCl salt (93% enrichment) generating around 20 W/cm3 of fission energy during irradiation and a temperature range that can be contained between bounds of 525-900°C.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Design and testing of an enriched uranium fueled molten salt irradiation vehicle
Molten salt reactors (MSRs) have garnered increasing attention recently with several demonstration efforts on the way. A key challenge to the licensing basis for these reactors is the lack of experimental data on fueled salts. This is expected to be crucial to the safety evaluation and licensing basis of reactors of this type deployed in the future. While capability for irradiating molten salts has started being reestablished in the recent decade, no enriched fuel irradiation capability has been developed and tested as of yet. A new experiment vehicle under development at Idaho National Laboratory (INL) is presented here. The Molten-salt Research Temperature-controlled Irradiation (MRTI) experiment was developed to host enriched-uranium bearing salt samples to be irradiated at a test reactor within the lab complex. One of the key scientific objectives is to provide irradiated salt samples for post irradiation examination (PIE) to study the impact of fission product generation and neutron/gamma radioactivity on the salt solution and salt-facing wall material. This paper provides a detailed overview of the mechanical design of the experiment, followed by an overview of the fabrication and assembly of an initial prototype vehicle (with non-fuel bearing salt). A summary of the key analyses conducted as a part of the performance and safety evaluation is then provided. Lastly, an overview of the test conducted in prototypic out-of-pile (non-neutron) environment are shown. These evaluations provide the foundation for a planned irradiation of and enriched uranium-bearing chloride salt sample in the near term. The upcoming irradiation will contain 13cm 3 of UCl 3 -NaCl salt (93% enrichment) generating around 20 W/cm 3 of fission energy during irradiation and a temperature range that can be contained between bounds of 525-900°C.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Applications of Thermochemical Modeling in Molten Salt Reactors
The extensively evaluated and consistent thermodynamic database, the Molten Salt Thermal Properties Database—Thermochemical (MSTDB-TC), was used along with additional thermodynamic values from other sources as examples of ways to examine molten salt reactor (MSR) fuel behavior. Relative stability with respect to halide potential and temperature for likely fuel and fission product components were mapped in Ellingham diagrams for the chloride and fluoride systems. The Ellingham diagrams provide a rich, visual means for identifying halide-forming components in proposed fuel/solvent salt systems. Thermochemical models and values from MSTDB-TC and ancillary sources were used in global equilibrium calculations to provide compositions for a close analysis of the behavior of a possible Molten Chloride Salt Fast Reactor and a Molten Salt Reactor Experiment-type system at high burnup (100 GWd/t). The results illustrated the oxidative nature of burnup in MSRs and provided information about redox behavior and possible control.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Measure the effect of molten halide salt exposure on creep rupture lifetime
Recent resurgence in the research and commercial interests in molten salt reactors (MSRs) as a viable advanced reactor concept to achieve the short- and long-term climate goals has resulted in ongoing efforts to demonstrate their commercial potential. These are relying on a combination of the extensive legacy knowledge from the molten salt reactor experiment (MSRE) and relatively recent data on materials compatibility of structural materials of interest such as 316H in molten salts environments. However, there is a critical lack of data on the mechanical behavior of alloys of interest for MSRS such as 316H, 617 and 709 in molten fluoride (FLiNaK or FLiBe) or chloride (NaCl-MgCl 2 ) salts. Limited legacy data from the molten salt reactor experiment (MSRE) program showed a significant reduction in creep rupture strength of a Ni-base alloy (Ni-15Cr-7Fe wt.%) in the molten fluoride NaF-ZrF4-UF4 (50-46-4 mol.%) salt. With ongoing efforts to commercialize different molten salt reactor concepts, the industry can considerably benefit from quantitative information on the impact of molten halide salts on the engineering properties such as creep and fatigue strength of materials of interest. Creep tests for 316H were conducted with fluoride (FLiNaK) and chloride (NaCl-MgCl 2 ) salts tat 650°C/150 MPa while alloys 709 and 617 were tested with FLiNaK at 700C/158 MPa and 750C.146 MPa respectively. Baseline tests were conducted in air to assess the impact of the molten salts on the creep behavior.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Measure the effect of molten halide salt exposure on creep rupture lifetime
Recent resurgence in the research and commercial interests in molten salt reactors (MSRs) as a viable advanced reactor concept to achieve the short- and long-term climate goals has resulted in ongoing efforts to demonstrate their commercial potential. These are relying on a combination of the extensive legacy knowledge from the molten salt reactor experiment (MSRE) and relatively recent data on materials compatibility of structural materials of interest such as 316H in molten salts environments. However, there is a critical lack of data on the mechanical behavior of alloys of interest for MSRS such as 316H, 617 and 709 in molten fluoride (FLiNaK or FLiBe) or chloride (NaCl-MgCl 2 ) salts. Limited legacy data from the molten salt reactor experiment (MSRE) program showed a significant reduction in creep rupture strength of a Ni-base alloy (Ni-15Cr-7Fe wt.%) in the molten fluoride NaF-ZrF4-UF4 (50-46-4 mol.%) salt. With ongoing efforts to commercialize different molten salt reactor concepts, the industry can considerably benefit from quantitative information on the impact of molten halide salts on the engineering properties such as creep and fatigue strength of materials of interest. Creep tests for 316H were conducted with fluoride (FLiNaK) and chloride (NaCl-MgCl 2 ) salts tat 650°C/150 MPa while alloys 709 and 617 were tested with FLiNaK at 700C/158 MPa and 750C.146 MPa respectively. Baseline tests were conducted in air to assess the impact of the molten salts on the creep behavior.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
First-of-a-Kind Fuel-bearing Molten Chloride Irradiation Experiment
As a dozen MSR developers in the U.S. work toward an aggressive commercialization timeline, many of their fueled-salts—notably, chloride-based compositions—have never been irradiated. Licensing and operating these reactors requires an understanding of (1) the source term, radiation chemistry, and gas generation; (2) unanticipated irradiation-induced corrosion effects; and (3) the impact of burnup on thermophysical properties, all of which can be deduced through irradiation testing. Idaho National Laboratory (INL) is ideally suited to leverage its expertise in chloride salt chemistry, as well as its Neutron Radiography Reactor (NRAD) facility in the Hot Fuels Examination Facility (HFEF) at the Materials and Fuels Complex (MFC), to conduct the world’s first fuel-bearing chloride salt irradiation and fill in the knowledge gaps pertaining to salt chemistry under irradiation. Molten-salt Research Temperature-controlled Irradiation (MRTI) consists of a salt-containing capsule that is internally heated inside of a secondary containment. The experiment must rely on resistive heating to melt the salt before irradiation (to avoid the impact of radiolysis) and once the reactor is turned on and fission reactions commence in the salt, the resistive power can then be reduced. Salt-immersed thermocouples coupled to a controller allow for the heater power to be adjusted as needed to meet experimental objectives. The bulk of the experimental results will be achieved through Post-Irradiation Examination (PIE). At which point a range of different measurements are anticipated to assess the salt/plenum/wall composition, the capsule corrosion rate, and the evolution of salt properties.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Synthesis and characterization of uranium trichloride in alkali-metal chloride media
Given a growing interest in uranium salts for pyrochemical processing of used fuel and uranium-fueled molten salt reactors, the synthesis of uranium trichloride in alkali-metal chloride media was investigated in a series of four experiments. Specifically, uranium metal powder and uranium hydride powder were prepared and separately blended with ammonium chloride and lithium chloride – potassium chloride eutectic in two runs, while the same powders were separately blended with ammonium chloride and sodium chloride in two additional runs. Each of the lithium chloride – potassium chloride containing blends was slowly heated to 923 K, while those containing sodium chloride were heated to 1123 K. During each heat up, the ammonium chloride sublimed into gaseous ammonia and hydrogen chloride, leading to the chlorination of uranium metal or uranium hydride and the formation of molten salt solutions of the respective chlorides. Experimental conditions were incorporated in the runs to promote formation of uranium trichloride over uranium tetrachloride in the respective media. Molten samples of each run product were taken and characterized via chemical analyses, diffractometry, and microscopy. The final products from each run were dark dense ingots of the respective salt systems with uranium concentrations ranging from 44 to 51 wt%. Finally, chemical analyses and diffractometry identified the predominant presence of uranium trichloride in these systems; however, a possible minor presence of uranium tetrachloride could not be conclusively dismissed.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Synthesis and characterization of uranium trichloride in alkali-metal chloride media
Given a growing interest in uranium salts for pyrochemical processing of used fuel and uranium-fueled molten salt reactors, the synthesis of uranium trichloride in alkali-metal chloride media was investigated in a series of four experiments. Specifically, uranium metal powder and uranium hydride powder were prepared and separately blended with ammonium chloride and lithium chloride – potassium chloride eutectic in two runs, while the same powders were separately blended with ammonium chloride and sodium chloride in two additional runs. Each of the lithium chloride – potassium chloride containing blends was slowly heated to 923 K, while those containing sodium chloride were heated to 1123 K. During each heat up, the ammonium chloride sublimed into gaseous ammonia and hydrogen chloride, leading to the chlorination of uranium metal or uranium hydride and the formation of molten salt solutions of the respective chlorides. Experimental conditions were incorporated in the runs to promote formation of uranium trichloride over uranium tetrachloride in the respective media. Molten samples of each run product were taken and characterized via chemical analyses, diffractometry, and microscopy. The final products from each run were dark dense ingots of the respective salt systems with uranium concentrations ranging from 44 to 51 wt%. Chemical analyses and diffractometry identified the predominant presence of uranium trichloride in these systems; however, a possible minor presence of uranium tetrachloride could not be conclusively dismissed.
D Herrmann, Steven↗
Predicting thermodynamic and thermophysical properties of molten chloride salts from ab-initio and classical molecular dynamics simulations
Molten salt reactors (MSRs) are among the advanced concepts pursued under the generation IV nuclear energy technology umbrella. However, the basic concept is not new and was first developed as part of the effort to power aircrafts with nuclear energy in the 1950’s. Later in the 1960’s, Oak Ridge National Laboratory (ORNL) built and operated the Molten-Salt Reactor Experiment (MSRE). This reactor used a fluoride salt with uranium as fuel. Fluorides salts are still highly relevant and proposed in several designs. In addition, chloride salts are being considered for MSRs operating in the fast neutron spectrum. This report focuses on chloride salts.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Optimal Chloride Salt Mixture for a Fusion Blanket
Deuterium-tritium fusion reactors cannot operate for a significant period without a closed tritium fuel cycle, according to a recent National Academies of Sciences (NAS) report on bringing fusion reactors to the US electrical grid. This fact places breeder blankets as one of the foundational systems for self-sustained fusion reactor operation. The typical functional requirements for a breeder blanket system include producing tritium, absorbing kinetic energy, transporting thermal energy, and being environmentally attractive. State-of-the-art research on liquid blankets has converged to primarily focus on (LiF) 2 and BeF 2 (FLiBe) molten salts and a metallic eutectic of lead and lithium (PbLi), but “virtually all of the technologies related to the tritium fuel cycle are at a low technological readiness level”. This work sought to explore optimum blanket configurations as it aligned with the Oak Ridge National Laboratory (ORNL) FY 2023 Laboratory Directed Research and Development Program’s research priority of developing and expanding the current understanding of fusion blanket science and technology. This purpose of this work was to address ORNL research priorities and NAS recommendations by investigating novel liquid blanket materials that could provide self-sustaining operation and draw on experience from research on molten salts used for advanced fission reactors, concentrated solar, and thermal energy storage. The hypothesis when proposing this research was that there could be chloride-based blanket designs that can exceed the tritium breeding ratios of (FLiBe) molten salt blankets while reducing the use of Be (FLiBe), avoiding the generation of HF (FLiBe), and minimizing magnetohydrodynamic (MHD)-perturbed flow fields (PbLi). The fastest and most cost-effective path to deploying liquid fusion breeder blankets could be from maximizing the synergistic technological overlap between fusion, fission, concentrated solar, and thermal energy storage industries.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Initial Engineering Framework for Species Tracking in MSRs Involving Fuel Salt and Structures
This report implements a high-fidelity multiphysics modeling framework using the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program tools to track leaching and plating of materials between the fuel salt and structures in Molten Salt Reactors (MSRs). Specifically, this framework is demonstrated in modeling various processes within MSRs including hot and cold leg corrosion, redox potential driven corrosion, colloid precipitation and deposition, and noble metal plating and decay heat modeling. The model integrates neutronics, thermal-hydraulics, depletion, and thermochemistry to simulate the evolving chemical behavior of the fuel salt in interactions with structural materials. Initial findings suggest that hot-cold leg corrosion in MSR systems may become significant if the redox potential of the fuel salt is not sufficiently controlled. Additionally, the impact of noble metal decay heat deposition in large power reactors is explored. The resulting engineering framework for species tracking will be applied in the future toward specific validation work with ongoing experimental efforts focusing on both chloride and fluoride salt loop experiments with in-situ corrosion and redox control instrumentation.
11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Design and Fabrication of a Temperature-Controlled Fueled Molten Salt Capsule Irradiation Experiment
Idaho National Laboratory (INL) is developing a Molten salt Research Temperature-controlled Irradiation (MRTI) experimental capsule for the Neutron Radiography (NRAD) reactor. The experiment is envisaged to be versatile and able to host a variety of salt-wall material combinations. The first test is designed to contain actinide-bearing chloride salt, which previously has not been subjected to a neutron field. The main objectives of the experiment are to produce irradiated salt samples for Post Irradiation Examination (PIE), to evaluate salt behavior under irradiation, and to test in-situ sensors/instrumentation. The final design for the experiment completed in 2022, and fabrication of the experiment is underway. The salt is double encapsulated providing insulation and redundancy in the case of leakage. A gas-gap between the inner capsule and the outer container enables tuning of thermal conduction to the NRAD coolant by altering its thickness and its gas-mixture. An inert gas mixture ratio in the gas-gap ensures the configurations reached a targeted average salt temperature of 600oC, while avoiding salt freezing or exceeding material limits. A resistive heater placed within a thermowell and controls the temperature of the experiment (both when the reactor is on or off). The selected configurations can contain over 10 cm3 of fuel-bearing chloride salt, which is sufficient for the purposes of the post-irradiation examination (PIE) and provides sufficient volume for two submerged thermocouple probes to monitor salt temperature. The capsule wall material is Inconel 625, and weld qualifications for the assembly have been developed. A glove-box laser weld technique was refined as part of this process to ensure a leak-tight assembly for the salt-bearing assembly and reduce the risks of impurities permeating into the salt. This work was supported through the INL Laboratory Directed Research & Development (LDRD) Program under DOE Idaho Operations Office Contract DE-AC07-05ID14517.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
ENYGF 2023 - Design of Temperature-controlled Fuel-salt Irradiation Experiment
Idaho National Laboratory (INL) is developing a Molten salt Research Temperature-controlled Irradiation (MRTI) experimental capsule for the Neutron Radiography (NRAD) reactor. The experiment is envisaged to be versatile and able to host a variety of salt-wall material combinations. The first test is designed to contain actinide-bearing chloride salt, which previously has not been subjected to a neutron field. The main objectives of the experiment are to produce irradiated salt samples for Post Irradiation Examination (PIE), to evaluate salt behavior under irradiation, and to test in-situ sensors/instrumentation. The final design for the experiment completed in 2022, and fabrication of the experiment is underway. The salt is double encapsulated providing insulation and redundancy in the case of leakage. A gas-gap between the inner capsule and the outer container enables tuning of thermal conduction to the NRAD coolant by altering its thickness and its gas-mixture. An inert gas mixture ratio in the gas-gap ensures the configurations reached a targeted average salt temperature of 600oC, while avoiding salt freezing or exceeding material limits. A resistive heater placed within a thermowell and controls the temperature of the experiment (both when the reactor is on or off). The selected configurations can contain over 10 cm3 of fuel-bearing chloride salt, which is sufficient for the purposes of the post-irradiation examination (PIE) and provides sufficient volume for two submerged thermocouple probes to monitor salt temperature. The capsule wall material is Inconel 625, and weld qualifications for the assembly have been developed. A glove-box laser weld technique was refined as part of this process to ensure a leak-tight assembly for the salt-bearing assembly and reduce the risks of impurities permeating into the salt. This work was supported through the INL Laboratory Directed Research & Development (LDRD) Program under DOE Idaho Operations Office Contract DE-AC07-05ID14517.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Neutron irradiation of alloy N and 316L stainless steel in contact with a molten chloride salt
Not Available
36 MATERIALS SCIENCE↗
Final report on assessment of molten salt corrosion testing of unirradiated and ion irradiated advanced manufactured high entropy alloys
Generation IV reactors and future fusion reactor designs have led to more demanding materials performance requirements due to their increased operating temperatures, corrosive coolants, and increased radiation doses compared to the current light-water reactor fleet. Among the innovative nuclear technologies under development, molten salt reactors stand out for their potential to offer superior fuel utilization, intrinsic safety characteristics, and economic viability. Of the proposed Generation IV designs, the gas fast reactor operates at 450 to 850°C and the molten salt reactor operates at 565 to 850°C, with the molten salt reactor design needing molten salt corrosion resistant materials [1, 2]. These increased temperatures and more extreme corrosion environments necessitate higher material performance, such as creep strength, radiation-tolerant microstructures, corrosion resistance, and high-temperature tensile properties. Hastelloy-N, a nickel-based alloy with additions of molybdenum and chromium, has been successfully employed to contain molten fluoride salt at temperatures up to 705°C. However, Hastelloy-N becomes embrittled upon neutron irradiation, primarily due to the accumulation of helium produced by (n,a) transmutation reactions. Furthermore, the corrosive nature of molten fluoride and chloride salts presents a formidable challenge, as these salts can react with and dissolve alloying elements such as Cr, Mo, and Fe, leading to selective leaching, loss of protective oxide layers, and accelerated degradation. High entropy alloys (HEAs) and refractory high entropy alloys (RHEAs) have emerged as a prominent area of interest, due to their ability to achieve tailored chemical compositions for specific applications. Unlike conventional alloys, HEAs are characterized by having multiple principal elements in equimolar or near equimolar ratios, leading to an unconventional alloying strategy [3]. This alloying strategy is believed to promote unique properties, such as single-phase stabilization of chemically compatible elements, lattice distortion effects due to atomic radius differences, and proposed sluggish diffusion effects. For extreme-environment applications, RHEAs have garnered much research interest because of the possibility of creating relatively ductile materials that can operate in extremely high-temperature environments, beyond the operating temperatures where other Ni-based superalloys begin to lose strength [4-6]. Idaho National Laboratory (INL) initiated a joint international effort with the Czech Republic to explore the feasibility of manufacturing HEAs for high-temperature nuclear applications using advanced manufacturing. This effort was funded at INL by the United States Department of Energy's Office of Nuclear Energy under the Advanced Reactor Technologies and Advanced Materials and Manufacturing Technologies (AMMT) Program. The HEAs were specifically designed for the corrosive and irradiation environments experienced in gas-cooled fast reactors, molten salt reactors, and fusion power. These alloys have been manufactured by multiple processes to determine the impact of manufacturing processes on the performance of the alloys in corrosive and irradiation environments. Preliminary molten salt corrosion testing showed that equimolar MoNbTiV and MoNbTi alloys exhibit exceptional performance, with arc-melted variants demonstrating only minimal degradation after 1000 hours of exposure to molten chloride salt at 700°C. Conversely, Nb2TiVZr2 showed significant molten salt corrosion susceptibility and microstructural instability during high-temperature molten salt exposures, and was, therefore deemed unfit for molten salt reactor applications. The MoNbTiV, MoNbTi, and Nb2TiVZr2 alloys were further evaluated through ion irradiation experiments conducted at the Michigan Ion Beam Laboratory at the University of Michigan. The microstructural stability and the evolution of irradiation-induced defects were characterized to assess the irradiation resistance of each of these alloys.
36 - MATERIALS SCIENCE↗
Characterization of Fe and Cr Dissolution and Reaction Product Formation in Molten Chloride Salts With and Without Impurities
There is considerable interest in molten chloride salts for several applications including thermal storage and next-generation molten salt reactors (MSRs). Several studies have concluded that Cl salts are highly corrosive to structural materials. Using Oak Ridge National Laboratory’s established methodology, Cl salt compatibility was assessed for candidate Ni-based alloys 230, 600 and 740 H at 600°–800°C in static welded capsules and in flowing thermal convection loop (TCL) salt experiments. Simply drying commercial Cl salt at 550°–650°C and adding~0.05 wt.%Mg was able to produce small specimen mass changes and limited surface attack after 100–1000 h exposures. Intentional additions of H 2 O, NiCl 2 and undried salt were used to better understand the role of impurities and achieve the>50 µm levels of attack reported in other studies. Further, characterisation of Cr depletion and oxide formation in conjunction with pre- and post-test salt chemistry measurements are being used to understand salt compatibility of structural materials.
36 MATERIALS SCIENCE↗