SEARCH · Engineering Papers
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.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
The goal of these studies is an increased understanding of the fundamental interactions and electronic structure involved in actinide metal bonding, coordination and solvation.
Our fundamental understanding of actinide radiation-induced redox chemistry is crucial to nuclear fuel cycle development, due to the unavoidable exposure of these elements to ionizing radiation fields, both inherent and from in-process applications. Plutonium (Pu) and americium (Am) both possess multiple oxidation states, the careful manipulation of which are essential in the study and utilization of their rich chemistry, developing new nuclear technologies, and securing the long-term sustainability of nuclear power. However, knowledge in this area is far from complete. Consequently, we have studied the radiation-induced chemistry of both Pu and Am through a variety of techniques. Temperature-controlled electron pulse radiolysis has been used to study Am for the first time, determining the feasibility of Am redox reactions under used nuclear fuel reprocessing conditions, (e.g. nitric acid, non-ambient temperature). Additionally, we have developed an experimentally evaluated multi-scale computer model for the prediction of gamma radiation-induced Pu redox chemistry due to radiolysis and disproportionation reactions in concentrated nitric acid solutions.
Not Available
Not Available
Not Available
Investigating the extraction and separation behavior of americium and curium using synergic dual-ligand solvent extraction systems and their conversion to novel extraction chromatographic resins.
DOE BES Highlight slide for program managers.
NS&T Highlight Slide for DOE
Accurately modeling optical spectra with absolute radiometric intensities is vital for nuclear forensics applications that depend on characterizing optical emissions from energetic nuclear phenomena. This requires precise knowledge of the individual atomic transition probabilities, known as Einstein A-coefficients, for each emission line. Obtaining these values theoretically or experimentally is often impractical due to the complex electronic structures and the number of transitions involved in atoms relevant to nuclear applications. In this study, we explore the use of machine learning to predict the Einstein A coefficients for atomic transitions. Seven models were evaluated that ranged from deep learning to decision tree algorithms, and found that gradient boosting performed best, specifically the Extreme Gradient Boosting (XGB) architecture, achieving a precision of 86% across transitions of 36 elements. Furthermore, the model was cross-validated using published transition probabilities reported in the literature and applied to estimate Pu plasma temperatures from a previous experiment conducted at Savannah River National Laboratory.
Real-time, trace alpha activity monitoring in extreme mixed radiation fields is a well-known challenge in fission product-rich streams containing mixtures of beta-gamma-alpha radiation-emitting isotopes, arising due to the extreme 10 6 :1 ratio of background beta-gamma vs. alpha radiation activity levels. This paper presents results from a novel approach to addressing this challenge, based on Tensioned Metastable Fluid Detector (TMFD) sensing technology. An acoustically driven technique was developed and tested at Purdue University (using dissolved Rn-Po and U-chain alpha emitters), and validated (with dissolved Pu) at Savannah River National Laboratory for real-time monitoring of alpha activity in the 100–10,000 dpm/mL range.
The Los Alamos National Laboratory exchange program is the only program of its kind for the distribution of plutonium (Pu) standards materials with a range of impurity contents to multiple laboratories for destructive measurements of elemental concentration. This paper discusses statistical methods used to address challenges in Pu metal exchange data by way of two case studies. Challenges include how to evaluate a data set when a large fraction of the values are minimum detection limits (MDLs), and how to determine potential outliers with limited in-formation on the true spread of the data.
Development of a simple and scalable synthesis of (TBA) 3 [W 5 O 18 MoNO] provides for the formation of the mixed-metal lacunary polyoxoalkoxide, (TBA) 2 [W 4 O 13 (OMe) 4 MoNO][Na(MeOH)]. This complex was used to synthesize a series of polyoxoalkoxide sandwich-type complexes with the general formula (TBA) 2 [M{W 4 O 13 (OMe) 4 MoNO} 2 ], where M = Zr(IV), Hf(IV), Th(IV), U(IV), and Np(IV). Compared to the analogous all-molybdenum complexes, the series have drastically different optical and redox properties. The results indicate that framework metal substitution acts as a tool for “orbital engineering”, with Density Functional Theory (DFT) calculations revealing that the major consequence of incorporation of tungsten into the complexes is localization of LUMO and LUMO+1 on the molybdenum centers remaining in the molecule. The change in the distribution of the frontier orbitals translates to discrepancies in the electronic properties of the series. Given the rarity of polyoxometalate complexes featuring a U(V) ion, one electron oxidation of (TBA) 2 [U(IV){W 4 O 13 (OMe) 4 MoNO} 2 ] was pursued. Isolation of the corresponding U(V) centered sandwich-type complex is reported, only the second example of U(V)-polyoxometalate complex described to date.
The development of nuclear waste forms for both existing and future nuclear wastes is critical to ensuring global environmental safety. This study focuses on waste management from molten salt reactors, where fuel exists in a salt form and could be processed in real time for the removal of neutron poisons such as xenon isotopes (e.g., 135 Xe) and rare earth elements (REEs, e.g., 149 Sm). To ensure safe, stable, and long-term disposal in geological repositories, REEs must be incorporated into a durable waste form. Iron-phosphate glasses are a promising candidate due to their low melting points, high chemical durability, and their ability to incorporate high concentrations of REEs. In this study, we successfully prepared iron-phosphate glass waste forms with high Nd loadings (up to 37 mass %) in batch sizes ranging from small (23 g) to large (1600 g). The resulting materials contained up to 75 mass % NdPO 4 , contributing to their mechanical resilience and exceptional chemical durability. These findings highlight the potential of iron-phosphate glasses as high-efficiency, chemically durable waste forms and demonstrate the successful transition from theoretical design to scaled-up production.
We report the first example of a polyoxometalate (POM) compound containing californium. Using a Wells–Dawson POM ligand, K 17 Cf(P 2 W 17 O 61 ) 2 ·2H 2 O was synthesized and characterized. Californium is the heaviest element ever crystalized with a POM. Significant solubility differences among the POM's f-element complexes were observed, enabling selective precipitation with separation factors rivaling liquid–liquid extraction.
Photochromic radionuclide-based “claw machines” characterizedviaa combination of isothermal titration calorimetry and spectroscopic analysis unlock a pathway for on demand radionuclide capture and release.
An outstanding puzzle in the structure of very heavy nuclei lies in the rotation response of deformed transuranic isotopes. While the rotation alignment of pairs of 𝑖 13/2 protons is ubiquitous and well understood, observing the analogous alignment of the 𝑗 15/2 neutrons has been elusive. In this work we present a new quantitative analysis approach: from their moments of inertia as a function of frequency, we compare the alignments of rotational bands with both “low” and high-𝑗 intrinsic structures in the 𝑁 = 151 isotones of Pu, Cm, Cf, and No, thereby distinguishing between the alignments of neutron versus proton pairs through “blocking” effects. In this way, the alignment of 𝑗 15/2 neutrons can be clearly identified for the first time. The protons and neutrons begin aligning at a very similar frequency. The contribution of 𝑗 15/2 neutrons to the total alignment is found to grow with increasing 𝑍 compared to 𝑖 13/2 protons. To explain these observations, it is necessary to adopt a self-consistent set of single-particle energies corresponding to the nuclear shape that minimizes the mass. The shape description needs to include high-order deformations up to at least 𝛽 6 .