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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2012

Polyacrylamide-hydroxyapatite composite: Preparation, characterization and adsorptive features for uranium and thorium

The composite of synthetically produced hydroxyapatite (HAP) and polyacrylamide was prepared (PAAm-HAP) and characterized by BET, FT-IR, TGA, XRD, SEM and PZC analysis. The adsorptive features of HAP and PAAm-HAP were compared for UO{sub 2}{sup 2+} and Th{sup 4+}. The entrapment of HAP into PAAm-HAP did not change the structure of HAP. Both structures had high affinity to the studied ions. The adsorption capacity of PAAm-HAP was than that of HAP. The adsorption dependence on pH and ionic intensity provided supportive evidences for the effect of complex formation on adsorption process. The adsorption kinetics was well compatible to pseudo second order model. The values of enthalpy and entropy changes were positive. Th{sup 4+} adsorption from the leachate obtained from a regional fluorite rock confirmed the selectivity of PAAm-HAP for this ion. In consequence, PAAm-HAP should be considered amongst favorite adsorbents for especially deposition of nuclear waste containing U and Th, and radionuclide at secular equilibrium with these elements. - Graphical abstract: SEM images of hydroxyapatite (HAP) and polyacrylamide-hydroxyapatite (PAAm-HAP), and the adsorption isotherms for Uranium and Thorium. Highlights: Black-Right-Pointing-Pointer Composite of PAAm-HAP was synthesized from hydroxyapatite and polyacrylamide. Black-Right-Pointing-Pointer The materials were characterized by BET, FT-IR, XRD, SEM, TGA and PZC analysis. Black-Right-Pointing-Pointer HAP and PAAm-HAP had high sorption capacity and very rapid uptake for UO{sub 2}{sup 2+} and Th{sup 4+}. Black-Right-Pointing-Pointer Super porous PAAm was obtained from PAAm-HAP after its removal of HAP content. Black-Right-Pointing-Pointer The composite is potential for deposition of U, Th and its associate radionuclides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2010

Improving Natural Uranium Utilization By Using Thorium in Low Moderation PWRs - A Preliminary Neutronic Scoping Study

The Th-U fuel cycle is not quite self-sustainable when used in water-cooled reactors and with fuel burnups higher than a few thousand of MWd/t characteristic of CANDU reactors operating with a continuous refueling. For the other industrially mature water-cooled reactors (i.e. PWRs and BWRs) it is economically necessary that the fuel has enough reactivity to reach fuel burnups of the order of a few tens of thousand of MWd/t. In this particular case, an additional input of fissile material is necessary to complement the bred fissile U-233. This additional fissile material could be included in the form of Highly Enriched Uranium (HEU) at the fabrication of the Th-U fuel. The objective of this preliminary neutronic scoping study is to determine (1) how much HEU and, consequently, how much natural uranium is necessary in such Th-U fuel cycle with U recycling and (2) how much TRansUranics (TRU=Pu, Np, Am and Cm) are produced. These numbers are then compared with those of a standard UO2 PWR. The thorium reactors considered have a homogeneous hexagonal lattice made up of the same (Th-U)O2 pins. Furthermore, at this point, we are not considering the use of blankets inside or outside the core. The lattice pitch has been varied to estimate the effect of the water-to-fuel volume ratio, and light water as well as heavy water have been considered. For most cases, an average burnup at discharge of 45,000 MWd/t has been considered.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

Feasibility study on the thorium fueled boiling water breeder reactor

The feasibility of (Th,U)O 2 fueled, boiling water breeder reactor based on conventional BWR technology has been studied. In order to determine the potential use of water cooled thorium reactor as a competitive breeder, this study evaluated criticality, breeding and void reactivity coefficient in response to changes made in MFR and fissile enrichments. The result of the study shows that while using light water as moderator, low moderator to fuel volume ratio (MFR=0.5), it was possible to breed fissile fuel in negative void reactivity condition. However the burnup value was lower than the value of the current LWR. On the other hand, heavy water cooled reactor shows relatively wider feasible breeding region, which lead into possibility of designing a core having better neutronic and economic performance than light water with negative void reactivity coefficient. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2013

Transmutation, Burn-Up and Fuel Fabrication Trade-Offs in Reduced-Moderation Water Reactor Thorium Fuel Cycles - 13502

Multiple recycle of long-lived actinides has the potential to greatly reduce the required storage time for spent nuclear fuel or high level nuclear waste. This is generally thought to require fast reactors as most transuranic (TRU) isotopes have low fission probabilities in thermal reactors. Reduced-moderation LWRs are a potential alternative to fast reactors with reduced time to deployment as they are based on commercially mature LWR technology. Thorium (Th) fuel is neutronically advantageous for TRU multiple recycle in LWRs due to a large improvement in the void coefficient. If Th fuel is used in reduced-moderation LWRs, it appears neutronically feasible to achieve full actinide recycle while burning an external supply of TRU, with related potential improvements in waste management and fuel utilization. In this paper, the fuel cycle of TRU-bearing Th fuel is analysed for reduced-moderation PWRs and BWRs (RMPWRs and RBWRs). RMPWRs have the advantage of relatively rapid implementation and intrinsically low conversion ratios. However, it is challenging to simultaneously satisfy operational and fuel cycle constraints. An RBWR may potentially take longer to implement than an RMPWR due to more extensive changes from current BWR technology. However, the harder neutron spectrum can lead to favourable fuel cycle performance. A two-stage fuel cycle, where the first pass is Th-Pu MOX, is a technically reasonable implementation of either concept. The first stage of the fuel cycle can therefore be implemented at relatively low cost as a Pu disposal option, with a further policy option of full recycle in the medium term. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Characterisation of Specimens from a Former Soviet Thorium Processing Facility to Support Site Remediation

The former Prydniprovski Chemical Plant (PChP) is a large ex-soviet nuclear materials processing site of roughly 260 hectares, located in central Ukraine. PcHP was in operation between 1948 and 1991 for the purposes of processing uranium and thorium ore into ore concentrate. During its operational lifetime, tens of millions of tonnes of radioactive waste was generated on the site. A consequence of these activities, coupled with the mismanagement of the resulting radioactive materials and by-products, is that approximately 45% of the southern part of the site has become radioactively contaminated. This area comprises some 100-200 buildings and structures, many of which are in a state of disrepair and dereliction. Around 20 of these buildings are heavily radioactively contaminated, with radiation levels from a few μSv/hr to a maximum of 4 mSv/hr reported. The European Commission is currently working with the Ukraine Ministry of Energy and Coal Use and the Nuclear Regulator to improve radiological safety and security at the site. In order for these remediation works to proceed, the site management needs to characterise the radioactive materials that are held there. As part of this activity, the team from the University of Bristol have undertaken a survey of one of the most heavily contaminated buildings, collecting a selection of in situ material samples. A suite of complimentary materials characterisation techniques (e.g. X-ray Fluorescence, Raman Spectroscopy, etc) have been deployed in order to determine the radionuclides and composition of the compounds present. Characterisation of these samples will allow the operators of the chemical plant to go forward with remediation works within the building.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2016

Ultra-Long-Life Fast Reactor Cores having Axial Blanket-Driver-Blanket Burnup Strategy with Thorium and PWR Spent Fuels

The sustainable energy over a long-term period can be supplied by ultra-long-life fast reactor cores that are designed by fully utilizing breeding by fast neutrons to be operated over several tens of years without refueling. But the fast reactor cores of this type usually have high positive coolant void reactivity worth resulted from the high TRU (Transuranics) contents in the high burnup, which can degrade the inherent safety through high positive coolant expansion reactivity coefficient. Recently, the authors have designed new small ultra-long-life cores that can be operated over 50{approx}60 EFPYs (Effective Full Power Years) and satisfy the self-controllability conditions under the unprotected accidents. The cores use axial blanket-driver-blanket configuration to achieve ultra-long operational cycle length where the fuel burnup propagates from the outer core to the inner core and from the axially central driver to the outer blanket regions. The objective of this work is to suggest the different design options with thorium addition and TRU and uranium from PWR spent fuels for effectively utilizing the large PWR spent fuel stocks and to analyze the performances of the cores. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples

Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, with total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Chromatographic separation of the theranostic radionuclide 111 Ag from a proton irradiated thorium matrix

Column chromatographic methods have been developed to separate no-carrier-added 111 Ag from proton irradiated thorium targets and associated fission products as an ancillary process to an existing 225 Ac separation design. In this paper, we report the separation of 111 Ag both prior and subsequent to 225 Ac recovery using CL resin, a solvent impregnated resin (SIR) that carries an organic solution of alkyl phosphine sulfides (R 3 P = S) and alkyl phosphine oxides (R 3 P = O). The recovery yield of 111 Ag was 93 ± 9% with a radiochemical purity of 99.9% (prior) and 87 ± 9% with a radiochemical purity of 99.9% (subsequent to) 225 Ac recovery. Both processes were successfully performed with insignificant impacts on 225 Ac yields or quality. Measured equilibrium distribution coefficients for silver and ruthenium (a residual contaminant) on CL resin in hydrochloric and nitric acid media are reported, to the best of our knowledge, for the first time. Finally and additionally, measured cross sections for the production of 111 Ag and 110m Ag for the 232 Th(p,f) 110m,111 Ag reactions are reported within.

111Ag↗
DOE OSTI2013

Comparative analysis of thorium and uranium fuel for transuranic recycle in a sodium cooled Fast Reactor

The present paper compares the reactor physics and transmutation performance of sodium-cooled Fast Reactors (FRs) for TRansUranic (TRU) burning with thorium (Th) or uranium (U) as fertile materials. The 1000 MWt Toshiba-Westinghouse Advanced Recycling Reactor (ARR) conceptual core has been used as benchmark for the comparison. Both burner and breakeven configurations sustained or started with a TRU supply, and assuming full actinide homogeneous recycle strategy, have been developed. State-of-the-art core physics tools have been employed to establish fuel inventory and reactor physics performances for equilibrium and transition cycles. Results show that Th fosters large improvements in the reactivity coefficients associated with coolant expansion and voiding, which enhances safety margins and, for a burner design, can be traded for maximizing the TRU burning rate. A trade-off of Th compared to U is the significantly larger fuel inventory required to achieve a breakeven design, which entails additional blankets at the detriment of core compactness as well as fuel manufacturing and separation requirements. The gamma field generated by the progeny of U-232 in the U bred from Th challenges fuel handling and manufacturing, but in case of full recycle, the high contents of Am and Cm in the transmutation fuel impose remote fuel operations regardless of the presence of U-232.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2019

Whole core analysis of the single-fluid double-zone thorium molten salt reactor (SD-TMSR)

The SD-TMSR (2,250 MW th ) is a Single-fluid Double-zone Thorium-based Molten Salt Reactor. The active core of the SD-TMSR is divided into the inner zone (486 fuel tubes) and the outer zone (522 fuel tubes) to improve the Th-U3 breeding performance. This work adopted the SERPENT-2 Monte Carlo code to analyze the whole core model of the SD-TMSR. Built-in SERPENT-2 capabilities simulated online reprocessing and refueling and calculated the multiplication factor and Breeding Ratio (BR). We found that the molten salt Temperature Coefficient of Reactivity ( α T ) was negative for initial and equilibrium states. This study investigated the variation of the multiplication factor, BR, and build-up of important nuclides in the core as a function of burnup. Under online reprocessing and refueling, we studied the variation of the reactivity during 60 years of reactor operation. Additionally, the neutron spectrum shift during the reactor operation was calculated. Finally, these simulations determined the appropriate 232 Th and 233 U feed rates for maintaining criticality and enabled analysis of the overall SD-TMSR fuel cycle performance.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Preliminary design of control rods in the single-fluid double-zone thorium molten salt reactor (SD-TMSR)

Recent studies on Molten Salt Reactors (MSRs) showed that the excess reactivity at the beginning of the operation is large for many fueling strategies and must be compensated by a reactivity control system. The current work introduces a reliable safety system based on control rods in addition to the online feed system reactivity control in the Single-fluid Double-zone Thorium-based Molten Salt Reactor (SD-TMSR). Three different initial fissile loadings are considered: 233 U, reactor-grade Pu, and transuranic (TRU) elements as a startup fuel. We applied six different absorbing materials to investigate the main operational and safety parameters in the SD-TMSR: natural B 4 C, enriched B 4 C with 90% 10 B, HfB 2 , HfH 1.62 , Eu 2 O 3 , and Gd 2 O 3 . The present work focuses on control rod design, integral and differential control rod worth, shutdown margin, and shadowing effects at steady-state. We employed the SERPENT-2 Monte-Carlo code to calculate the reactivity worth and analyze the performance of the reactivity control system. We showed that 233 U and reactor-grade Pu startup cores maintain adequate shutdown margin with all considered absorbers. Finally, this report proposes a design of control rod clusters that compensate the excess reactivity of the SD-TMSR loaded with different initial fissile material.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2021

Reactions of atomic thorium and uranium cations with CF 4 studied by guided ion beam tandem mass spectrometry

The fundamental chemistry of the actinides continues to be an area of interest because of their use in nuclear fuel cycles. Here, the kinetic energy dependences of the reactions of thorium and uranium cations with CF 4 were studied using guided ion beam tandem mass spectrometry. The products observed include AnF x + (An = Th or U, x = 1-3) and CF y + (y = 1-3). Although most reactions are exothermic according to literature thermochemistry, all cross sections display strong endothermic features indicating a restriction in the reactivity at low energies. For both actinides, only the AnF + + CF 3 product channel is observed at low energies; however, its formation proceeds very inefficiently. Furthermore, these results indicate that the reactions of Th + and U + with CF 4 are not thermodynamically driven and suggest that the low-energy reactivity results from precise alignment of the reactants.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

First-principles studies of the structural, electronic, and optical properties of a novel thorium compound Rb{sub 2}Th{sub 7}Se{sub 15}

The structural, electronic, and optical properties of a recently synthesized thorium compound Rb{sub 2}Th{sub 7}Se{sub 15} have been calculated in the density functional theory framework for the first time. The calculated direct band gap was 1.471 eV (generalized gradient approximation) and 1.171 eV (local density approximation), with both results being close to the experimental result of 1.83 eV. High covalency/iconicity of the Th–Se/Rb–Se bonds was demonstrated by calculating effective Mulliken charges of all ions. The polarized calculations of the complex dielectric function are presented; dependence of the calculated index of refraction was fitted to the Sellmeyer equation in the wavelength range from 500 to 2500 nm. - Graphical abstract: Calculated band structure of Rb{sub 2}Th{sub 7}Se{sub 15}. - Highlights: • The first theoretical analysis of the Rb{sub 2}Th{sub 7}Se{sub 15} properties is reported. • Structural, electronic and optical properties of Rb{sub 2}Th{sub 7}Se{sub 15} were calculated. • An indirect character of Rb{sub 2}Th{sub 7}Se{sub 15} band gap was confirmed. • Dependence of the refractive index on the wavelength was calculated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Na n MTh 6 F 30 : A Large Family of Quaternary Thorium Fluorides

Recently we reported the synthesis, crystal structures and magnetic properties of compounds in the Na n MU 6 F 30 series, where n = 4 or 3, and where M is a divalent or trivalent metal cation, respectively. Here in this article we advance our investigation of this structure type by expanding it to the thorium containing compounds Na n MTh 6 F 30 , where n = 3 in the case of M III = Al, Sc, Ti, V, Cr, Fe, Ga, or In; n = 4 when MII = Mg, Mn, Co, Ni, Cu, or Zn; and n varies from 3.87 to 4.39 when the M site is partially occupied by a trivalent rare earth element. Magnetic properties of the compounds containing magnetic ions M = Ti 3+ , V 3+ , Cr 3+ , Mn 2+ , Fe 3+ , Co 2+ , Ni 2+ , and Cu 2+ were studied to demonstrate that the substitution of Th(IV) for U(IV) prevents the magnetic ions from coupling magnetically and, therefore, exhibit simple paramagnetic behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Synthesis and Evaluation of a Bifunctional Chelator for Thorium-227 Targeted Radiotherapy

Thorium-227 (227Th) is an α-emitting radionuclide currently under investigation for targeted alpha therapy. Available chelators used for this isotope suffer from challenging multistep syntheses. Here, we present the synthesis and preclinical evaluation of a novel bifunctional chelator, p-SCN-Bn-DOTHOPO, which contains an isothiocyanate group that is suitable for conjugation to biological molecules. This bifunctional chelator was prepared with a 26% overall yield in four steps and conjugated to the human epidermal growth factor receptor 2 targeting antibody, trastuzumab. The resulting immunoconjugate was labeled with [227Th]ThIV (pH 5.5, room temperature, 60 min) with ≥95% radiochemical yield and purity. The conjugate was also labeled with zirconium-89 (89Zr), which can be used for positron emission tomography imaging. The radiometal complexes were subsequently investigated for their biological stability. The results described here provide insight into ligand design strategies and optimization of chelators for the development of the next generation of 89Zr and 227Th radiopharmaceuticals.

Thorium↗
DOE OSTI2017

Catalytic Dehydrogenation of Dimethylamine Borane by Highly Active Thorium and Uranium Metallocene Complexes

In the thorium and uranium complexes (C 5 Me 5 ) 2 AnMe 2 , [(C 5 Me 5 ) 2 An(H)(μ-H)] 2 (An = Th, U) and [(C 5 Me 5 ) 2 U(H)] 2 dehydrogenate dimethylamine borane (Me2NH·BH3) at room temperature. Upon mild heating at 45 °C, turnover frequencies (TOFs) of 400 h –1 are obtained, which is comparable to some of the fastest Me 2 NH·BH 3 dehydrogenation catalysts known in the literature. We propose a β-hydride elimination mechanism for dehydrogenation because of the observation of Me 2 N=BH 2 , Me 2 N=BMe 2 , and Me 2 N=BHMe in the 11 B NMR spectra of catalytic and stoichiometric reactions. The similar catalytic metrics between the actinide dimethyl and hydride complexes with Me 2 NH·BH 3 indicate that the actinide hydride complexes are the active catalysts in this chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Bond Dissociation Energy, Ionization Energy, and Electronic Structure of Thorium Dimer

Diatomic thorium, Th 2 , has been investigated using a laser ablation, supersonic expansion source to produce the molecule and resonant two-photon ionization spectroscopy to measure its bond dissociation energy (BDE) and ionization energy (IE). The molecule has a high density of states in the vicinity of its bond dissociation energy, leading to rapid predissociation as soon as this energy is exceeded. The BDE is identified from this predissociation threshold as D 0 (Th 2 ) = 2.857(7) eV, where the assigned error limit is provided in parentheses in units of the last quoted digit. Similarly, the one-photon ionization threshold has been measured, providing the ionization energy IE(Th 2 ) = 5.042(4) eV. Together with a thermochemical cycle and the atomic ionization energy, these values provide the BDE of the cation, giving D 0 (Th 2 + ) = 4.122(8) eV. Computations show that Th 2 has three nearly degenerate low-lying electronic states (1 3 Σ u + , 1 1 Σ g + , and 1 3 Δ g ) with bonding dominated by 7s and 6d orbitals, indicating predominantly transition-metal-like behavior. The 1 3 Σ u + state exhibits a triple bond, whereas the 1 1 Σ g + and 1 3 Δ g states possess quadruple-bond character and correspondingly shorter bonds. Although 1 3 Σ u + is predicted to be the lowest state without spin–orbit coupling, the large spin–orbit stabilization of the 1 3 Δ g state makes its Ω = 1 g component the ground state. Furthermore, the calculated dissociation energy (2.840 eV) and ionization energy of Th 2 (5.098 eV) are both in excellent agreement with experiment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗