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Liezers, Martin

Publications and source records attributed to Liezers, Martin.

Micro-Quantification of Helium-3 and Helium-4 in TPBAR Components

This report documents the method development for measuring helium isotopes in micrometer-sized samples of tritium producing burnable absorption rod (TPBAR) components. Helium isotopes were measured as a tracer for tritium, which decays to 3 He with a half-life of 12.33 years. Getter and cladding materials from the TPBARs were analyzed, as they are designed to trap tritium. Therefore, constraining the diffusivity of tritium through these materials is of key importance. To first establish the reliability of the noble gas mass spectrometer, a reference gas with a relative 4 He/ 3 He ratio of 1000 was pre-mixed. This standard was measured several times to ensure measurements were reproducible. Unirradiated and irradiated getter and cladding samples of TPBARs were cut into 1-100 µm 3 cubes and analyzed for 3 He and 4 He content. The unirradiated materials had helium content equal to or less than that of the measured instrument background. Irradiated cladding also had instrument background levels of helium while irradiated getters had elevated levels of 3 He, interpreted to be the decay product of tritium. No diffusion of 4 He was observed in any of these materials, however, indicating that the 3 He detected in the irradiated getter was produced in situ after tritium diffusion and decay. These findings validate this method as a way to trace tritium diffusion in reactor materials.

07 ISOTOPE AND RADIATION SOURCES↗

Particulate mass migration and mixing in cylindrically contained explosions

Abstract To explore particulate movement near the plasma of chemical explosions, rugged tracer particles were placed within and on the exterior of metal charges and electrically detonated. The particles were collected on/in the porous walls of plastic cylinders at diameters that correlated to the plasma width during different phases of the explosion. The particles’ positions were determined by Boolean logic analysis of their luminescent intensity. The cylinders which caught particles from the initial phases of the explosion retained placement information, while wider cylinders showed uniform mixing. These results/analysis methodology can help improve the understanding of particulate mixing in harsh environments. Graphical abstract

36 MATERIALS SCIENCE↗

R-Value Measurements Performed on Actinide Targets Irradiated using the GODIVA IV Critical Assembly in FY22

The separation and characterization of two irradiated uranium targets, a depleted uranium (DU) and a highly enriched uranium (HEU) target as well as a plutonium (Pu) target, was conducted in April of 2022. The three targets were assembled at Los Alamos National Laboratory (LANL) and irradiated using the GODIVA critical assembly at the National Criticality Experiments Research Center (NCERC). Splits of the dissolved targets were received by Pacific Northwest National Laboratory (PNNL) after which the PNNL and LANL teams chemically separated the solutions using independent separation schemes and analyzed the separated fractions for short lived actinides and fission products. Chemical separations were traced with stable or radioactive tracers to allow for the determination of chemical yields, analyzing using either inductively coupled plasma optical emission spectroscopy (ICP-OES), inductively coupled plasma mass spectrometry (ICP-MS) or gamma emission analysis (GEA) depending on the nature of the tracer. The Pu target solution was traced with stable elements at LANL to follow elemental fractionation during a Pu removal step. Many analytical techniques were used by PNNL including kinetic phosphorescence analysis (KPA), ICP-OES, ICP-MS, GEA, and thermal ionization mass spectrometry (TIMS) depending on the analyte’s need.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Hydrothermal Liquid Recovery of Rare Earth Elements and Critical Materials

This project demonstrated the technical viability of using tunable hydrothermal liquid (HTL) solutions to recover valuable minerals from a range of source materials. The effort focused upon rare earth elements (REE) and other minerals critical to the industrial security of the United States. This effort demonstrated, for the first time, that s, supercritical water (SCW) in particular, can: Extract critical and valuable minerals from a range of matrices ranging from rock ore to biomass; The process can be used to recover a wide range of minerals; This novel extraction chemistry can be cheap, simple, and nontoxic/”green”: The chemical extraction uses water, the cheapest industrial acid (sulfuric), and simple salts (i.e. sodium sulfate). However, other acids, salts, and additives could be used as appropriate. This Laboratory Directed Research and Development (LDRD) project identified that the process is complex with many interacting factors, but the benefits are significant if the complexities can be resolved. Challenges remain in the development of this technology and are described in this report. However, the results are positive, and commercial partners have already expressed interest. In summary, a novel, green, inexpensive mineral extraction process has been developed and demonstrated in a small batch reactor system. The effort provided information for an invention disclosure, proposal to DOE, and will support future business development efforts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Rugged nanoparticle tracers for mass tracking in explosive events

Tracing the flow of solid matter during an explosion requires a rugged tag that can be measured by a unique identifiable signature. Silica-covered semiconductor quantum dots (QDs) provide a unique and tunable photoluminescent signature that emits from within a sacrificial outer layer. Five types of silica-covered zinc sulfide QDs were synthesized and covalently bound to commercial luminescent powders. The combination of five dots and five powders enables a matrix of 25 unique tags. The tracers are shown to be tolerant of environments associated with chemical explosives and provides a unique tag to evaluate debris fields.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

A versatile and low-cost chip-to-world interface: enabling ICP-MS characterization of isotachophoretically separated lanthanides on a microfluidic device

Microfluidics offer novel and state-of-the-art pathways to process materials. Microfluidic systems drastically reduce timeframes and costs associated with traditional lab-scale efforts in the area of analytical sample preparations. The challenge arises in effectively connecting microfluidics to off-chip analysis tools to accurately characterize samples after treatment on-chip. Here, a fused silica microfluidic device (MFD) is connected to a fused-silica capillary in order to create a world-to-chip connection between the MFD and an inductively coupled plasma mass spectrometer (ICP-MS). Specifically, this is demonstrated by utilizing isotachophoresis (ITP) on a microfluidic chip to separate samples containing up to 14 lanthanides into elementally pure bands. The separated sample is successfully transferred across a 7 nL dead space at the microchip-capillary junction, such that separation resolution is maintained and even increased through the interface and into the ICP-MS, where the elemental composition of the separated sample is analysed. Lanthanide samples of varying composition are detected using ICP-MS, demonstrating this versatile and cost-effective approach that does not degrade the separation quality achieved on the MFD. This simple and inexpensive connection enables fast, low-cost sample preparation immediately prior to injection into an ICP-MS or other analytical instruments.

Lackey, Hope E.↗