Radiochemistry Commons^™

Compact 1 Ghz Electron Paramagnetic Resonance Spectrometers For Preclinical Imaging Studies, Tanden A. Hovey

Electronic Theses and Dissertations

Magnetic resonance is one of the most generally useful scientific techniques. New horizons of understanding are revealed as technological advances make possible explorations of nuclear spins and electron spins at higher and lower magnetic fields and electromagnetic frequencies. While the greatest current effort is on ever higher magnetic fields and microwave frequencies, both in nuclear magnetic resonance (NMR) and electron paramagnetic resonance (EPR), the Eaton lab focusses on developing high signal-to-noise performance EPR at low microwave frequencies. EPR provides information about O2, pH, viscosity, glutathione concentrations, and reactive oxygen species in living organisms that MRI cannot. To yield clinically or …

Radiotheranostics For Gynecological Pathologies, Joni Sebastiano

Dissertations, Theses, and Capstone Projects

Molecular imaging, specifically positron emission tomography (PET), is vital for detecting disease and understanding its biological makeup. The exploitation of radiolabeled antibodies for PET imaging has proven to be indispensable to the field of molecular imaging over the last several decades. The development of radioimmunoconjugates for use in immunoPET has not only allowed for the sensitive, specific, and high-resolution detection of disease, but has also enabled a deeper understanding of the disease biology, ultimately guiding more personalized therapeutic strategies. Most typically, this technology is harnessed for the diagnosis and treatment of cancer, however more recently, the field has explored the …

At The Crossroads Of Traditional And Nuclear Forensics: Decontaminating Radiologically Contaminated Dna Evidence Using Magnetic Beads, Rin Nyx Ruby

UNLV Theses, Dissertations, Professional Papers, and Capstones

Known for its impressive discriminatory power, deoxyribonucleic acid (DNA) fingerprinting stands as the “gold standard” of forensic investigation. However, complications arise when such evidence is contaminated with radioactive material. Though biological samples exposed to ionizing radiation can still yield comprehensive DNA profiles, most forensic laboratories lack the facilities which meet the safety and security requirements necessary for handling radioactive material. While nuclear facilities can decontaminate samples prior to forensic analysis, conventional methods for radiological decontamination – such as mechanical cleaning and chemical washes – may degrade the quality of the forensic evidence. The purpose of this study is to evaluate …

The Behavior And Complexation Of Technetium Under Conditions Relevant For Nuclear Fuel Reprocessing, Rachel E. Greenberg

Dissertations, Theses, and Capstone Projects

Spent nuclear fuel is reprocessed by utilizing several large-scale solvent extraction processes. One of the most prevalent of these processes is the plutonium uranium reduction extraction (PUREX) process. This process involves an organic phase composed of tributyl phosphate (TBP) in kerosene and an aqueous phase comprised of concentrated nitric acid. Both uranium (U) and plutonium (Pu) are extracted into the organic phase by nitrate and TBP complexation while the various fission products remain in the initial aqueous phase. Pu is then chemically reduced to its trivalent state and back-extracted into a second aqueous phase, thereby separating the two fissile materials. …

Development Of Mixed O/S-Donor Imidazole Thione Ligands For Trivalent Lanthanide/Actinide Separations, Rhianna Wolsleger

All Dissertations

Separation of lanthanides and actinides is difficult due to their very similar size and charge. Increasing selectivity for actinides over lanthanides is possible by incorporating a softer, more polarizable donor atom into a chelating ligand, since the softer donor atom is capable of greater orbital overlap with the 5f orbitals of the actinides vs the 4f orbitals of the lanthanides. Sulfur-containing imidazole thione chelating ligands have not been investigated for this purpose but possess a resonance structure that puts significant negative charge on the sulfur, enabling it to form strong metal-sulfur bonds compared to other sulfur-containing ligands such as thioethers …

Intrinsic Gas-Phase Behavior Of Uranium Species: A Comprehensive Reactivity Study Of [O=U≡Ch]+ And [Uh]+, Justin Terhorst

Electronic Theses and Dissertations

The intrinsic chemistry of actinide elements, particularly uranium, remains a key challenge in understanding f-block reactivity due to the complexity introduced by solvent interactions, counter-ions, and complex equilibria in the condensed phase. In this dissertation, a systematic gas-phase study utilizing preparative tandem ion-trap mass spectrometry (PTMSⁿ) is presented, focusing on the reactivity of uranium-centered species, specifically [OUCH]⁺, an oxy uranium methylidyne species, and [UH]⁺ ions. By stripping away solvent effects and isolating the ions, PTMSⁿ provides a powerful platform to probe the fundamental chemical behavior of uranium species in their intrinsic state.

The …

Uranium(Vi) & Thorium(Iv) Speciation In Organic Media Containing Organophosphorus & Diglycolamide Extractants, Joel Castillo

UNLV Theses, Dissertations, Professional Papers, and Capstones

Developing sustainable green energy systems is a continually growing concern as the world is faced with urgent issues of climate change and global warming. Nuclear energy provides one of the most efficient solutions to supplying power to the electrical grid without causing more carbon pollution. There are nearly a hundred thousand metric tons of used nuclear fuel (UNF) stored on-site at decommissioned nuclear power plants for an indefinite period of time. Achieving a finalized closed fuel cycle is a crucial part in developing the nuclear energy necessary for combating the issues of pollution and greener energy. Understanding actinide speciation especially …

Nuclear Fuel Cycle Chemistry: A Density Functional Study, Eduardo Montoya

UNLV Theses, Dissertations, Professional Papers, and Capstones

The nuclear fuel cycle aptly describes the life cycle of nuclear fuel sources such as uranium. From its early forms in naturally bearing ores, to its high-temperature sintering into a fuel pellet, the chemistry uranium experiences throughout the fuel cycle is diverse, driving many experimental efforts towards understanding its chemistry to both improve nuclear technologies and advance the safety and handling of nuclear materials. Computing techniques and methodologies can be used to supplement experimental research and are readily available to researchers interested in utilizing computing-based data to support experimental findings. Density functional theory (DFT) is commonly practiced, reliably predicting the …

Development Of Uranium Fluoride Microstructures, Harry Jang

UNLV Theses, Dissertations, Professional Papers, and Capstones

Uranium microstructured materials with controlled size and shape have found applications in several branches of the nuclear industry including as targets for medical isotopes production, fuels for nuclear reactors, standards for analytical measurements, and energy sources for space exploration. Morphological studies of actinide materials are also highly relevant to nuclear forensics-related work. Other potential applications include information storage, catalysis, sensors, and luminescent devices. Most studies on uranium microstructured materials have focused on binary oxides, nitrides, carbides, and fluorides, with the spherical shape being the dominant morphology. Prior to the work reported in this dissertation, aside from UF4 microspheres (ms) and …

44ti/44sc Generator Development And Radiolabeling Optimization For Medical Applications, Christine E. Schmidt-Kennelty

Dissertations, Theses, and Capstone Projects

In recent years, there has been a growing interest in scandium-44 (⁴⁴Sc) for medical applications due to its favorable decay properties. With a relatively short half-life of 3.97 hours and high positron branching ratio of 94.3%, ⁴⁴Sc is an ideal candidate for positron emission tomography (PET) imaging. However, producing ⁴⁴Sc without an on-site cyclotron limits access, as its short half-life makes it impractical to ship to more remote locations.

To address this issue, ⁴⁴Ti/⁴⁴Sc generators have become a focal point of research, providing an onsite source of⁴⁴Sc. Despite their potential, current …

Extraction Of Neutron-Gamma Irradiated Diffusion Pump Oils, Cooper L. Tillman

All Theses

This work successfully demonstrates solvent extraction methods for separation of oil from the by-products when two commercially available vacuum pump oils were exposed to an intense neutron and gamma-ray radiation environment. Nuclear fusion power at a commercial scale has accelerated the need for radiation resistant vacuum technology, such as oil-based diffusion pumps. Polyphenyl ether and aromatic silicone oils were irradiated at the Rhode Island Nuclear Science Center (RINSC) up to MGy absorbed doses with neutron and gamma-ray radiation. Solvent extractions were performed using hexane and isopropanol to characterize the oil extraction as a function of total absorbed dose. The by-products …

Positron Emission Tomography In Oncology And Environmental Science, Samantha Delaney

Dissertations, Theses, and Capstone Projects

The last half century has played witness to the onset of molecular imaging for the clinical assessment of physiological targets. While several medical imaging modalities allow for the visualization of the functional and anatomical properties of humans and living systems, few offer accurate quantitation and the ability to detect biochemical processes with low-administered drug mass doses. This limits how physicians and scientists may diagnose and treat medical issues, such as cancer, disease, and foreign agents.

A promising alternative to extant invasive procedures and suboptimal imaging modalities to assess the nature of a biological environment is the use of positron emission …

Photoelectic Driven Decomposition Of Uracil Via Hard X-Ray Irradiation, Trimaan Malik

UNLV Theses, Dissertations, Professional Papers, and Capstones

Radiation damage into biological samples creates substantial challenges across a wide range of fields, from biochemistry to materials science. This comprehensive study investigates the effects of x-ray irradiation on uracil, the only nucleobase exclusive to Ribonucleic acid (RNA), to understand how doping with 10% (by mass) of specific powdered elements impacts the sustained radiation damage. The experiments were conducted at the Brockhouse Undulator Beamline of the Canadian Light Source synchrotron. Virgin and doped uracil samples were irradiated with hard x-rays, above their respective absorption edges, and studied with x-ray diffraction to compare their decomposition behaviors. The Uracil reflections on the …

Celestial Bodies, Rebecca L. Rand, Mark Popinchalk

Capstones

Most of us will never come close to touching space. But space touches us every day. On Celestial Bodies, journalist Rebecca Rand and astronomer Mark Popinchalk explore the ways outer space interacts with life on earth.

In Episode 1, hosts Rebecca Rand and Mark Popinchalk explore how, for millions of years, trees have been recording celestial events in space. Within the rings of their trunks, trees store radiation from solar flares, supernovae, and changes in the earth’s magnetic field. The hosts talk to Dr. Ben Pope to learn more about what we can discover by looking at radioactive molecules …

Actinide Behavior In Soft Ligand Environments And Higher Oxidation States Of Neptunium In Aqueous Media With Solid-State Synthesis Of Np(Vii) Compounds, Kelly Floyd Seeley

UNLV Theses, Dissertations, Professional Papers, and Capstones

The fundamental properties of Uranium and Neptunium were investigated with Powder X-Ray Diffraction (PXRD) to study the behavior or 5f electrons with chalcogen, alkali metals, and alkaline earth metals. Two novel compounds were generated: NaCuUS₃ and NaCuNpS₃. There are several crystal structures that form in the family of AMM’Q (A = s-block, M = d-block, M’ = d-block or f-block, and Q = chalcogen), with oxidation states of A¹⁺, M¹⁺, M’⁴⁺, and Q^2- ions from the family of type I compounds. Work was continued to …

The Development Of Novel Radioscandium And Hydroxypyridinonate Based Radiopharmaceuticals, Michael Phipps

Dissertations, Theses, and Capstone Projects

The use of radiometals in radiopharmaceutical development has drastically increased over the last decade, owed in part to the diverse chemistry and emission characteristics of the radiometals, which allow chemists to create a toolbox of agents to better tailor patient care. Challenges with the use of radiometals include the selection of the metal and the development of optimized chelators to cover the diverse chemistry of the metals which make up the majority of the periodic table. Scandium is the first transition metal and has multiple radioisotopes whose emission characteristics have potential application in medicine. 3,4,3-LI(1,2-HOPO) is a chelator whose denticity, …

Separation Of Zr From Complex Matrices For Isotope Harvesting Applications, Jake A. Bence

Dissertations, Theses, and Capstone Projects

Zr isotopes have various applications in nuclear science, such as ⁸⁶Zr and ⁸⁹Zr in nuclear medicine, ⁸⁸Zr as a diagnostic isotope relevant to stockpile stewardship, and the fission product ⁹⁵Zr useful as an s-process branch nucleus for study in astrophysics. To access these isotopes of interest, dedicated production methods and subsequent processing chemistry are required. Direct production routes can be technically challenging and difficult to obtain enough activity to meet demand. The processing chemistry of Zr isotopes is tedious due to the tendency for Zr to hydrolyze in solution without highly acidic conditions or a strong …

The Development Of Novel Radioimmunoconjugates For The Pet Imaging And Radioimmunotherapy Of Cancer, Samantha M. Sarrett

Dissertations, Theses, and Capstone Projects

Antibodies have long played a vital role in nuclear medicine for both the diagnosis and therapy of various malignancies. The role and development of antibodies in nuclear medicine can be broadly separated into three different categories: 1) bioconjugation strategies, 2) immunoPET imaging, and 3) radioimmunotherapy. This dissertation will attempt to comprehensively cover each of these categories through a series of studies, protocols, and reviews. For the bioconjugation strategies, we will describe the development of a novel site-selective bioconjugation strategy using an innovative lysine-targeting reagent, PFP-bisN₃, to prepare [⁸⁹Zr]Zr-^SSKDFO-pertuzumab for visualizing HER2+ breast cancer. Further, …

Impacts Of Preferential Flow On Tc-99and Np-237 Vadose Transport In Soils At The Savannah River Site, Josh Parris

All Theses

Since the 1950s, the United States has produced approximately 90,000 metric tons of spent nuclear fuel (SNF) (Office of Nuclear Energy, 2022); however, no long-term storage solutions are available. Technecium-99 and neptunium-237, two fission products found in SNF, readily form highly mobile species in oxidizing conditions (Hu, 2008; Bondietti, 1979) and have respective half-lives of 2.13 x 10⁵ and 2.14 x10⁶ years (Hu, 2010). Considering these characteristics, ⁹⁹Tc and ²³⁷Np are two risk-driving isotopes found in SNF storage. The process of macropore-facilitated preferential flow, transport through cracks within a soil matrix, has been recognized to increase …

Synthesis, Radiolabeling And Evaluation Of A Suite Of Tracers With 44Sc For Detecting Extracellular Dna, Zhiyao Li

McKelvey School of Engineering Graduate Student Theses & Dissertations

Neutrophil extracellular traps involve the rapid translocation of DNA to the outside of the cell under certain stimuli. This structure forms a fibrous network that is able to limit the spread of pathogens and to kill microorganisms. It has also been shown to be present in various pathological processes such as inflammation, autoimmune diseases, and cancer metastasis. Currently, the formation process of NETs in vivo is being extensively studied. However noninvasive detection and quantitation has yet to be achieved. A class of PET tracers are described here that consists of a DNA dye as the backbone that is labeled with …

Development Of Optical Nanomaterial For Enhanced Cerenkov Imaging, Qize Zhang

Dissertations, Theses, and Capstone Projects

Cancer is a significant public health problem worldwide and is the second leading cause of death in the United States. Imaging has increasingly been used over the last two decades to improve the diagnosis and guidance of tumor tissue removal surgery. Among the most widely used techniques for in vivo imaging are planar and tomographic fluorescence imaging and bioluminescence imaging. Despite their utility, these techniques are primarily restricted to preclinical use. Factors that have prevented translation from the bench to the bedside include depth-penetration considerations, regulatory issues, and toxicity. A recent development in nuclear imaging has been the ability to …

An Entropic Approach To Dynamics, Pedro Henrique Moreira Pessoa

Legacy Theses & Dissertations (2009 - 2024)

The present thesis deals with different aspects of probability, the method of maximum entropy, information geometry, and dynamical systems and their applications to statistical physics and complex systems. Those topics come together in the framework for dynamics termed entropic dynamics. Work on the topic was initiated by my PhD advisor Professor Ariel Caticha and many colleagues at University at Albany as a method for explaining the dynamical processes in quantum mechanics from first principles of probability theory.

Revisiting The Chemistry Of Uranium And Rhenium Fluorides: Implication To Fuel Cycle And Nuclear Forensics Science, James Amos-Aimé Louis-Jean

UNLV Theses, Dissertations, Professional Papers, and Capstones

Fluorine plays a major role in the nuclear industry where F2(g) and HF(g) are critical to the preparation of UF6 and UF4. These materials are prepared for uranium enrichment to increase the isotopic concentration of 235U. During separation efforts, the isotope 99Tc (a high yield fission product, 6.1% from 235U) is extracted along with uranium and can be converted to binary technetium fluorides (i.e., TcF4, TcF6) during re-enrichment of used uranium material. This provides a route for 99Tc to reenter the reactor environment and affect the nuclear properties of fuel pellets made with reprocessed uranium. The objective of this work …

“Translation Of Hdac6 Pet Imaging Using [18f]Ekz-001 – Cgmp Production And Measurement Of Hdac6 Target Occupancy In Nhps” – A Review, Dania Rahal

Chemistry & Biochemistry Undergraduate Honors Theses

The inhibition of histone deacetylase 6 (HDAC6) has been reported to alleviate the effects of neurodegenerative diseases such as Alzheimer’s disease. The brain-penetrant PET radioligand [¹⁸F]EKZ-001 has high affinity and selectivity towards HDAC6 and therefore suggests great promise in therapeutic treatment studies and development for neurodegenerative diseases. “Translation of HDAC6 PET imaging using [¹⁸F]EKZ-001 – cGMP production and measurement of HDAC6 target occupancy in NHPs” has achieved an effective, fully automated method of producing [¹⁸F]EKZ-001 in compliance with current good manufacturing practices (cGMP) to support the translation of [¹⁸F]EKZ-001 PET for …

Extractive Membranes For The Detection And Screening Of Waterborne Plutonium, James Foster

All Dissertations

The development of rapid screening tools for special nuclear materials remains a crucial focus for nonproliferation efforts. Traditional approaches for the analysis of trace-level Pu isotopes in water requires tedious and time-consuming sample preparation steps that do not lend well to expeditious screening. Therefore, a novel analytical method that combines both Pu concentration and source preparation into a single detection system would make for an invaluable tool for nuclear security applications. Extractive membranes absorbers can help to fulfill this role as they are capable of concentrating Pu to detectable limits while subsequently serving as alpha spectrometry sample sources. In Chapter …

Design & Analysis Of Mixed-Mode Integrated Circuit For Pulse-Shape Discrimination, Bryan Orabutt

McKelvey School of Engineering Graduate Student Theses & Dissertations

In nuclear science experiments it is usually necessary to determine the type of radiation, its energy and direction with considerable accuracy. The detection of neutrons and discriminating them from gamma rays is particularly difficult. A popular method of doing so is to measure characteristics intrinsic to the pulse shape of each radiation type in order to perform pulse-shape discrimination (PSD).

Historically, PSD capable systems have been designed with two approaches in mind: specialized analog circuitry, or digital signal processing (DSP). In this work we propose a PSD capable circuit topology using techniques from both the analog and DSP domains. We …

Electron Spin Relaxation Of Nitroxide Spin Labels And Relaxation Processes, Thacien Ngendahimana

Electronic Theses and Dissertations

MTSL is the nitroxide spin label that is most commonly used in site-directed spin labeling. However, due to rotation of its gem-dimethyl groups that average anisotropic interactions, T_m becomes short above about 70 K and this makes DEER experiments difficult at these temperatures. Strategies for decreasing spin echo dephasing and electron spin lattice relaxation rates are important for design of nitroxide spin labels and molecular qubits.

In searching for labels with longer T_m, new nitroxide spin labels devoid of gemdimethyl groups or with more rigid structures were synthesized at the University of Nebraska and pulsed EPR measurements …

Seasonal Transport Of Dissolved Inorganic Carbon And Total Alkalinity Across The Louisiana Shelf, Michelle M. Anderson

LSU Master's Theses

Rivers and wetlands are a major source of terrestrial derived carbon for coastal ocean margins. Unfortunately, Louisiana’s wetlands are threatened by ongoing high rates of erosion, deterioration, and unprecedented rates of river water discharge that changes seasonally, leading to a net loss of terrestrial carbon into the northern Gulf of Mexico (nGOM). There exists a current lack of understanding about the distribution of dissolved inorganic carbon (DIC) and total alkalinity (TAlk) within the shallowest regions of the Louisiana shelf. Even less is known about how the transport of DIC alters seasonally with changes in river outflow and shelf currents. Quantifying …

The Reduction, Sequestration, And/Or Coordination Of Technetium-99 Utilizing Polyoxometalates And Nanomaterials, Colleen Mb Gallagher

Dissertations, Theses, and Capstone Projects

Research into the sequestration of radionuclides from aqueous media is being conducted due to the contamination of aqueous waste effluents and groundwater with highly toxic long-lived radionuclides. These contaminants are introduced into water and streams from legacy nuclear sites, nuclear reactor operations, nuclear fuel reprocessing, nuclear weapons testing, and plutonium production. A major contributor (~6%) to the waste from thermal neutron fission of uranium-235 is the radionuclide technetium-99 (⁹⁹Tc). It is considered a long-lived radioisotope with a half-life of 2.1x10⁵ years. It is a weak beta emitter with a max energy of 0.29 MeV and is most …

Synthesis And Characterization Of Synthetic Urban Melt Glass, Rebecca Kristien Lowe

UNLV Theses, Dissertations, Professional Papers, and Capstones

Melt glass formed from the explosion of a nuclear device is a unique post-detonation material that can aid in the ensuing forensics investigation. Trapped in the melt glass are chemical and isotopic signatures that can provide diagnostic and source information about the weapon by comparison with documentation of previous detonations. A nuclear terrorist attack would likely take place in an urban environment and as such, the melt glass formed would consist of a complex matrix including urban materials like cement and glass, activation products from the large neutron flux that will be seen, and fission products from the detonation. The …