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At least 19 records

Liquid centrifugation-based isotope separation of 7 Li, 37 Cl and D

Liquid centrifugation is an emerging method to separate isotopes. By spinning a liquid containing target isotopes (e.g., pure chemical or solution), the heavier isotope will be enriched at the outer part of a centrifuge, and the lighter ones will be enriched at the inner part of a centrifuge. The separation capability is positively correlated with rotation speed, outer radius and mass difference between isotopes to separate. This award targets to understand whether liquid centrifugation is effective in separating isotopes important for nuclear fission technologies. The results include the following three sections: 1) Effects of solute concentration on isotope separation; 2) Preliminary progress of building a low-speed countercurrent centrifuge, and 3) Analysis on possible candidates for 7 Li and 37 Cl. The award trained one research scientist, one Ph.D. student, one master student, and one undergraduate on liquid centrifugation and isotope measurements.

07 ISOTOPE AND RADIATION SOURCES↗

Liquid solution centrifugation for safe, scalable, and efficient isotope separation

A general method of separating isotopes by centrifuging dissolved chemical compounds in a liquid is introduced. This technique can be applied to almost all elements and leads to large separation factors. The method has been demonstrated in several isotopic systems including Ca, Mo, O, and Li with single-stage selectivities of 1.046 to 1.067 per neutron mass difference (e.g., 1.43 in 40 Ca/ 48 Ca), which are beyond the capabilities of various conventional methods. Equations are derived to model the process, and the results agree with those of the experiments. The scalability of the technique has been demonstrated by a three-stage enrichment of 48 Ca with a total 40 Ca/ 48 Ca selectivity of 2.43, and the scalability is more broadly supported through analogies to gas centrifuge, whereby countercurrent centrifugation can further multiply the separation factor by 5 to 10 times per stage in a continuous process. Optimal centrifuge conditions and solutions can achieve both high-throughput and highly efficient isotope separation.

07 ISOTOPE AND RADIATION SOURCES↗

Simulation studies for beam commissioning at FRIB Advanced Rare Isotope Separator

The Facility for Rare Isotope Beams (FRIB) includes a powerful superconducting driver accelerator and an Advanced Rare Isotope Separator (ARIS). The ARIS collects and purifies the rare isotope fragments of interest for experiments in nuclear physics, nuclear astrophysics, fundamental symmetries, etc. ARIS consists of a vertical pre-separator and downstream horizontal separator section (C-Bend). Each section can provide a high-resolution separation alternatively. The resolution reduction due to the emittance induced by momentum compression can be avoided by isotope separation in different dispersive planes. Beam commissioning of ARIS for the first experiments was completed and demonstrated particle identification of fragments. The beam tuning in ARIS largely relies on numerical simulations since the limited space for diagnostics. Here, we report the result of the beam trajectory correction, transverse matching, and beam-based misalignment studies at ARIS.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

An Overview of the Radioisotope Electromagnetic Isotope Separation Capabilities at Idaho National Laboratory

Electromagnetic isotope separation (EMIS) has been an effective tool for the enrichment of isotopes for over 80 years. In the early 1990’s the U.S. reduced or eliminated electromagnetic isotope separation capabilities, but in the last decade, increased demand for both stable and radioactive enriched isotopes have led to the reestablishment of small-medium scale EMIS capabilities in the U.S. National Laboratory Complex.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Advanced Isotope Separation Technology for Fusion Fuel

Deuterium-tritium fusion is the easiest nuclear fusion reaction among known fusion reactions. Since tritium is extremely rare, it is artificially produced by irradiating lithium metal. The separation, isolation, and storage of the tritium isotope has been a major focus of the Savannah River Site (SRS) for many decades. Thermal diffusion, fractional absorption, and cryogenic distillation have all been used in the past, and each has significant operational and safety challenges. A process known as the Thermal Cycling Absorption Process (TCAP) was invented at SRS, and because of its overwhelming advantages in safety, efficiency, size, and reduced tritium inventory, it has replaced all other hydrogen isotope separation processes at SRS. Here, the working principles and current development of hydrogen isotope separation using TCAP at SRS are explained as a potential advanced isotope separation process for the fusion fuel cycle.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Modeling Isotope Separation in Electrochemical Lithium Deposition

Naturally occurring Li consists of two stable isotopes, 6 Li with an abundance of about 7.5%, and 7 Li making up the remainder with 92.5%. The development of a 6 Li enrichment technique, in terms of technical reliability and environmental safety to reach 6 Li future requirements, represents a key step in the roadmap for nuclear fusion energy supply worldwide. This paper uses finite element analysis-based models to simulate electrochemical Li isotope separation, which is an attractive method in terms of simplicity, safety, and scalability. In the model, we quantitatively analyze how different electrochemical factors including thermodynamics, charge-transfer kinetics, and diffusivities affect the separation process (separation factor), together with cell parameters, such as cell length and current density. The maximum separation factor of 1.128 could be obtained with the cell under the optimal thermodynamic, kinetic, and diffusive conditions, which is among the highest separation factors ever reported. Furthermore, these results will assist in designing the actual isotope separation setup with large separation factor and appropriate timing for sample collection.

07 ISOTOPE AND RADIATION SOURCES↗

Hydrogen isotope separation methods and systems

Methods and systems for the separation of hydrogen isotopes from one another are described. Methods include utilization of a hydrogen isotope selective separation membrane that includes a hydrogen isotope selective layer (e.g., graphene) and a hydrogen ion conductive supporting layer. An electronic driving force encourages passage of isotopes selectively across the membrane at an elevated separation temperature to enrich the product in a selected hydrogen isotope.

07 ISOTOPE AND RADIATION SOURCES↗

Toward Hydrogen Isotope Separations through Strong Hydrogen Adsorption at Open Copper(I) Sites in an Ultramicroporous Metal-Organic Framework

Metal-organic frameworks with coordinatively unsaturated metal sites (open metal sites) capable of engaging in orbital interactions with pi-acidic gases are of interest for enabling ambient-temperature gas separations, such as hydrogen isotope separations. In view of the weakly pi-acidic nature of H2, we sought to strengthen pi-backbonding-mediated H2 adsorption through pore confinement effects. Toward that end, we synthesized and characterized the ultramicroporous metal-organic framework CuxZn5-xCl4-yHz(bbta)3 (CuIZn-MFU-4; H2bbta = 1H,5H-benzo(1,2-d:4,5-d')bistriazole), featuring pi-basic trigonal pyramidal CuI sites that reside within 7 A of one another at their closest. Gas adsorption measurements reveal an H2 adsorption enthalpy of -38 kJ/mol, exceeding that of the larger-pore analog (CuIZn-MFU-4l; -33 kJ/mol) and representing the strongest H2 adsorption yet achieved in a metal-organic framework. The stronger H2 adsorption in CuIZn-MFU-4 is attributed to a combination of pore confinement effects and the increased ..sigma..-accepting nature of the CuI sites caused by a more electron-withdrawing bbta2- linker, as supported by structural, spectroscopic, and computational evidence. With the strongest H2 adsorption, equilibrium isotope effects in CuIZn-MFU-4 lead to a D2/H2 selectivity (as estimated by ideal adsorbed solution theory) of 1.35 even at 298 K, approaching the values reported below 200 K for conventional porous materials.

08 HYDROGEN↗

Measurement of isotopic separation of argon with the prototype of the cryogenic distillation plant Aria for dark matter searches

The Aria cryogenic distillation plant, located in Sardinia, Italy, is a key component of the DarkSide-20k experimental program for WIMP dark matter searches at the INFN Laboratori Nazionali del Gran Sasso, Italy. Aria is designed to purify the argon, extracted from underground wells in Colorado, USA, and used as the DarkSide-20k target material, to detector-grade quality. In this paper, we report the first measurement of argon isotopic separation by distillation with the 26 m tall Aria prototype. We discuss the measurement of the operating parameters of the column and the observation of the simultaneous separation of the three stable argon isotopes: ${}^{36}\hbox {Ar}$, ${}^{38}\textrm{Ar}$, and ${}^{40}\textrm{Ar}$. We also provide a detailed comparison of the experimental results with commercial process simulation software. This measurement of isotopic separation of argon is a significant achievement for the project, building on the success of the initial demonstration of isotopic separation of nitrogen using the same equipment in 2019.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Chlorine Isotope Separations using Thermal Diffusion

As of the close of 2023 a thermal diffusion isotope separations (TDIS) apparatus was constructed, successful shakedown testing was achieved and enrichments of isotopic concentrations relative to natural abundance 35/37 Cl were collected. Further, the model for these enrichment experiments drove the timing for sampling and other critical, extrapolated functions that are discussed herein. Our decision to move forward in 2024 with the installation of a larger set of separation tubes and associated equipment was based on the successful development of the predictive model. The Chlorine Isotopes Project Team at PNNL is prepared to claim that the installation and hence its separative power is restricted only by the spatial limitations of the laboratory, and this at present appears to be the limiting feature to first pass high enriched 37 Cl.

07 ISOTOPE AND RADIATION SOURCES↗

Commissioning of the Advanced Rare Isotope Separator ARIS at FRIB

The Facility for Rare Isotope Beams (FRIB) at Michigan State University (MSU) consists of a newly constructed linear accelerator and fragment separator that are designed for enhanced production rates of rare isotopes for use in research and other societal applications. Recent activities through to August 2022 took place to commission the Advanced Rare Isotope Separator (ARIS) and carry out the first experiments. This followed commissioning of the newly constructed linac that is designed to provide orders of magnitude higher beam power than the previously coupled cyclotrons. This required that more advanced target, beam dump, and collimation systems of the new separator be designed and constructed to sustain unprecedented conditions by heavy ion beams. Commissioning with ~1 kW beams began recently and results from activities that began in late 2021 are reported here. Comparisons between the previous and current facilities are provided.

43 PARTICLE ACCELERATORS↗

Comparison of Designs of Hydrogen Isotope Separation Columns by Numerical Modeling

Mixtures of gas-phase hydrogen isotopologues (diatomic combinations of protium, deuterium, and tritium) can be separated using columns containing a solid such as palladium that reversibly absorbs hydrogen. A temperature-swing process can transport hydrogen into or out of a column by inducing temperature-dependent absorption or desorption reactions. Here, we consider two designs: a thermal cycling absorption process, which moves hydrogen back and forth between two columns, and a simulated moving bed (SMB), where columns are in a circular arrangement. We present a numerical mass and heat transport model of absorption columns for hydrogen isotope separation. It includes a detailed treatment of the absorption–desorption reaction for palladium. By comparing the isotope concentrations within the columns as a function of position and time, we observe that SMB can lead to sharper separations for a given number of thermal cycles by avoiding the remixing of isotopes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Benchmarking Hydrogen Isotope Separation Efficiency of Pd/k–Packed TCAP Columns

By leveraging the large isotope effect in the palladium hydrogen isotope system, the Thermal Cycling Absorption Process (TCAP) provides an efficient and advantageous means to separate protium, deuterium, and tritium. To meet increased future tritium processing demands, such as those needed for fusion power plants, current designs of the separation columns need to be adapted and optimized using the progress made in understanding hydrogen isotope science. One key to this optimization lies in understanding the baseline performance for currently employed separation packing materials. Pd/k and molecular sieves, as commonly used for the separation of hydrogen isotopes, are herein evaluated to establish a baseline for their separation efficiency. Van Deemter plots are formulated, and the influence of each parameter is evaluated to determine areas for improvement.

Thermal Cycling Absorption Process (TCAP)↗

Systems for separating isotopes from a sample of fission products

Systems and methods for efficient, effective, and safe separation and isolation of multiple isotopes (e.g., Mo, Zr, Ba, Sr, Te, and lanthanide isotopes) from fission products includes use of a plurality of chromatography columns, each containing a chromatographic resin formulated to target one or more particular isotopes. The system is operable in a “series” configuration to load the multiple columns by a single pass of the sample. Then, the system may be transitioned (e.g., using valves) to a “parallel” configuration in which multiple columns of the system may be operated simultaneously to elute targeted isotopes. Additional parallel operations of the columns, using different eluent compositions, may be used to elute different targeted isotopes. The system may be reconditioned in preparation for a subsequent sample.

Snow, Mathew S.↗

CO 2 electroreduction favors carbon isotope 12 C over 13 C and facilitates isotope separation

We discovered that CO 2 electroreduction strongly favors the conversion of the dominant isotope of carbon ( 12 C) and discriminates against the less abundant, stable carbon 13 C isotope. Both absorption of CO 2 in the alkaline electrolyte and CO 2 electrochemical reduction favor the lighter isotopologue. As a result, the stream of unreacted CO 2 leaving the electrolyzer has an increased 13 C content, and the depletion of 13 C in the product is several times greater than that of photosynthesis. Using a natural abundance feed, we demonstrate enriching of the 13 C fraction to ~1.3% (i.e., +18%) in a single-pass reactor and propose a scalable and economically attractive process to yield isotopes of a commercial purity. Our finding opens pathways to both cheaper and less energy-intensive production of stable isotopes ( 13 C, 15 N) essential to the healthcare and chemistry research, and to an economically viable, disruptive application of electrolysis technologies developed in the context of sustainability transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Chlorine isotope separations using thermal diffusion

In a chloride molten salt fast reactor (Cl-MSFR), the fuel salt might be comprised of a specific eutectic composition of alkali and alkaline chlorides that solubilize major and minor actinide chlorides as the fertile component(s). Each of the chloride species contain the natural abundance ( 35 Cl ~76% and 37 Cl ~24%) of the two stable isotopes of chlorine 35 Cl and 37 Cl. There has been an ongoing controversy for the operation of the Cl-MSFRs concerning the potential of the 35 Cl(n,γ) 36 Cl, 35 Cl(n,p) 35 S, 35 Cl(n,α) 32 S reactions to produce 36 Cl, 32 S, and 32 P at relevant energies [Bulmer 1956]. The undesirable attributes of irradiated 35 Cl are enumerated further below.

07 ISOTOPE AND RADIATION SOURCES↗