Physical Sciences and Mathematics Commons^™

Intragroup Separation Of Trivalent Lanthanides And Actinides For Neutron Capture Experiments In Stockpile Stewardship Sciences, Narek Gharibyan

UNLV Theses, Dissertations, Professional Papers, and Capstones

Knowledge of low-energy cross sections for stable and unstable nuclei in neutron-, γ- and ion induced reactions is important in both the simulation and radiochemistry diagnosis of nuclear device performance. This dissertation explores extraction chromatography and ion chromatography methods for the intragroup separation of trivalent actinides and lanthanides in support of cross section measurements for isotopes of interest. For trivalent actinides, americium (Am(III)) and curium (Cm(III)), separation is necessary to assist in experiments related to the measurement of neutron capture cross section for ²⁴¹ Am and the production of ^{242 m} Am/^242g Am isomeric ratio. Extraction chromatography resins …

Equilibrium Speciation Of Select Lanthanides In The Presence Of Acidic Ligands In Homo- And Heterogeneous Solutions, Troy Robinson

UNLV Theses, Dissertations, Professional Papers, and Capstones

This dissertation explores lanthanide speciation in liquid solution systems related to separation schemes involving the acidic ligands: bis(2-ethylhexyl) phosphoric acid (HDEHP), lactate, and 8-hydroxyquinoline. Equilibrium speciation of neodymium (Nd³⁺ ), sodium (Na⁺ ), HDEHP, water, and lactate in the TALSPEAK liquid-liquid extraction system was explored under varied Nd³⁺ loading of HDEHP in the organic phase and through extraction from aqueous HCl and lactate media. System speciation was probed through vapor pressure osmometry, visible and Fourier Transform Infrared (FTIR) spectroscopy, ²² Na and ¹³ C labeled lactate radiotracer distribution measurements, Karl Fischer titrations, and equilibrium pH measurements. Distribution …

Synthesis, Extraction, Dissolution, And Voltammetry Of F-Species In A Room Temperature Ionic Liquid Solvent, Wendy Jacqueline Pemberton

UNLV Theses, Dissertations, Professional Papers, and Capstones

Room temperature ionic liquids (RTILs) are salts that are liquids from as low as -96 °C to up to 100 °C. RTILs are of high interest in many fields of study because of their negligible vapor pressure, high electrochemical stability, high conductivity, and wide electrochemical windows. These diverse solvents have recently been used in organic synthesis, as extraction solvents, and as electrochemical solvents. It is as a direct result of the multifunctional capabilities of these RTIL solvents that they are examined in this work. The ability to probe the chemistry of lanthanides and actinides is based on the unique properties …

Preparation And Characterization Of Extraction Chromatography Resins Using N-Donor Extractants For Trivalent Actinide And Lanthanide Separations, Christopher L. Klug

UNLV Theses, Dissertations, Professional Papers, and Capstones

Actinide and lanthanide elements exist in the geosphere and biosphere due to both natural abundances and anthropogenic activities. The investigation of the presence and transport of actinides through the environment is of great scientific interest. In order to prepare environmental samples for precise measurements, the individual actinides must be separated from the chemically similar lanthanides, and from neighboring actinides. Existing extraction chromatography resins are either poorly suited for this separation, have bleeding problems, are not reusable, or fail the CHON principle. In an effort to resolve these issues, malonamides and N-donor extractants from the BTP and BTBP classes of solvent …

Electrochemical Separation Of Curium And Americium, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

The objective was to use electrochemical techniques to develop a thermodynamic understanding of actinide and lanthanide species in RTIL solutions, and use this data to effectively separate species with very similar chemical properties.

In consultation with a DOE collaborator, electrochemical methods and materials were evaluated and used to exploit the thermodynamic differences between similar chemical species enhancing the ability to selectively target and sequester individual species from mixtures. This project, in its third year, successfully completed phases 1, 2. Phase 3 was partially completed. The project expanded to include phase 4.

The following were specific goals for 2007-2008:

• To …

Evaluation Of Fundamental Radionuclide Extraction Data For Urex, Kenneth Czerwinski

Separations Campaign (TRP)

The speciation of technetium and actinides in advanced solvent extraction systems is the basis for their manipulation in separations. The ability to understand and predict radionuclide speciation is paramount to successful modeling of proposed separation systems. This project will examine the speciation of radionuclides in different stages of the uranium extraction (UREX) separation scheme, providing data useful to modeling. The areas to be examined include the speciation of uranium and plutonium with tributylphosphate and the kinetics and thermodynamics of lanthanides and actinides in the TALSPEAK (Trivalent actinide lanthanide separation by phosphorous reagent extraction from aqueous complexes) system. The complexation constants …

Electrochemical Separation Of Curium And Americium, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

The objectives of this project are to use electrochemical techniques to develop a thermodynamic understanding of actinide and lanthanide species in RTIL solution, and to use this data to effectively separate species with very similar chemical properties. In consultation with a national laboratory collaborator, electrochemical methods and materials will be evaluated and used to exploit the thermodynamic differences between similar chemical species, enhancing the ability to selectively target and sequester individual species from mixtures. This project is in its third year and has successfully completed phases 1 and 2. Phase 3 has been partially completed. The tasks have been expanded …

The Electrochemical Separation Of Curium And Americium: Quaterly Report January - March, 2006, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

This research report outlines the current status and progress associated with the electrochemical separation of Curium and Americium. For two and a half years, research has been actively performed on this project, and is currently on schedule for the proposed timelines.

Progress:

• The electrochemical characterization of Ce and Eu complexed with EDTA, NTA, and Citrate has been completed.

• Synthesis of the polymer substrate and the chelating ligand is underway. Approximately 50 grams of disulfide has been produced to produce the chelating thiol group required for the last set of studies.

• Gold substrates have been prepared to perform …

Electrochemical Separation Of Curium And Americium, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

The objective of this project is to use electrochemical techniques to develop a thermodynamic understanding of actinide and lanthanide species in aqueous solution and use this data to effectively separate species with very similar chemical properties. In consultation with a national laboratory collaborators, electrochemical methods and materials will be evaluated and used to exploit the thermodynamic differences between similar chemical species enhancing the ability to selectively target and sequester individual species from mixtures. This project is in its third year and has successfully completed Phases 1 and 2.

The following were specific goals for this year:

• To develop a fundamental …

The Electrochemical Separation Of Curium And Americium: Quaterly Report April - June, 2005, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

This research report outlines the current status and progress associated with the electrochemical separation of Curium and Americium.

Results

• We have completed the electrochemical investigation in of the Ce³⁺/Ce⁴⁺ redox couple and have determined the optimum experimental conditions.

• Computer modeling of the cerium using the JChess speciation-modeling program has been completed for the Ce redox couple. Traditional complexing ligands such as EDTA, oxalate, NTA, phosphate, acetate, and sulfate have been purchased and will be used to initiate the complexation and electrochemical characterization.

• Electrochemical investigations have continued on the Eu²⁺/Eu³⁺ redox …

Electrochemical Separation Of Curium And Americium, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

The objective of this project is to use electrochemical techniques to develop a thermodynamic understanding of actinide and lanthanide species in aqueous solution and use this data to effectively separate species with very similar chemical properties. In consultation with our DOE collaborator, electrochemical methods and materials will be evaluated and used to exploit the thermodynamic differences between similar chemical species enhancing our ability to selectively target and sequester individual species from mixtures.

The following were specific goals for this year:

• To develop a fundamental understanding of the thermodynamic properties of actinide and lanthanide species such as Cm, Am, Ce, Nd, …

The Electrochemical Separation Of Curium And Americium: Quaterly Report August-December 2004, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

This research report outlines the current status and progress associated with the electrochemical separation of Curium and Americium. The following pages outline the progress on our project to date. We have been actively performing research on this project for three months and are currently on schedule in terms of the proposed timelines.

The initial focus of the project involved setting up the laboratories for the studies outlined in the grant proposal. The instrumentation needed included an electrochemical work station that will perform the bulk of the electrochemical studies. This instrument will complement the electrochemical instrumentation in Dr. Hatchett’s laboratory and …

Electrochemical Separation Of Curium And Americium, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

The objective of this project is to develop a method for the separation of Am from Cm based on electrochemical techniques. Electrochemical systems that allow the thermodynamics of actinide and lanthanide complexes to be systematically evaluated and tuned will be examined. The influence of complex formation on the ability to selectively isolate a given species electrochemically will be evaluated. Metal-ligand complex formation provides a useful derivation technique to increase solubility in solution environments that favor precipitation. In addition, the thermodynamic properties of a complex relative to the isolated species may be shifted to more suitably measurable electrochemical separation regimes. Electrochemical …

The Electrochemical Separation Of Curium And Americium: Quaterly Report January - March 2004, David W. Hatchett, Kenneth Czerwinski

Separations Campaign (TRP)

This research report outlines the current status and progress associated with the electrochemical separation of Curium and Americium.

Data collection and analysis of the Ce³⁺/Ce⁴⁺ redox couple in various supporting electrolytes has continued. All electrolyte systems were investigated at Pt, Au, and Glassy Carbon working electrodes. Analysis of these data was accomplished by performing appropriate background subtractions to reveal net peaks due to Ce redox behavior. Successful identification of the Ce redox couple was achieved with all electrolyte/electrode systems, although a decline in peak resolution was observed with increasing acid concentration. Optimal conditions in this experiment were …