Frontier Actinide Radiation Chemistry
Frontier Actinide Radiation Chemistry
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
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Recent Advances in Actinide Radiation Chemistry
The attached presentation discusses recent advances in actinide radiation chemistry from the perspective of the INL Center for Radiation Chemistry Research, to be presented virtually at the Los Alamos National Laboratory G. T. Seaborg Institute Seminar Series.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Radiation Chemistry and the Nuclear Fuel Cycle
This presentation will give a general overview of radiation chemistry in the nuclear fuel cycle, and outline some relevant work being conducted in the INL Radiochemical Separations and Radiation Science Department. This will include a discussion of using multiscale modeling to study plutonium radiation chemistry in nitric acid solutions. (Presentation cancelled)
38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗
Radiation chemistry in the Jovian stratosphere - Laboratory simulations
The results of the present low-pressure/continuous-flow laboratory simulations of H2/He/CH4/NH3 atmospheres' plasma-induced chemistry indicate radiation yields of both hydrocarbon and N2-containing organic compounds which increase with decreasing pressure. On the basis of these findings, upper limits of 1 million-1 billion molecules/sq cm/sec are established for production rates of major auroral-chemistry species in the Jovian stratosphere. It is noted that auroral processes may account for 10-100 percent of the total abundances of most of the observed polar-region organic species.
Mcdonald, Gene D.↗
The Inorganic Chemist?s Guide to Actinide Radiation Chemistry - BES Highlight
DOE BES Highlight slide for program managers.
37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
The Inorganic Chemist?s Guide to Actinide Radiation Chemistry - NS&T Highlight Slide
NS&T Highlight Slide for DOE
37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
Sulfur Chloride Radiation Chemistry Activities
Presentation highlight the INL Center for Radiation Chemistry Research's contributions the Material Recovery & Waste Form Development Campaign on sulfur chloride processing technologies.
38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗
The inorganic chemist's guide to actinide radiation chemistry: a review
This review aims to provide an overview of the current state of radiation chemistry with respect to the actinide elements, thorium through californium. Despite the inherent radioactivity of the actinides, only a few studies explore the effects of ionizing radiation on their redox chemistry and surrounding environment. This fundamental knowledge gap, coupled with the current renaissance in actinide-based technologies such as nuclear power, space exploration, and medicine, underscores the importance of research in this interdisciplinary area. This review will focus on the interactions between reactive species formed by radiolysis with actinides and their complexes, offering an inorganic chemist's perspective on research in radiation chemistry. In addition, a thorough discussion of our current understanding of radiation-induced changes in actinide speciation in both aqueous solution and the solid-state will be provided, focusing on changes in oxidation state distribution, complexation, and secondary coordination effects within inorganic materials. Finally, this review will discuss challenges and opportunities for inorganic chemists to explore this unique intersection of fields.
Actinides↗
A Radiation Chemistry Code Based on the Greens Functions of the Diffusion Equation
Ionizing radiation produces several radiolytic species such as.OH, e-aq, and H. when interacting with biological matter. Following their creation, radiolytic species diffuse and chemically react with biological molecules such as DNA. Despite years of research, many questions on the DNA damage by ionizing radiation remains, notably on the indirect effect, i.e. the damage resulting from the reactions of the radiolytic species with DNA. To simulate DNA damage by ionizing radiation, we are developing a step-by-step radiation chemistry code that is based on the Green's functions of the diffusion equation (GFDE), which is able to follow the trajectories of all particles and their reactions with time. In the recent years, simulations based on the GFDE have been used extensively in biochemistry, notably to simulate biochemical networks in time and space and are often used as the "gold standard" to validate diffusion-reaction theories. The exact GFDE for partially diffusion-controlled reactions is difficult to use because of its complex form. Therefore, the radial Green's function, which is much simpler, is often used. Hence, much effort has been devoted to the sampling of the radial Green's functions, for which we have developed a sampling algorithm This algorithm only yields the inter-particle distance vector length after a time step; the sampling of the deviation angle of the inter-particle vector is not taken into consideration. In this work, we show that the radial distribution is predicted by the exact radial Green's function. We also use a technique developed by Clifford et al. to generate the inter-particle vector deviation angles, knowing the inter-particle vector length before and after a time step. The results are compared with those predicted by the exact GFDE and by the analytical angular functions for free diffusion. This first step in the creation of the radiation chemistry code should help the understanding of the contribution of the indirect effect in the formation of DNA damage and double-strand breaks.
Plante, Ianik↗
MRWFD Center for Radiation Chemistry Research Activities
Presentation for DOE-NE Aqueous Separation 2021 PIs’ Meeting updating on the FY21 research activities of the INL Center for Radiation Chemistry Research.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Step-by-Step Simulation of Radiation Chemistry Using Green Functions for Diffusion-Influenced Reactions
Radiolytic species are formed approximately 1 ps after the passage of ionizing radiation through matter. After their formation, they diffuse and chemically react with other radiolytic species and neighboring biological molecules, leading to various oxidative damage. Therefore, the simulation of radiation chemistry is of considerable importance to understand how radiolytic species damage biological molecules [1]. The step-by-step simulation of chemical reactions is difficult, because the radiolytic species are distributed non-homogeneously in the medium. Consequently, computational approaches based on Green functions for diffusion-influenced reactions should be used [2]. Recently, Green functions for more complex type of reactions have been published [3-4]. We have developed exact random variate generators of these Green functions [5], which will allow us to use them in radiation chemistry codes. Moreover, simulating chemistry using the Green functions is which is computationally very demanding, because the probabilities of reactions between each pair of particles should be evaluated at each timestep [2]. This kind of problem is well adapted for General Purpose Graphic Processing Units (GPGPU), which can handle a large number of similar calculations simultaneously. These new developments will allow us to include more complex reactions in chemistry codes, and to improve the calculation time. This code should be of importance to link radiation track structure simulations and DNA damage models.
Plante, Ianik↗
Step-by-Step Simulation of Radiation of Radiation Chemistry Using Green Functions for Diffusion-Influenced Reactions
The irradiation of biological systems leads to the formation of radiolytic species such as H(raised dot), (raised dot)OH, H2, H2O2, e(sup -)(sub aq), etc.[1]. These species react with neighboring molecules, which result in damage in biological molecules such as DNA. Radiation chemistry is there for every important to understand the radiobiological consequences of radiation[2]. In this work, we discuss an approach based on the exact Green Functions for diffusion-influenced reactions which may be used to simulate radiation chemistry and eventually extended to study more complex systems, including DNA.
Plante, Ianik↗
Backend Nuclear Fuel Cycle Radiation Chemistry
Given global commitments to significantly increase nuclear energy capacity, it is now more important than ever to develop efficient used nuclear fuel management strategies to improve resource utilization, energy security, and waste minimization. Here, an overview of nuclear energy, backend fuel cycle challenges, and advances in used nuclear fuel reprocessing radiation chemistry will be presented. More specifically, the use of electron pulse irradiation techniques to explore radiation-induced reaction mechanisms in actinide containing solutions and solvent systems.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
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↗
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↗
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↗
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↗
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↗