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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Multiscale Strategy for Predicting Radiation Chemistry in Polymers

A primary mode for radiation damage in polymers arises from ballistic electrons that induce electronic excitations, yet subsequent chemical mechanisms are poorly understood. We develop a multiscale strategy to predict this chemistry starting from subatomic scattering calculations. Nonadiabatic molecular dynamics simulations sample initial bond-breaking events following the most likely excitations, which feed into semiempirical simulations that approach chemical equilibrium. Application to polyethylene reveals a mechanism explaining the low propensity to cross-link in crystalline samples.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Radiation Chemistry and the Nuclear Fuel Cycle

Internal presentation for "UK Professor and PhD Student Visit: Presentation on Separations and Waste Forms along with National Programs."

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Actinide Radiation Chemistry and Used Nuclear Fuel Reprocessing

Although the actinides boast many unique physical and chemical properties, their inherent susceptibility to radioactive decay—and subsequent consequences of radiation-induced chemistry—are what make them truly interesting and challenging elements to understand. From a closed nuclear fuel cycle perspective, the ability to predict and control the effects of actinide-driven radiolysis is critical for the design, development, and deployment of advanced used nuclear fuel reprocessing strategies and technologies. The absorption of ionizing radiation from actinide decay leads to the formation of a variety of transient and steady-state radicals, ions, and molecular radiolysis products that can lead to significant changes in a reprocessing solvent system’s physical and chemical properties, which ultimately limits that process’ efficiency and longevity. Presented here is an overview of recent advances in actinide radiation chemistry as it applied to used nuclear fuel reprocessing.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS2014

RITRACKS: A Software for Simulation of Stochastic Radiation Track Structure, Micro and Nanodosimetry, Radiation Chemistry and DNA Damage for Heavy Ions

The code RITRACKS (Relativistic Ion Tracks) has been developed over the last few years at the NASA Johnson Space Center to simulate the effects of ionizing radiations at the microscopic scale, to understand the effects of space radiation at the biological level. The fundamental part of this code is the stochastic simulation of radiation track structure of heavy ions, an important component of space radiations. The code can calculate many relevant quantities such as the radial dose, voxel dose, and may also be used to calculate the dose in spherical and cylindrical targets of various sizes. Recently, we have incorporated DNA structure and damage simulations at the molecular scale in RITRACKS. The direct effect of radiations is simulated by introducing a slight modification of the existing particle transport algorithms, using the Binary‐Encounter‐Bethe model of ionization cross sections for each molecular orbitals of DNA. The simulation of radiation chemistry is done by a step‐by‐step diffusion‐reaction program based on the Green's functions of the diffusion equation]. This approach is also used to simulate the indirect effect of ionizing radiation on DNA. The software can be installed independently on PC and tablets using the Windows operating system and does not require any coding from the user. It includes a Graphic User Interface (GUI) and a 3D OpenGL visualization interface. The calculations are executed simultaneously (in parallel) on multiple CPUs. The main features of the software will be presented.

Plante, I↗
DOE OSTI2026

Non-Equilibrium Actinide Radiation Chemistry and the Nuclear Fuel Cycle

Actinides are inherently unstable elements that frequently coexist with other radioisotopes, generating intense ionizing radiation fields that drive the formation of non equilibrium oxidation states. These transient species exert a profound mechanistic influence on the radiation response of actinide containing systems due to their unique redox chemistry. Despite their importance, they remain poorly understood, yet such insight is essential for advancing actinide science and accurately predicting radiation driven behavior. Actinide separations—critical for nuclear energy technologies, strategic deterrence, space exploration, and nuclear medicine—depend on precise control of actinide oxidation states to recover targeted elements from complex matrices such as used nuclear fuel. However, during these processes, actinides, their coordination complexes, and the separation media are all exposed to intense, multicomponent (alpha, beta, gamma, etc.) radiation fields that can alter process efficiency, selectivity, and chemical stability. Understanding, controlling, and mitigating radiation induced reactions is therefore key to innovating and optimizing next generation separation technologies. This seminar will provide an overview of the nuclear fuel cycle and non equilibrium actinide radiation chemistry in the context of recovering actinides from used nuclear fuel, with a particular emphasis on direct dissolution–based reprocessing strategies. We will explore time resolved electron pulse radiolysis and alpha and gamma dose accumulation studies, integrated with multiscale computational modeling, to elucidate the molecular level roles of radiation driven, non equilibrium actinide species in process performance and in the radiolytic stability of organic ligands used for actinide recovery. These insights offer new pathways for designing advanced separation methods and next generation solvent systems, with broad implications for the future of the nuclear fuel cycle.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
DOE OSTI2026

Non-Equilibrium Actinide Radiation Chemistry and the Nuclear Fuel Cycle

Invited John and Naomi Fackler Lectureship in Chemistry and English seminar at Valparaiso University, IN, USA. Actinides are inherently unstable elements that frequently coexist with other radioisotopes, generating intense ionizing radiation fields that drive the formation of non-equilibrium oxidation states. These transient species exert a profound mechanistic influence on the radiation response of actinide-containing systems due to their unique redox chemistry. Despite their importance, they remain poorly understood, yet such insight is essential for advancing actinide science and accurately predicting radiation-driven behavior. Actinide separations—critical for nuclear energy technologies, strategic deterrence, space exploration, and nuclear medicine—depend on precise control of actinide oxidation states to recover targeted elements from complex matrices such as used nuclear fuel. However, during these processes, actinides, their coordination complexes, and the separation media are all exposed to intense, multicomponent (alpha, beta, gamma, etc.) radiation fields that can alter process efficiency, selectivity, and chemical stability. Understanding, controlling, and mitigating radiation-induced reactions is therefore key to innovating and optimizing next-generation separation technologies. This seminar will provide an overview of the nuclear fuel cycle and non-equilibrium actinide radiation chemistry in the context of recovering actinides from used nuclear fuel, with a particular emphasis on direct-dissolution–based reprocessing strategies. We will explore time-resolved electron pulse radiolysis and gamma dose accumulation studies to elucidate the molecular-level roles of radiation-driven, non-equilibrium actinide species in process performance and in the radiolytic stability of organic ligands used for actinide recovery. These insights offer new pathways for designing advanced separation methods and next-generation solvent systems, with broad implications for the future of the nuclear fuel cycle.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
DOE OSTI2024

Multiscale Modeling of Plutonium Radiation Chemistry in Nitric Acid Solutions. 1. Cobalt-60 Gamma Irradiation of Pu(IV)

We report careful manipulation of the plutonium oxidation states is essential in the study and utilization of its rich redox chemistry. To achieve this level of control, a comprehensive mechanistic understanding of radiation-induced plutonium redox chemistry is critical due to the unavoidable exposure of plutonium to ionizing radiation fields, both inherent and from in-process applications. To this end, we have developed an experimentally evaluated multiscale computer model for the prediction of gamma radiation-induced Pu(IV) redox chemistry in concentrated nitric acid solutions (1.0, 3.0, and 6.0 M). Under these acidic, aqueous solution conditions, cobalt-60 gamma irradiation afforded marginal net conversion of Pu(IV) to Pu(VI), the extent of which was dependent on the concentration of HNO 3 and absorbed gamma dose. Multiscale calculations, which are in excellent agreement with experimental data, indicate that this observation is due to a combination of inherent plutonium disproportionation reactions and several radiation-induced processes, including redox cycling between Pu(IV) and Pu(III), as achieved by the reduction of Pu(IV) by nitrous acid and hydrogen peroxide, the oxidation of Pu(III) by nitrate and hydroxyl radicals, and the sequential oxidation of Pu(IV) to Pu(V) and Pu(VI) by the remaining available yield of nitrate radicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1969

Production of metals and compounds by radiation chemistry

Preparation of metals and compounds by radiation induced chemical reactions involves irradiation of metal salt solutions with high energy electrons. This technique offers a method for the preparation of high purity metals with minimum contamination from the container material or the cover gas.

Marsik, S. J.↗
DOE OSTI2021

The Reactivity of Polyethylene Microplastics in Water under Low Oxygen Conditions Using Radiation Chemistry

Polyethylene (PE) is an intensely utilized polymer, which has consequently led to it becoming a common environmental contaminant. PE and other plastic waste are known to be highly persistent in surface waters; however, chemical and physical changes do take place over time, dependent mostly on highly variable natural conditions, such as oxygen (O2) availability. Gamma radiation was used to generate reactive oxygen species, namely hydroxyl radicals, in initially aerated aqueous solutions to simulate the natural weathering of microplastics in waters where there are fluctuations and often depletions in dissolved O2. The headspace of the irradiated PE-containing solutions was probed for the formation of degradation products using solid-phase microextraction (SPME) fibers in combination with gas chromatography mass spectrometry (GCMS). The major species detected were n-dodecane, with trace levels of tridecane, 2-dodecanone, and hexadecane, which were believed to be predominately adsorbed in the PE microplastics in excess of their aqueous solubility limits. Surface characterization by Raman spectroscopy and light and dark field microscopy indicated no change in the chemical composition of the irradiated PE microplastics under low O2 to anaerobic conditions. However, morphological changes were observed, indicating radical combination reactions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Contribution Slides for External IAEA Conference Radiation Chemistry Review

Contribution slides for an invited talk (presented by Professor Mohamad Al-Sheikhly, University of Maryland ) at the International Atomic Energy Agency (IAEA)- Virtual Workshop on Radiation Technology for Industry and Environment. The title of the review talk is "Future Trends in Radiation Technology Applications in Advancing Science and Engineering".

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS2009

Extraterrestrial Radiation Chemistry and Molecular Astronomy

Astronomical observations of both solar system and interstellar regions have revealed a rich chemical inventory that includes most classes of organic molecules and selected inorganics. For example, gas-phase ethylene glycol and SOz have been observed by astronomers, while solidphase detections include OCS, H2O2 , and the cyanate anion.' All of these are found in environments that are, by earthly standards, exceedingly hostile: temperatures of 10 - 100 K, miniscule densities, and near-ubiquitous ionizing-radiation fields. Beyond the simplest chemical species, these conditions have made it difficult-to-impassible to account for the observed molecular abundances using gas-phase chemistry, suggesting solid-phase reactions play an important role. In extraterrestrial environments, cosmic rays, UV photons, and magnetospheric radiation all drive chemical reactions, even at cryogenic temperatures. To study this chemistry, radiation astrochemists conduct experiments on icy materials, frozen under vacuum and exposed to sources such as keV electrons and MeV protons. Compositional changes usually are followed with IR spectroscopy and, in selected cases, more-sensitive mass-spectral techniques. This talk will review some recent results on known and suspected extraterrestrial molecules and ions. Spectra and reaction pathways will be presented, and predictions made for interstellar chemistry and the chemistry of selected solar system objects. Some past radiation-chemical contributions, and future needs, will be explored.

Hudson, Reggie L.↗
DOE OSTI2021

Modeling the Fundamental Radiation Chemistry of the Organic Diluent, and the Effect of Metal Ion Complexation on the Radiochemical Behavior of Active Compounds

All used nuclear fuel (UNF) reprocessing technologies must operate efficiently in the presence of an intense, multi-component (predominantly alpha, beta, and gamma) radiation field. Consequently, radiation-induced degradation of reprocessing systems is of concern, as it negatively impacts process performance over time due to the destruction of both active compounds (ligands, phase modifiers, holdback agents, etc.) and the formation of degradation products. Reprocessing solvent system radiolysis has been linked to changes in separation efficiency and physical properties of solvent mixtures, solvent-recycle longevity, crud formation, and other unexpected outcomes that impact the efficient recovery of valuable materials (e.g., the actinides) and the volume of hazardous radioactive waste for final disposal, i.e., in a geological repository. Consequently, a fundamental understanding of radiolytic processes and their effects on reprocessing solvent system performance is critical for: (i) the cost-effective development and innovation of separation technologies; (ii) the design and implementation of predictive radiation chemical models for process monitoring and lifetimes; and (iii) potentially the ability to exploit radiolytic phenomenon to our benefit, e.g., strategic radiolysis of active molecules to liberate specific degradation products that aid subsequent process stages. Despite extensive investigation into the radiolytic behavior of active solvent system compounds, little attention has been given to understanding (i) the radiation chemical behavior and modification of the organic diluent and (ii) the effect of metal ion complexation on the radiochemical behavior of active compounds.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS2014

A Radiation Chemistry Code Based on the Green's Function of the Diffusion Equation

Stochastic radiation track structure codes are of great interest for space radiation studies and hadron therapy in medicine. These codes are used for a many purposes, notably for microdosimetry and DNA damage studies. In the last two decades, they were also used with the Independent Reaction Times (IRT) method in the simulation of chemical reactions, to calculate the yield of various radiolytic species produced during the radiolysis of water and in chemical dosimeters. Recently, we have developed a Green's function based code to simulate reversible chemical reactions with an intermediate state, which yielded results in excellent agreement with those obtained by using the IRT method. This code was also used to simulate and the interaction of particles with membrane receptors. We are in the process of including this program for use with the Monte‐Carlo track structure code Relativistic Ion Tracks (RITRACKS). This recent addition should greatly expand the capabilities of RITRACKS, notably to simulate DNA damage by both the direct and indirect effect.

Plante, Ianik↗
NASA NTRS2017

Radiation Chemistry of Solid Acetone in the Interstellar Medium - A New Dimension to an Old Problem

A laboratory investigation of acetone, an interstellar and cometary molecule, has produced new results concerning its decomposition in a radiation environment. Mid-infrared spectroscopy has been used to follow amorphous acetone's destruction by ionizing radiation (1 MeV protons) at 20 K. Radiation products identified are the CH4, CO, and CO2 usually made in such experiments, along with ketene, allene, and the acetonyl radical, all identified here for the first time in irradiated solid acetone. Evidence for the reduction product 2-propanol was suggestive, but a firm identification could not be made either for it or for the C2 hydrocarbons (i.e., C2H6, C2H4, C2H2). The acetyl radical was not observed as a radiation product. Isotopically labeled reagents were used to demonstrate ketene formation and to emphasize that multiple approaches are needed for robust assignments of infrared spectral features of irradiated icy solids. Results from a supporting radiation experiment with isotopically labeled acetic acid are described. Comparisons are made to a previous study of acetone's stability in extraterrestrial radiation environments, and caution is urged in measuring and interpreting CO abundances in irradiated icy solids.

cometary molecule↗
NASA NTRS2017

Radiation Chemistry of Solid Acetone in the Interstellar Medium - A New Dimension to an Old Problem

A laboratory investigation of acetone, an interstellar and cometary molecule, has produced new results concerning its decomposition in a radiation environment. Mid-infrared spectroscopy has been used to follow amorphous acetone’s destruction by ionizing radiation (1 MeV protons) at 20 K. Radiation products identified are the CH4, CO, and CO2 usually made in such experiments, along with ketene, allene, and the acetonyl radical, all identified here for the first time in irradiated solid acetone. Evidence for the reduction product 2-propanol was suggestive, but a firm identification could not be made either for it or for the C2 hydrocarbons (i.e., C2H6, C2H4, C2H2). The acetyl radical was not observed as a radiation product. Isotopically labeled reagents were used to demonstrate ketene formation and to emphasize that multiple approaches are needed for robust assignments of infrared spectral features of irradiated icy solids. Results from a supporting radiation experiment with isotopically labeled acetic acid are described. Comparisons are made to a previous study of acetone’s stability in extraterrestrial radiation environments, and caution is urged in measuring and interpreting CO abundances in irradiated icy solids.

R. L. Hudson↗