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At least 19 records

Development Efforts for Detritiating Legacy Heavy Water Moderator

Conclusions • Department of Energy is evaluating reclaiming contaminated heavy water to commercial virgin heavy water specifications • SRNL evaluated leading commercial technologies to detritiate heavy water • To minimize the process hazards, water distillation was proposed as the best candidate • Addition of LPCE and cryogenic distillation can help process 100% of water with little to no waste storage • Significant advances over the past 40 years, but demonstration system needed to prove necessary detritiation factors for heavy water

Angelette, Lucas M. [Savannah River National Labor↗

CNL Technologies for Heavy Water Detritiation - 19437

Canadian Nuclear Laboratories (CNL) is responsible for a large amount of heavy water owned by the Government of Canada. A significant portion of this heavy water has been downgraded and is chemically and/or radiologically contaminated (besides tritium). Storage, monitoring and disposal of this water incurs significant costs. Upgrading following chemical purification (including removal of radionuclides other than tritium) of this water is feasible with commercial processes. However, removal of the tritium to the level that would allow the heavy water to be available for non-nuclear applications requires very specialized processes. CNL has developed and demonstrated the Combined Electrolysis and Catalytic Exchange (CECE) detritiation technology to reduce the tritium to the level at which the heavy water can be classified as non-radioactive. The CECE process consists of a Liquid Phase Catalytic Exchange (LPCE) bed, where the transfer of hydrogen isotopes between water and gaseous hydrogen occurs, and an electrolysis cell (E-cell) that produces hydrogen and separates the isotopes of hydrogen, adding to the enrichment achieved in the LPCE catalyst bed. The application of the CECE technology to the tritium-contaminated heavy water would restore its full market value. As part of a project supported by CNL Decommissioning and Waste Management, a business case is being developed to build and operate a facility that will purify and detritiate heavy water to render it commercially attractive. The main goal of the current study is to evaluate the net benefits of detritiation and product sale versus the cost of permanent storage or disposal. Such a facility would not only eliminate the need to store the heavy water as a radioactive waste material and provide revenue, but would also serve as a demonstration of CNL's technology for similar applications elsewhere. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Detritiation and Recovery of Heavy Water Moderator for Commercial Use

Historical Inventory Savannah River Site hosted five tritium production reactors from the 1950s through 1990s • Pressurized heavy water reactor • D2O moderator • Approximately 1900 m3 of legacy moderator water is in storage • Ranges from 1% D2O to 99.8% D2O • Varying amounts of tritium, relatively low amounts of other radioactive elements • Due to shortage in D2O production, US Department of Energy is investigating detritiating the heavy water for commercial uses

Angelette, Lucas M. [Savannah River National Labor↗

Physics analysis and design of heavy water reflected thermal test reactor

Here, this work investigates the option of modifying the Advanced Test Reactor by replacing the current beryllium reflector with heavy water. Such a change may provide some potential benefits for not only increasing the thermal irradiation capabilities but also resolving other problems such as reflector integrity issues due to fast fluence damage, which is always a limiting factor in the lifetime of the current beryllium reflector. This paper presents the analysis and estimation of the ATR core physics parameters by replacing the current beryllium reflector with heavy water (D 2 O). The paper first describes the details of two selected conceptual designs, which are partially reflected with either beryllium or graphite, and how they are derived from the baseline beryllium reflector concept. Then, reactor physics performance parameters for the two new concepts are assessed by comparing with those of the baseline concept. The performance parameters considered in this paper include in-pile tube neutron and gamma fluxes and heating rates, maximum loop voiding reactivity, core power behavior with different power splits, predicted cycle length with a given fuel loading, and thermal hydraulic analysis with a higher lobe power split. It is important to note that this study focuses on the reactor physics aspects and does not delve into the engineering challenges associated with such a design modification.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Advanced Fuel Cycle Cost Basis Report: Module D1-7 Contact-Handled Pelletized Pressurized Heavy Water (PHWR) UOX Fuel Fabrication (Rev.1)

In addition to literature-based pressurized heavy-water reactor (PHWR) fuel price information in the 2017 AFC-CBR, the what-it-takes (WIT) unit cost data in this update is informed by new analysis and escalation of the 1978 PHWR-UOX fuel life cycle cost (LCC) data from ORNL reports prepared for the 1977–1980 Nonproliferation Alternative Systems Assessment Program (NASAP). (These reports are referenced and summarized in detail in Module D1-PR.) The PHWR fuel fabrication LCC data in these reports is scaled from a bottom-up cost estimate for a reference technology pressurized-water reactor (PWR)—uranium oxide (UOX) fuel fabrication plant by using algorithms that consider the manufacturing process complexity, fuel design complexity, plant floor space requirements, and the radiation and health, safety, and environmental (HS&E) regulatory environment of PHWR-UOX fuel production vis-à-vis light-water reactor (LWR)-UOX production (PWR fuel in this case). The module name has been changed from “Canadian Deuterium Uranium (CANDU)” to the more generic PHWR fuel fabrication in recognition that not all power reactors that might use this fuel type are considered. Unfortunately, the detailed algorithms and their design bases were not archived at the end of the NASAP effort of the commercial CANDU concept specifically developed in the middle of the last century by Atomic Energy of Canada Limited (AECL).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High-repetition-rate, multi-MeV deuteron acceleration from converging heavy water microjets at laser intensities of 10 21 W/cm 2

Herein we demonstrate high repetition-rate deuteron acceleration by irradiating a continuously flowing, ambient temperature liquid heavy water jet with the high-intensity ALEPH laser. The laser delivered up to 5.5 J (120 TW, 1.2 × 10 21 W/cm 2 ) laser energy on target at 0.5 Hz. A high repetition-rate Thomson parabola spectrometer measured the deuteron beam energy spectra on each shot for 60 sequential shots (two minutes). Peak fluxes of 5 x 10 10 deuterons/sr/pulse, corresponding to an average flux of 1.5 x 10 12 deuterons/sr/min, were demonstrated with deuteron energies reaching up to 4.4 MeV. High shot-to-shot stability is observed up to 40%–50% of the maximum deuteron energy. These deuteron beams are suited for fast neutron production through deuteron breakup in a converter yielding energies similar to deuteron–deuteron (D–D, 2.45 MeV) fusion reactions of importance for material damage studies.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Study of the potential for improving the economics of hydrogen liquefaction through the use of centrifugal compressors and the addition of a heavy water plant

An approach to the liquefaction of hydrogen was developed which permits the application of standard centrifugal compressors in place of reciprocating machines. A second fluid, such as propane, is added to the hydrogen prior to compression to form a mixture having a molecular weight much greater than that of hydrogen alone, so that a standard centrifugal compressor can be used. After compression, the mixture is cooled to cryogenic temperature levels where the propane condenses out of the mixture and is separated as a liquid. Since a small amount of deuterium is produced during hydrogen liquefaction, the potential of recovering deuterium and selling it as a co-product was investigated. Deuterium, in the form of heavy water, can be used in certain nuclear reactors as a neutron moderator to reduce the neutron velocity and enhance the probability of neutron collision with uranium nucleii.

Baker, C. R.↗

Stratospheric profiles of heavy water vapor isotopes and CH3D from analysis of the ATMOS Spacelab 3 infrared solar spectra

The isotopic composition of stratospheric water vapor and methane was investigated. Stratospheric profiles of HDO, (H-18)2O, (H-17)2O, and CH3D were derived from solar occultation spectra recorded on April 30 - May 1, 1985 by the Atmospheric Trace Molecule Spectroscopy Fourier transform spectrometer aboard Spacelab 3. The profiles of the three water-vapor isotopes showed an increase in the volume mixing ratio with altitude. The measured profiles of D/H in water vapor showed a large depletion in the lower stratosphere (about 63 percent relative to standard mean ocean water, SMOW, at 20 km) and a small increase in D/H with altitude at higher altitudes, up to 34 km. The D/H ratio in stratospheric methane was close to the corresponding isotopic ratio in SMOW.

Rinsland, C. P.↗

Isotope effects on the high pressure viscosity of liquid water measured by differential dynamic microscopy

In this paper, differential dynamic microscopy is performed in diamond anvil cells to measure the viscosity of water along the 24 °C isotherm to high-pressure by determination of the tracer diffusion coefficient of monodisperse silica spheres of known diameter and application of the Stokes-Einstein-Sutherland equation. This technique allows liquid samples to be compressed to greater pressure prior to freezing than with other viscometry methods. The highest-pressure measurement was made at 1.67 GPa, considerably deeper into the supercompressed regime than previously reported. The effect of isotopic composition is investigated with samples of normal water, heavy water, and partially deuterated water. When data below 0.25 GPa are excluded a free volume model fits the observed viscosities well yielding a theoretical glass transition density close to that observed in very-high-density amorphous ice. The improved fit above 0.25 GPa coincides with the loss of other anomalous behaviors in liquid water caused by hydrogen bonding and represents a transition to properties closer to those of a simple liquid.

74 ATOMIC AND MOLECULAR PHYSICS↗

Reflectance of aqueous solutions

The optical properties and optical constants of water and aqueous solutions were studied to develop an accurate tabulation of graphical representations of the optical constants through a broad spectrum. Manuscripts of articles are presented concerning extinction coefficients, relative specular reflectance, and temperature effect on the water spectrum. Graphs of absolute reflectance, phase shifts, index of refraction, and extinction coefficients for water, heavy water and aqueous solutions are included.

Querry, M. R.↗

Effect of water on carbon monoxide-oxygen flame velocity

The flame velocities were measured of 20 percent oxygen and 80 percent carbon monoxide mixtures containing either light water or heavy water. The flame velocity increased from 34.5 centimeters per second with no added water to about 104 centimeters per second for a 1.8 percent addition of light water and to 84 centimeters per second for an equal addition of heavy water. The addition of heavy water caused greater increases in flame velocity with equilibrium hydrogen-atom concentration than would be predicted by the Tanford and Pease square-root relation. The ratio of the flame velocity of a mixture containing light water to that of a mixture containing heavy water was found to be 1.4. This value is the same as the ratio of the reaction rate of hydrogen to that of deuterium and oxygen. A ratio of reaction rates of 1.4 would also be required for the square-root law to give the observed ratio of flame-velocity changes.

Mcdonald, Glen E↗

Preparative cell electrophoresis at 1 and 0 gravity

It is attempted to show that the use of heavy water (D2O) as starting cushion for the cells combines the advantages of the required density difference, with no lasting biochemical or physiochemical influence on the cells. Phosphate buffers of low ionic strength were prepared in distilled water or heavy water. A vertical starch gel electrophoresis was used to support a cylindrical polystyrene electrophoresis tube used for lymphocyte separations, 25 cm in length and 0.75 cm I.D., prepared from a 10 ml disposable pipet. Erythrocyte separations were carried out in a jacketed rectangular plexiglas chamber. It is pointed out that the described preparative D2O gradient electrophoresis method cannot be readily used for the measurement of electrophoretic mobilities for analytical purposes. However, for the preparative separation of cells with only slightly different electrokinetic properties the method appears promising, simple, and entirely inocuous to the cells.

Van Oss, C. J.↗

Minimization of Nuclear Waste using AHWR Reactor Technology

Nuclear sciences have grown from creating reactors to a greater understanding of how to dispose off the waste exhibited by the nuclear activities. Various methodologies have been proposed and are being used in order to do the same. This poster poses great attention to 'Using a fuel cycle dedicated to the production of the lower quantity of minor actinides, is one of the key targets in reducing nuclear waste in india'. A significant fraction of thorium is utilized as a fertile host in the Advanced Heavy Water Reactor (AHWR300-LEU) fuel. Being lower in the periodic table, it leads to a reduction of minor actinides. It produces only half of the minor actinides as a waste as compared to modern LWRs. As thorium oxide has inert nature, it benefits in its prolonged storage. Therefore, safe disposal of spent fuel is achieved due to the inert matrix, on completion of one fuel cycle mode. AHWR is a 300 MWe, vertical, pressure-tube type, boiling light water-cooled, and heavy water-moderated reactor. Employs natural circulation for removal of heat from the reactor core. In-situ conversion of {sup 232}Th into {sup 233}U. The reactor design permits flexible fuel cycle options. There are two types of AHWR depending upon the fuel cycle options. Uses thorium-based oxide fuels: two fuel cycle options. With the adoption of thorium fuel cycle, AHWR300-LEU produces less minor actinides. As compared to modern LWRSs, it produces almost 37% less amount of actinides for the same amount of energy production, which in turn minimizes the burden on waste disposal requirements. But, it is associated with radionuclides such as {sup 231}Pa (produced through absorption of one neutron and emission of two neutrons). Since, the reaction rate of (n,2n) reactions is very low in thermal neutron reactors, thus making the fuel cycle the favorable one. Thorium oxide (ThO{sub 2}) is chemically stable and is the highest oxidation state of thorium, therefore the inert nature of the matrix is advantageous for safe disposal of spent fuel in case of adoption of open fuel cycle mode and offers prolonged storage of spent fuel. The AHWR is thorium fueled Indian nuclear reactor that assimilates several new features with diminished environmental concern due to reduced waste generation. Since thorium fuel cycle produces less long lived nuclear waste, thus it can possibly bring the world cleaner and more sustainable nuclear energy. Currently, India being the only country with large scale research program of thorium nuclear power serves a platform for the development and demonstration of all technologies and advanced safety systems.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The Ionization Constants of DCO{sub 3}{sup -} and DPO{sub 4}{sup 2-} under Candu Reactor Primary Coolant Conditions by Raman Spectroscopy

The ionization constants of bicarbonate and hydrogen phosphate have been measured in light and heavy water up to 325 deg. C using Raman spectroscopy. Ionization constants in heavy water at temperatures above 100 deg. C have been measured for very few acids and bases. Together with other results, this work will be used to develop and verify models of the deuterium isotope effect on oxide solubilities in Candu reactor primary coolant. A custom-built titanium/sapphire flow cell was paired with a Horiba Jobin Yvon HR800 LabRAM system to collect Raman spectra of aqueous solutions under Candu primary coolant temperatures. The temperature-controlled cell is made of materials that are relatively inert under the extreme experimental conditions required for hydrothermal studies. Raman spectra were collected with detector polarizations parallel and perpendicular to the laser polarization. These were subtracted and corrected to obtain the reduced isotropic spectrum, which contains only symmetric vibrations, has a flat baseline, and has peak areas proportional to species concentration. Vibrational modes involving deuterium are shifted to lower wavenumbers in heavy water due to the increased mass of deuterium over hydrogen. The speciation between the two solvents is also measurably different. The relative concentration of the acidic species in solution increases with temperature, making its peaks easier to fit at high temperatures. The Raman band positions shift to lower wavenumbers with increasing temperature because the hydrogen bonding in bulk water begins to break down, which strengthens hydrogen bonding to the ions. The basic equilibrium constants were determined from the concentration of each species in solution combined with an activity coefficient model. A simplified form of the 'density' model was then fitted to the data. These fit results were combined with literature values of pK{sub w} in light and heavy water to determine the pK{sub a} values at saturation vapor pressure. The experimental results show excellent agreement with known literature values in light water where they exist at lower temperatures. These equilibrium constants are the first to be reported for both chemical systems in heavy water above 25 deg. C. This work extends the equilibrium constants in H{sub 2}O: - For HCO{sub 3}{sup -} from 250 deg. C to 325 deg. C; - For HPO{sub 4}{sup 2-} from 50 deg. C to 300 deg. C. These are the first ever ionization constants in D{sub 2}O for DPO{sub 4}{sup 2-} and the first values above 25 deg. C for DCO{sub 3}{sup -}. These results will be used to develop predictive models for the deuterium isotope effect on activated corrosion product transport under Candu nuclear reactor primary coolant conditions.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Characterization of C-Reactor (105-C) Moderator Tanks 204 and 205

Area Completion Project (ACP)/Savannah River Nuclear Solutions (SRNS) has requested Savannah River National Laboratory (SRNL) to perform chemical and radiological analyses on moderator heavy water samples from C-Reactor (105-C) in Moderator Tanks 204 and 205. The heavy water samples have been characterized using SRNL analytical methods. Information generated from the characterization of these heavy water samples provide a basis for determining the residual contamination remaining in the tanks. These analyses are needed in order to update the C-Reactor Contaminant migration groundwater model and report, to help determine a disposition pathway for the moderator water, and to ship samples off-site to the Southwest Research Institute (SWRI). This report presents characterization results for the March 2024 C-Reactor Moderator Tank 204 and 205 heavy water samples. SRNL results are critical to allow ACP to complete this Performance Based Incentive project on time. Based on the characterization data provided in this report, results of these samples meet customer expectations and satisfy the Technical Assistance Request (TAR).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗