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At least 523 records · Page 29

Possible lunar source areas of meteorite ALHA 81005 Geochemical remote sensing information

Antarctic meteorite ALHA 81005 is a regolith breccia apparently sent to earth by an impact event in the lunar highlands. Laboratory studies of this sample provide information that is used to understand the source region on the moon using remote sensing data. The meteorites low thorium content is inconsistent with thorium values measured for the central lunar nearside from orbit with Apollo gamma-ray spectrometers. Similarly, the mineral assemblages inferred from near-IR spectra of small impact craters on the lunar nearside do not exhibit the significant component of olivine and Fe-bearing feldspar that is observed in the meteorite spectra. The existing remote sensing data suggest the most probable source region for ALHA 81005 is the nearside limb or the lunar farside and that the composition of ALHA 81005 represents a surface unit that has not previously been extensively sampled.

Pieters, C. M.↗

U.S. Department of Energy Isotope Program

The National Isotope Development Center (NIDC) interfaces with the User Community and manages the coordination of isotope production across the facilities and business operations involved in the production, sale, and distribution of isotopes. A virtual center, the NIDC is funded by the Isotope Development and Production for Research and Applications (IDPRA) subprogram of the Office of Nuclear Physics in the U.S. Department of Energy Office of Science. PNNL’s Isotope Program operates in a multi-program category-2 nuclear facility, the Radiochemical Processing Laboratory (RPL), that contains 16 hot cells and 20 gloveboxes. As part of the DOE Isotope Program, the Pacific Northwest National Laboratory dispenses strontium-90, neptunium-237, radium-223, and thorium-227. PNNL’s Isotope Program uses a dedicated hot-cell for strontium-90 dispensing and a dedicated glovebox for radium-223 and thorium-227 dispensing. PNNL’s Isotope Program has access to state of the art analytical equipment in the RPL to support their research and production activities. DOE Isotope Program funded research at PNNL has advanced the application of automated radiochemistry for isotope such as zirconium-89 and astatine-211 in partnership with the University of Washington.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Promising Fuel Cycle Options for R&D – Results, Insights, and Future Directions

The Fuel Cycle Options (FCO) campaign in the U.S. DOE Fuel Cycle Research & Development Program conducted a detailed evaluation and screening of nuclear fuel cycles. The process for this study was described at the 2014 ICAPP meeting. This paper reports on detailed insights and questions from the results of the study. The comprehensive study identified continuous recycle in fast reactors as the most promising option, using either U/Pu or U/TRU recycle, and potentially in combination with thermal reactors, as reported at the ICAPP 2014 meeting. This paper describes the examination of the results in detail that indicated that there was essentially no difference in benefit between U/Pu and U/TRU recycle, prompting questions about the desirability of pursuing the more complex U/TRU approach given that the estimated greater challenges for development and deployment. The results will be reported from the current effort that further explores what, if any, benefits of TRU recycle (minor actinides in addition to plutonium recycle) may be in order to inform decisions on future R&D directions. The study also identified continuous recycle using thorium-based fuel cycles as potentially promising, in either fast or thermal systems, but with lesser benefit. Detailed examination of these results indicated that the lesser benefit was confined to only a few of the evaluation metrics, identifying the conditions under which thorium-based fuel cycles would be promising to pursue. For the most promising fuel cycles, the FCO is also conducting analyses on the potential transition to such fuel cycles to identify the issues, challenges, and the timing for critical decisions that would need to be made to avoid unnecessary delay in deployment, including investigation of issues such as the effects of a temporary lack of plutonium fuel resources or supporting infrastructure. These studies are placed in the context of an overall analysis approach designed to provide comprehensive information to the decision-making process.

continuous recycle↗

Evaluation of solid solution formation between ThO2 and δ-Bi2O3 by molecular precursor route

Highlights: • Molecular precursor route for the solid solution evaluation of ThO{sub 2}-BiO{sub 1.5}. • Up to 60 mol % of Bi{sup 3+} could be dissolved in fluorite structured ThO{sub 2}. • Oxygen vacancies manifested as defect bands after Bi{sup 3+} incorporation. • Narrowing of direct band gap with increasing Bi{sup 3+} concentration. - Abstract: The high chelating ability of nitrilotriacetic acid has been advantageously utilized to prepare molecular precursors containing thorium and bismuth. This aided to determine the extent of solid solution formation between thoria and δ-Bi{sub 2}O{sub 3} in fluorite structure by calcining the precursors in air. Up to 60 atomic % of Bi{sup 3+} could be substituted for Th{sup 4+} in fluorite structure beyond which phase separation occurred. Slight increase in cubic lattice constant was observed with increasing bismuth content along with indication of increased tensile strain of lattice. Porous morphology and presence of bismuth in calcined samples were confirmed from SEM and EDX measurements. Defect bands emerged in the Raman spectra near 590 cm{sup −1} in addition to a fluorite band near 460 cm{sup −1} for the bismuth substituted samples. Intermediate energy states were formed by the substitution of Bi{sup 3+} for Th{sup 4+} arising possibly from oxygen vacancies and it resulted in narrowing of direct band gap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Measurement of cross sections for the {sup 232}Th(P,4n){sup 229}Pa reaction at low proton energies

The alpha-emitters {sup 225}Ac and {sup 213}Bi are of great interest for alpha-radioimmunotherapy which uses radioisotopes attached to cancer-seeking antibodies to efficiently treat various types of cancers. Both radioisotopes are daughters of the long-lived {sup 229}Th(t{sub 1/2} = 7880y). {sup 229}Th can be produced by proton irradiation of {sup 232}Th and {sup 230}Th, either directly or through production of isobars that beta-decay into {sup 229}Th. To obtain excitation functions, {sup 232}Th and {sup 230}Th have been irradiated at the On-Line Test Facility at the Holifield Radioactive Ion Beam Facility at ORNL. Benchmark tests conducted with Cu and Ni foils show very good agreement with literature results. The experiments with thorium targets were focused on the production of {sup 229}Pa and its daughter {sup 225}Ac from both {sup 232}Th and {sup 230}Th. Differential cross-sections for production of {sup 229}Pa and other Pa isotopes have been obtained.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Excitation of the Isomeric {sup 229m}Th Nuclear State via an Electronic Bridge Process in {sup 229}Th{sup +}

We consider the excitation of the nuclear transition {sup 229g}Th-{sup 229m}Th near 7.6 eV in singly ionized thorium via an electronic bridge process. The process relies on the excitation of the electron shell by two laser photons whose sum frequency is equal to the nuclear transition frequency. This scheme allows us to determine the nuclear transition frequency with high accuracy. Based on calculations of the electronic level structure of Th{sup +} which combine the configuration-interaction method and many-body perturbation theory, we estimate that a nuclear excitation rate in the range of 10 s{sup -1} can be obtained using conventional laser sources.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

ThO 2 and Th 1– x U x O 2 Nanoscale Materials and Thin Films for Nuclear Science Applications

This study investigates the dynamics and mechanisms of solution combustion synthesis (SCS) for the preparation of nanoscale ThO 2 and Th 1–x U x O 2 materials, utilizing metal nitrates (Th(NO 3 ) 4 and UO 2 (NO 3 ) 2 ) and acetylacetone (C 5 H 8 O 2 ) as reactants dissolved in a 2-methoxyethanol (C 3 H 8 O 2 ) solvent. By combining thermodynamic calculations, dynamic time–temperature profile measurements with differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA), this research reveals how variations in acetylacetone concentration and uranium content influence the structural parameters of the synthesized oxides. The time–temperature measurements show that the heating rate and maximum combustion temperatures are sensitive to acetylacetone concentration. DSC-TGA results indicate shifts in exothermic peak temperatures as the uranium content changes. The complexation between thorium and acetylacetone emerges as a critical factor, impacting combustion parameters and the structural characteristics of the final products. The uniform distribution of Th and U in the Th 1–x U x O 2 solid solution and the formation of nanoscale particles with strained crystallites are considered essential for the low-temperature densification of these materials for nuclear fuel pellet applications. Additionally, high-quality ThO 2 and Th 1–x U x O 2 thin (100–150 nm) films are successfully synthesized via electrospray deposition of combustible solutions followed by a brief period of heat treatment. Furthermore, these films exhibit excellent structural and morphological uniformity, making them ideal candidates for nuclear measurements, irradiation damage studies, and investigations into the physical properties of both pure and mixed oxides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Accelerator Production of {sup 225}Ac For Alpha-Immunotherapy

{sup 225}Ac has tremendous potential for the treatment of metastatic cancer due to the four alpha-particles emitted during its decay to stable {sup 209}Bi. Additionally, it is one of the few alpha-emitters being considered for clinical trials. The anticipated {sup 225}Ac demand for these trials is expected to far exceed the annual worldwide supply of approximately 1,000 mCi/yr. Consequently, the DOE Office of Science has funded investigations into accelerator-based production of {sup 225}Ac. Existing {sup 232}Th(p,x){sup 225}Ac cross section data indicate that up to 480 mCi/day of {sup 225}Ac could be created by bombarding a thick target of natural thorium with 100 MeV protons at the Los Alamos Isotope Production Facility. To verify these predictions, experiments are underway at the Los Alamos Neutron Science Center to measure the {sup 232}Th(p,x){sup 225}Ac production cross sections for protons in the energy range 40-200 MeV, and at 800 MeV. For 800 MeV protons, preliminary results indicate that the {sup 225}Ac production cross section is 12.4{+-}0.6 mb and the {sup 225}Ra production cross section is 3.2{+-}0.2 mb. Moreover, preliminary results suggest that the {sup 227}Ac production cross section is 16{+-}1 mb. Experiments to measure these same cross sections at proton energies below 200 MeV are planned for the last half of calendar year 2010.

43 PARTICLE ACCELERATORS↗

Renewability and sustainability aspects of nuclear energy

Renewability and sustainability aspects of nuclear energy have been presented on the basis of two different technologies: (1) Conventional nuclear technology; CANDU reactors. (2) Emerging nuclear technology; fusion/fission (hybrid) reactors. Reactor grade (RG) plutonium, {sup 233}U fuels and heavy water moderator have given a good combination with respect to neutron economy so that mixed fuel made of (ThO{sub 2}/RG‐PuO{sub 2}) or (ThC/RG-PuC) has lead to very high burn up grades. Five different mixed fuel have been selected for CANDU reactors composed of 4 % RG‐PuO{sub 2} + 96 % ThO{sub 2}; 6 % RG‐PuO{sub 2} + 94 % ThO{sub 2}; 10 % RG‐PuO{sub 2} + 90 % ThO{sub 2}; 20 % RG‐PuO{sub 2} + 80 % ThO{sub 2}; 30 % RG‐PuO{sub 2} + 70 % ThO{sub 2}, uniformly taken in each fuel rod in a fuel channel. Corresponding operation lifetimes have been found as ∼ 0.65, 1.1, 1.9, 3.5, and 4.8 years and with burn ups of ∼ 30 000, 60 000, 100 000, 200 000 and 290 000 MW.d/ton, respectively. Increase of RG‐PuO{sub 2} fraction in radial direction for the purpose of power flattening in the CANDU fuel bundle has driven the burn up grade to 580 000 MW.d/ton level. A laser fusion driver power of 500 MW{sub th} has been investigated to burn the minor actinides (MA) out of the nuclear waste of LWRs. MA have been homogenously dispersed as carbide fuel in form of TRISO particles with volume fractions of 0, 2, 3, 4 and 5 % in the Flibe coolant zone in the blanket surrounding the fusion chamber. Tritium breeding for a continuous operation of the fusion reactor is calculated as TBR = 1.134, 1.286, 1.387, 1.52 and 1.67, respectively. Fission reactions in the MA fuel under high energetic fusion neutrons have lead to the multiplication of the fusion energy by a factor of M = 3.3, 4.6, 6.15 and 8.1 with 2, 3, 4 and 5 % TRISO volume fraction at start up, respectively. Alternatively with thorium, the same fusion driver would produce ∼160 kg {sup 233}U per year in addition to fission energy production in situ, multiplying the fusion energy by a factor of ∼1.3.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Correlation consistent basis sets for actinides. I. The Th and U atoms

New correlation consistent basis sets based on both pseudopotential (PP) and all-electron Douglas-Kroll-Hess (DKH) Hamiltonians have been developed from double- to quadruple-zeta quality for the actinide atoms thorium and uranium. Sets for valence electron correlation (5f6s6p6d), cc − pV nZ − PP and cc − pV nZ − DK3, as well as outer-core correlation (valence + 5s5p5d), cc − pwCV nZ − PP and cc − pwCV nZ − DK3, are reported (n = D, T, Q). The -PP sets are constructed in conjunction with small-core, 60-electron PPs, while the -DK3 sets utilized the 3rd-order Douglas-Kroll-Hess scalar relativistic Hamiltonian. Both series of basis sets show systematic convergence towards the complete basis set limit, both at the Hartree-Fock and correlated levels of theory, making them amenable to standard basis set extrapolation techniques. To assess the utility of the new basis sets, extensive coupled cluster composite thermochemistry calculations of ThF{sub n} (n = 2 − 4), ThO{sub 2}, and UF{sub n} (n = 4 − 6) have been carried out. After accurately accounting for valence and outer-core correlation, spin-orbit coupling, and even Lamb shift effects, the final 298 K atomization enthalpies of ThF{sub 4}, ThF{sub 3}, ThF{sub 2}, and ThO{sub 2} are all within their experimental uncertainties. Bond dissociation energies of ThF{sub 4} and ThF{sub 3}, as well as UF{sub 6} and UF{sub 5}, were similarly accurate. The derived enthalpies of formation for these species also showed a very satisfactory agreement with experiment, demonstrating that the new basis sets allow for the use of accurate composite schemes just as in molecular systems composed only of lighter atoms. The differences between the PP and DK3 approaches were found to increase with the change in formal oxidation state on the actinide atom, approaching 5-6 kcal/mol for the atomization enthalpies of ThF{sub 4} and ThO{sub 2}. The DKH3 atomization energy of ThO{sub 2} was calculated to be smaller than the DKH2 value by ∼1 kcal/mol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The use of Eupatorium Odoratum as bio-monitor for radionuclides determination in Manjung, Perak

The accumulation of radionuclides in plants can be used as bio-monitoring in the environment. This technique is a cost-effective as the plants used to uptake deposited radionuclides from soil, commonly as soil-to-plant transfer factor (TF), which is widely used for calculating radiological risk. Radionuclides deposited in the soil carry by the air as particles or gases lead to the accumulation in soil. Eupatorium odoratum, known as pokok kapal terbang in Malaysia was chosen as sample for their abundances and properties to measure surface soil contamination. The plants were collected in three different directions (North, North-East and South-East) from Manjung district. The plants were collected in same size and then separated in to three parts (roots, stems and leaves) to determine the transfer factor from soil to each part. The concentrations of thorium (Th) and uranium (U) were analyzed using Energy Disperse X-Ray Fluorescence (EDXRF) and found in the range of 1.20-3.50 mg/kg and 1.20-3.90 mg/kg in roots, 1.40-3.90 mg/kg and 1.50-5.90 mg/kg in stems and 1.50-2.50 mg/kg and 2.00-6.00 mg/kg in leaves, respectively. Transfer factor (TF) was calculated through concentrations as reported in this article and show that the plants have transferred and accumulated radionuclides in significant values. From radionuclides concentrations in topsoil, the radiological risk was calculated and the present result show that external hazard index (H{sub ex}) is below than unity indicate low radiological risk at that area.

54 ENVIRONMENTAL SCIENCES↗

Surface physicochemical properties and decay of the low-lying isomer in the {sup 229}Th nucleus

The effect of the {sup 229}Th nucleus proximity to the CsI surface on the decay probability of its anomalously low lying isomeric level is studied. Results of experimental and theoretical studies show that the CsI surface does not produce chemical bonding with Th and does not noticeably change its valence shells. Hence, it is an optimal substrate for measuring the probability of the {sup 229}Th isomer state decay via internal electron conversion. The half-life of the {sup 229}Th{sup m} isomer in the thorium atom is calculated for neutral chemical environment. (paper)

07 ISOTOPE AND RADIATION SOURCES↗

Comprehensive Baseline Environmental Monitoring of an Interim Legacy Waste Store in Arid Zone Australia - 20062

Radionuclide containing soil and rubble from the clean-up of a former uranium, thorium and rare earth minerals processing research facility carried out in the early 50's and 60's is currently stored at the Woomera Test Range in South Australia awaiting final disposal. Prior to developing a final disposal pathway commensurate with waste acceptance criteria, a comprehensive baseline environmental monitoring has been carried out to establish the background radiation levels. The survey included in situ gamma scanning of the surface soil ({sup 238}U, {sup 232}Th, {sup 40}K), a laboratory analysis of 86 soil samples (from 0-20 cm depth), which involved XRF measurements (U, Th, and rare earth metals) and spectroscopic analysis ({sup 238}U, {sup 232}Th, {sup 226}Ra and daughter nuclides). A time series of radon concentration measurements in air was established, while soil radon ({sup 222}Rn) and thoron ({sup 220}Rn) flux measurements were undertaken at 18 different locations. The 2018 comprehensive baseline survey demonstrated radiation levels in the immediate vicinity of the Woomera interim waste store are typical background values of soil and rock. No contamination was detected. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Dynamic Analysis of the Next Generation Molten-Salt Breeder Reactor System

The conceptual design of a 1000 MWe two-fluid molten-salt breeder reactor (MSBR) station was performed during 1966-1970 at Oak Ridge National Laboratory (ORNL) with the goal of using the U-233 fuel cycle. This modular design with four reactor modules has an electrical output of 250 MW/module. The abundance of Th-232 was attractive in converting it to U-233 in a thermal breeder reactor. The two-fluid reactor is graphite-moderated 'with a {sup 7}LiF-BeF{sub 2}-UF{sub 4} fuel salt circulated through the core and a {sup 7}LiF-ThF{sub 4}-BeF{sub 2} blanket salt circulated through separate flow channels distributed throughout the core, as well as in a surrounding under-moderated region'. This reactor design has the advantages of not producing Pu isotopes and easy chemical separation of U-233 in the blanket material. The low fuel cost and the graphite replacement cost are attractive for such a design, with an estimated cost of $141/kW at 1968-dollar value. Potential non-proliferation features of MSBR, the low costs of raw materials, and established chemical separation of fission products are important factors in further development of MSBRs as an alternative to current light water reactors. These reactors are often referred to as liquid fluoride thorium reactor (LFTR). The current research on the modeling of the MSBR is based on an earlier work on the preliminary dynamic model of the MSBR concept. Revisions are made to the original model. The physics parameters have been modified for the current modeling effort based on additional information including more recent values of model parameters from and several typographical misprints in equations and values. Details of this effort will be presented in a full follow-up paper. This work presents the detailed nodal models of reactor fluid core, blanket fluid loop, graphite moderator, fuel fluid heat exchanger, and the blanket fluid heat exchanger. A set of simulations has been performed to validate the model using the commercial software MATLAB{sup TM}-Simulink. Simulations were performed for the cases of source perturbation and reactivity perturbation. The model is inherently nonlinear. A description of the MSBR conceptual design, along with a tabulation of relevant system parameters, is presented. The results of simulation demonstrate stable behavior of the MSBR dynamics, temperature feedback effects, and load-following capability of the MSBR system.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Isolation of a TMTAA-Based Radical in Uranium bis-TMTAA Complexes

Here, we report the synthesis, characterization, and electronic structure studies of a series of thorium(IV) and uranium(IV) bis-tetramethyltetraazaannulene complexes. These sandwich complexes show remarkable stability towards air and moisture, even at elevated temperatures. Electrochemical studies show the uranium complex to be stable in three different oxidation states; isolation of the oxidized species reveals a rare case of a non-innocent tetramethyltetraazaannulene (TMTAA) ligand.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Isolation of a TMTAA-Based Radical in Uranium bis-TMTAA Complexes

Here, we report the synthesis, characterization, and electronic structure studies of a series of thorium(IV) and uranium(IV) bis-tetramethyltetraazaannulene complexes. These sandwich complexes demonstrate remarkable stability towards air and moisture, even at elevated temperatures. Electrochemical studies show the uranium complex to be stable in three different oxidation states; isolation of the oxidized species revealed a rare case of a non-innocent TMTAA ligand.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nuclear Problems of Thermonuclear Power Generation

The current status of the nuclear problems of the thermonuclear fusion research program and, in particular, tritium, is discussed. It is noted that thermonuclear power generation without a uranium or thorium blanket is problematic; the key nuclear problems of the fusion–fission hybrid system remain unsolved. It is proposed that an integrated strategic analysis be made of the thermonuclear research program and the realistic possibilities of its application in nuclear power-engineering.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗