The effect of fuel chemistry on UO2 dissolution

DOE Office of Scientific and Technical Information (OSTI.GOV)

Casella, Amanda; Hanson, Brady; Miller, William

2016-08-01

The dissolution rate of both unirradiated UO2 and used nuclear fuel has been studied by numerous countries as part of the performance assessment of proposed geologic repositories. In the scenario of waste package failure and groundwater infiltration into the fuel, the effects of variables such as temperature, dissolved oxygen, and water and fuel chemistry on the dissolution rates of the fuel are necessary to provide a quantitative estimate of the potential release over geologic time frames. The primary objective of this research was to determine the influence these parameters have on the dissolution rate of unirradiated UO2 under repository conditionsmore » and compare them to the rates predicted by current dissolution models. Both unirradiated UO2 and UO2 doped with varying concentrations of Gd2O3, to simulate used fuel composition after long time periods where radiolysis has minor contributions to dissolution, were examined. In general, a rise in temperature increased the dissolution rate of UO2 and had a larger effect on pure UO2 than on those doped with Gd2O3. Oxygen dependence was observed in the UO2 samples with no dopant and increased as the temperature rose; in the doped fuels less dependence was observed. The addition of gadolinia into the UO2 matrix showed a significant decrease in the dissolution rate. The matrix stabilization effect resulting from the dopant proved even more beneficial in lowering the dissolution rate at higher temperatures and dissolved O2 concentrations in the leachate where the rates would typically be elevated.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andersson, Anders David Ragnar; Stanek, Christopher Richard; Noordhoek, Mark

Uranium silicides, in particular U 3Si 2, are being explored as an advanced nuclear fuel with increased accident tolerance as well as competitive economics compared to the baseline UO 2 fuel. They benefit from high thermal conductivity (metallic) compared to UO 2 fuel (insulator or semi-conductor) used in current Light Water Reactors (LWRs). The U-Si fuels also have higher fissile density. In order to perform meaningful engineering scale nuclear fuel performance simulations, the material properties of the fuel, including the response to irradiation environments, must be known. Unfortunately, the data available for USi fuels are rather limited, in particular formore » the temperature range where LWRs would operate. The ATF HIP is using multi-scale modeling and simulations to address this knowledge gap.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andersson, Anders David Ragnar; Stanek, Christopher Richard; Noordhoek, Mark J.

Uranium silicides, in particular U 3Si 2, are being explored as an advanced nuclear fuel with increased accident tolerance as well as competitive economics compared to the baseline UO2 fuel. They benefit from high thermal conductivity (metallic) compared to UO 2 fuel (insulator or semi-conductor) used in current Light Water Reactors (LWRs). The U-Si fuels also have higher fissile density. In order to perform meaningful engineering scale nuclear fuel performance simulations, the material properties of the fuel, including the response to irradiation environments, must be known. Unfortunately, the data available for USi fuels are rather limited, in particular for themore » temperature range where LWRs would operate. The ATF HIP is using multi-scale modeling and simulations to address this knowledge gap.« less

Incorporation mechanisms of actinide elements into the structures of U 6+ phases formed during the oxidation of spent nuclear fuel

NASA Astrophysics Data System (ADS)

Burns, Peter C.; Ewing, Rodney C.; Miller, Mark L.

1997-05-01

Uranyl oxide hydrate and uranyl silicate phases will form due to the corrosion and alteration of spent nuclear fuel under oxidizing conditions in silica-bearing solution. The actinide elements in the spent fuel may be incorporated into the structures of these secondary U6+ phases during the long-term corrosion of the UO 2 in spent fuel. The incorporation of actinide elements into the crystal structures of the alteration products may decrease actinide mobility. The crystal chemistry of the various oxidation states of the actinide elements of environmental concern is examined to identify possible incorporation mechanisms. The substitutions Pu 6+U 6+ and (Pu 5+, Np 5+)U 6+ should readily occur in many U 6+ structures, although structural modification may be required to satisfy local bond-valence requirements. Crystal-chemical characteristics of the U 6+ phases indicate that An 4+ (An: actinide)U 6+ substitution is likely to occur in the sheets of uranyl polyhedra that occur in the structures of the minerals schoepite, [(UO 2) 8O 2(OH) 12](H 2O) 12, ianthinite, [U 24+ (UO 2) 4O 6(OH) 4(H 2O) 4](H 2O) 5, becquerelite, Ca[(UO 2) 3O 2(OH) 3] 2(H 2O) 8, compreignacite, K 2[(UO 2) 3O 2(OH) 3] 2(H 2O) 8, α-uranophane, Ca[(UO 2)(SiO 3OH)] 2(H 2O) 5, and boltwoodite, K(H 2O)[(UO 2)(SiO 4)], all of which are likely to form due to the oxidation and alteration of the UO 2 in spent fuel. The incorporation of An 3+ into the sheets of the structures of α-uranophane and boltwoodite, as well as interlayer sites of various uranyl phases, may occur.

Effects of Beryllium and Compaction Pressure on the Thermal Diffusivity of Uranium Dioxide Fuel Pellets

NASA Astrophysics Data System (ADS)

Camarano, D. M.; Mansur, F. A.; Santos, A. M. M.; Ferraz, W. B.; Ferreira, R. A. N.

2017-09-01

In nuclear reactors, the performance of uranium dioxide (UO2) fuel is strongly dependent on the thermal conductivity, which directly affects the fuel pellet temperature, the fission gas release and the fuel rod mechanical behavior during reactor operation. The use of additives to improve UO2 fuel performance has been investigated, and beryllium oxide (BeO) appears as a suitable additive because of its high thermal conductivity and excellent chemical compatibility with UO2. In this paper, UO2-BeO pellets were manufactured by mechanical mixing, pressing and sintering processes varying the BeO contents and compaction pressures. Pellets with BeO contents of 2 wt%, 3 wt%, 5 wt% and 7 wt% BeO were pressed at 400 MPa, 500 MPa and 600 MPa. The laser flash method was applied to determine the thermal diffusivity, and the results showed that the thermal diffusivity tends to increase with BeO content. Comparing thermal diffusivity results of UO2 with UO2-BeO pellets, it was observed that there was an increase in thermal diffusivity of at least 18 % for the UO2-2 wt% BeO pellet pressed at 400 MPa. The maximum relative expanded uncertainty (coverage factor k = 2) of the thermal diffusivity measurements was estimated to be 9 %.

Analytical determination of thermal conductivity of W-UO2 and W-UN CERMET nuclear fuels

NASA Astrophysics Data System (ADS)

Webb, Jonathan A.; Charit, Indrajit

2012-08-01

The thermal conductivity of tungsten based CERMET fuels containing UO2 and UN fuel particles are determined as a function of particle geometry, stabilizer fraction and fuel-volume fraction, by using a combination of an analytical approach and experimental data collected from literature. Thermal conductivity is estimated using the Bruggeman-Fricke model. This study demonstrates that thermal conductivities of various CERMET fuels can be analytically predicted to values that are very close to the experimentally determined ones.

Non-Destructive Characterization of UO2+x Nuclear Fuels

DOE PAGES

Pokharel, Reeju; Brown, Donald W.; Clausen, Bjørn; ...

2017-10-27

This article describes the effect of fabrication conditions on as-sintered microstructures of various stoichiometric ratios of uranium dioxide, UO 2+x, with the aim of enhancing the understanding of fabrication process and developing and validating a predictive microstructurebased model for fuel performance. We demonstrate the ability of novel, non-destructive methods such as near-field high-energy X-ray diffraction microscopy (nf-HEDM) and micro-computed tomography (μ-CT) to probe bulk samples of high-Z materials by non-destructively characterizing three samples: UO 2.00, UO 2.11, and UO 2.16, which were sintered at 1450°C for 4 hours. The measured 3D microstructures revealed that grain size and porosity were influencedmore » by deviation from stoichiometry.« less

Colloids from the aqueous corrosion of uranium nuclear fuel

NASA Astrophysics Data System (ADS)

Kaminski, M. D.; Dimitrijevic, N. M.; Mertz, C. J.; Goldberg, M. M.

2005-12-01

Colloids may enhance the subsurface transport of radionuclides and potentially compromise the long-term safe operation of the proposed radioactive waste repository at Yucca Mountain. Little data is available on colloid formation for the many different waste forms expected to be buried in the repository. This work expands the sparse database on colloids formed during the corrosion of metallic uranium nuclear fuel. We characterized spherical UO 2 and nickel-rich montmorilonite smectite-clay colloids formed during the corrosion of uranium metal fuel under bathtub conditions at 90 °C. Iron and chromium oxides and calcium carbonate colloids were present but were a minor population. The estimated upper concentration of the UO 2 and clays was 4 × 10 11 and 7 × 10 11-3 × 10 12 particles/L, respectively. However, oxygen eventually oxidized the UO 2 colloids, forming long filaments of weeksite K 2(UO 2) 2Si 6O 15 · 4H 2O that settled from solution, reducing the UO 2 colloid population and leaving predominantly clay colloids. The smectite colloids were not affected by oxygen. Plutonium was not directly observed within the UO 2 colloids but partitioned completely to the colloid size fraction. The plutonium concentration in the colloidal fraction was slightly higher than the value used in the viability assessment model, and does not change in concentration with exposure to oxygen. This paper provides conclusive evidence for single-phase radioactive colloids composed of UO 2. However, its impact on repository safety is probably small since oxygen and silica availability will oxidize and effectively precipitate the UO 2 colloids from concentrated solutions.

UO2 fuel pellets fabrication via Spark Plasma Sintering using non-standard molybdenum die

NASA Astrophysics Data System (ADS)

Papynov, E. K.; Shichalin, O. O.; Mironenko, A. Yu; Tananaev, I. G.; Avramenko, V. A.; Sergienko, V. I.

2018-02-01

The article investigates spark plasma sintering (SPS) of commercial uranium dioxide (UO2) powder of ceramic origin into highly dense fuel pellets using non-standard die instead of usual graphite die. An alternative and formerly unknown method has been suggested to fabricate UO2 fuel pellets by SPS for excluding of typical problems related to undesirable carbon diffusion. Influence of SPS parameters on chemical composition and quality of UO2 pellets has been studied. Also main advantages and drawbacks have been revealed for SPS consolidation of UO2 in non-standard molybdenum die. The method is very promising due to high quality of the final product (density 97.5-98.4% from theoretical, absence of carbon traces, mean grain size below 3 μm) and mild sintering conditions (temperature 1100 ºC, pressure 141.5 MPa, sintering time 25 min). The results are interesting for development and probable application of SPS in large-scale production of nuclear ceramic fuel.

Modeling the UO2 ex-AUC pellet process and predicting the fuel rod temperature distribution under steady-state operating condition

NASA Astrophysics Data System (ADS)

Hung, Nguyen Trong; Thuan, Le Ba; Thanh, Tran Chi; Nhuan, Hoang; Khoai, Do Van; Tung, Nguyen Van; Lee, Jin-Young; Jyothi, Rajesh Kumar

2018-06-01

Modeling uranium dioxide pellet process from ammonium uranyl carbonate - derived uranium dioxide powder (UO2 ex-AUC powder) and predicting fuel rod temperature distribution were reported in the paper. Response surface methodology (RSM) and FRAPCON-4.0 code were used to model the process and to predict the fuel rod temperature under steady-state operating condition. Fuel rod design of AP-1000 designed by Westinghouse Electric Corporation, in these the pellet fabrication parameters are from the study, were input data for the code. The predictive data were suggested the relationship between the fabrication parameters of UO2 pellets and their temperature image in nuclear reactor.

Effect of point defects on the thermal conductivity of UO2: molecular dynamics simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiang-Yang; Stanek, Christopher Richard; Andersson, Anders David Ragnar

2015-07-21

The thermal conductivity of uranium dioxide (UO 2) fuel is an important materials property that affects fuel performance since it is a key parameter determining the temperature distribution in the fuel, thus governing, e.g., dimensional changes due to thermal expansion, fission gas release rates, etc. [1] The thermal conductivity of UO 2 nuclear fuel is also affected by fission gas, fission products, defects, and microstructural features such as grain boundaries. Here, molecular dynamics (MD) simulations are carried out to determine quantitatively, the effect of irradiation induced point defects on the thermal conductivity of UO 2, as a function of defectmore » concentrations, for a range of temperatures, 300 – 1500 K. The results will be used to develop enhanced continuum thermal conductivity models for MARMOT and BISON by INL. These models express the thermal conductivity as a function of microstructure state-variables, thus enabling thermal conductivity models with closer connection to the physical state of the fuel [2].« less

Development Status of a CVD System to Deposit Tungsten onto UO2 Powder via the WCI6 Process

NASA Technical Reports Server (NTRS)

Mireles, O. R.; Kimberlin, A.; Broadway, J.; Hickman, R.

2014-01-01

Nuclear Thermal Propulsion (NTP) is under development for deep space exploration. NTP's high specific impulse (> 850 second) enables a large range of destinations, shorter trip durations, and improved reliability. W-60vol%UO2 CERMET fuel development efforts emphasize fabrication, performance testing and process optimization to meet service life requirements. Fuel elements must be able to survive operation in excess of 2850 K, exposure to flowing hydrogen (H2), vibration, acoustic, and radiation conditions. CTE mismatch between W and UO2 result in high thermal stresses and lead to mechanical failure as a result UO2 reduction by hot hydrogen (H2) [1]. Improved powder metallurgy fabrication process control and mitigated fuel loss can be attained by coating UO2 starting powders within a layer of high density tungsten [2]. This paper discusses the advances of a fluidized bed chemical vapor deposition (CVD) system that utilizes the H2-WCl6 reduction process.

Synthesis and sintering of UN-UO2 fuel composites

NASA Astrophysics Data System (ADS)

Jaques, Brian J.; Watkins, Jennifer; Croteau, Joseph R.; Alanko, Gordon A.; Tyburska-Püschel, Beata; Meyer, Mitch; Xu, Peng; Lahoda, Edward J.; Butt, Darryl P.

2015-11-01

The design and development of an economical, accident tolerant fuel (ATF) for use in the current light water reactor (LWR) fleet is highly desirable for the future of nuclear power. Uranium mononitride has been identified as an alternative fuel with higher uranium density and thermal conductivity when compared to the benchmark, UO2, which could also provide significant economic benefits. However, UN by itself reacts with water at reactor operating temperatures. In order to reduce its reactivity, the addition of UO2 to UN has been suggested. In order to avoid carbon impurities, UN was synthesized from elemental uranium using a hydride-dehydride-nitride thermal synthesis route prior to mixing with up to 10 wt% UO2 in a planetary ball mill. UN and UN - UO2 composite pellets were sintered in Ar - (0-1 at%) N2 to study the effects of nitrogen concentration on the evolved phases and microstructure. UN and UN-UO2 composite pellets were also sintered in Ar - 100 ppm N2 to assess the effects of temperature (1700-2000 °C) on the final grain morphology and phase concentration.

Sequestration of radioactive iodine in silver-palladium phases in commercial spent nuclear fuel

NASA Astrophysics Data System (ADS)

Buck, Edgar C.; Mausolf, Edward J.; McNamara, Bruce K.; Soderquist, Chuck Z.; Schwantes, Jon M.

2016-12-01

Radioactive iodine is the Achilles' heel in the design for the safe geological disposal of spent uranium oxide (UO2) nuclear fuel. Furthermore, iodine's high volatility and aqueous solubility were mainly responsible for the high early doses released during the accident at Fukushima Daiichi in 2011. Studies Kienzler et al., however, have indicated that the instant release fraction (IRF) of radioiodine (131/129I) does not correlate directly with increasing fuel burn-up. In fact, there is a peak in the release of iodine at around 50-60 MW d/kgU, and with increasing burn-up, the IRF of 131/129I decreases. The reasons for this decrease have not fully been understood. We have performed microscopic analysis of chemically processed high burn-up UO2 fuel (80 MW d/kgU) and have found recalcitrant nano-particles containing, Pd, Ag, I, and Br, possibly consistent with a high pressure phase of silver iodide in the undissolved residue. It is likely that increased levels of Ag and Pd from 239Pu fission in high burnup fuels leads to the formation of these metal halides. The occurrence of these phases in UO2 nuclear fuels may reduce the impact of long-lived 129I on the repository performance assessment calculations.

Processing and microstructural characterisation of a UO2-based ceramic for disposal studies on spent AGR fuel

NASA Astrophysics Data System (ADS)

Hiezl, Z.; Hambley, D. I.; Padovani, C.; Lee, W. E.

2015-01-01

Preparation and characterisation of a Simulated Spent Nuclear Fuel (SIMFuel), which replicates the chemical state and microstructure of Spent Nuclear Fuel (SNF) discharged from a UK Advanced Gas-cooled Reactor (AGR) after a cooling time of 100 years is described. Given the relatively small differences in radionuclide inventory expected over longer time periods, the SIMFuel studied in this work is expected to be also representative of spent fuel after significantly longer periods (e.g. 1000 years). Thirteen stable elements were added to depleted UO2 and sintered to simulate the composition of fuel pellets after burn-ups of 25 and 43 GWd/tU and, as a reference, pure UO2 pellets were also investigated. The fission product distribution was calculated using the FISPIN code provided by the UK National Nuclear Laboratory. SIMFuel pellets were up to 92% dense and during the sintering process in H2 atmosphere Mo-Ru-Rh-Pd metallic precipitates and grey-phase ((Ba, Sr)(Zr, RE) O3 oxide precipitates) formed within the UO2 matrix. These secondary phases are present in real PWR and AGR SNF. Metallic precipitates are generally spherical and have submicron particle size (0.8 ± 0.7 μm). Spherical oxide precipitates in SIMFuel measured up to 30 μm in diameter, but no data were available in the public domain to compare this to AGR SNF. The grain size of actual AGR SNF (∼ 3-30 μm) is larger than that measured in AGR SIMFuel (∼ 2-5 μm).

Characterization of Actinides Complexed to Nuclear Fuel Constituents Using ESI-MS.

PubMed

McDonald, Luther W; Campbell, James A; Vercouter, Thomas; Clark, Sue B

2016-03-01

Electrospray ionization-mass spectrometry (ESI-MS) was tested for its use in monitoring spent nuclear fuel (SNF) constituents including U, Pu, dibutyl phosphate (DBP), and tributyl phosphate (TBP). Both positive and negative ion modes were used to evaluate the speciation of U and Pu with TBP and DBP. Furthermore, apparent stability constants were determined for U complexed to TBP and DBP. In positive ion mode, TBP produced a strong signal with and without complexation to U or Pu, but, in negative ion mode, no TBP, U-TBP, or Pu-TBP complexes were observed. Apparent stability constants were determined for [UO2(NO3)2(TBP)2], [UO2(NO3)2(H2O)(TBP)2], and [UO2(NO3)2(TBP)3]. In contrast DBP, U-DBP, and Pu-DBP complexes were observed in both positive and negative ion modes. Apparent stability constants were determined for the species [UO2(DBP)], [UO2(DBP)3], and [UO2(DBP)4]. Analyzing mixtures of U or Pu with TBP and DBP yielded the formation of ternary complexes whose stoichiometry was directly related to the ratio of TBP to DBP. The ESI-MS protocols used in this study will further demonstrate the utility of ESI-MS and its applicability to process control monitoring in SNF reprocessing facilities.

High wettability of liquid caesium iodine with solid uranium dioxide.

PubMed

Kurosaki, Ken; Suzuki, Masanori; Uno, Masayoshi; Ishii, Hiroto; Kumagai, Masaya; Anada, Keito; Murakami, Yukihiro; Ohishi, Yuji; Muta, Hiroaki; Tanaka, Toshihiro; Yamanaka, Shinsuke

2017-09-13

In March 2011, the Fukushima Daiichi Nuclear Power Plant accident caused nuclear fuel to melt and the release of high-volatility fission products into the environment. Caesium and iodine caused environmental contamination and public exposure. Certain fission-product behaviours remain unclear. We found experimentally that liquid CsI disperses extremely favourably toward solid UO 2 , exhibiting a contact angle approaching zero. We further observed the presence of CsI several tens of micrometres below the surface of the solid UO 2 sample, which would be caused by the infiltration of pores network by liquid CsI. Thus, volatile fission products released from molten nuclear fuels with complex internal composition and external structure migrate or evaporate to varying extents, depending on the nature of the solid-liquid interface and the fuel material surface, which becomes the pathway for the released fission products. Introducing the concept of the wettability of liquid chemical species of fission products in contact with solid fuels enabled developing accurate behavioural assessments of volatile fission products released by nuclear fuel.

Pyrolytic carbon-coated nuclear fuel

DOEpatents

Lindemer, Terrence B.; Long, Jr., Ernest L.; Beatty, Ronald L.

1978-01-01

An improved nuclear fuel kernel having at least one pyrolytic carbon coating and a silicon carbon layer is provided in which extensive interaction of fission product lanthanides with the silicon carbon layer is avoided by providing sufficient UO.sub.2 to maintain the lanthanides as oxides during in-reactor use of said fuel.

The effect of ion irradiation on the dissolution of UO 2 and UO 2 -based simulant fuel

DOE PAGES

Popel, Aleksej J.; Wietsma, Thomas W.; Engelhard, Mark H.; ...

2017-11-21

Our aim is to study the separate effect of fission fragment damage on the dissolution of simulant UK advanced gas-cooled reactor nuclear fuel in water. Plain UO 2 and UO 2 samples, doped with inactive fission products to simulate 43 GWd/tU of burn-up, were fabricated. A set of these samples were then irradiated with 92 MeV 129Xe 23+ ions to a fluence of 4.8 × 10 15 ions/cm 2 to simulate the fission damage that occurs within nuclear fuels. The primary effect of the irradiation on the UO 2 samples, observed by scanning electron microscopy, was to induce a smootheningmore » of the surface features and formation of hollow blisters, which was attributed to multiple overlap of ion tracks. Dissolution experiments were conducted in single-pass flow-through (SPFT) mode under anoxic conditions (<0.1 O 2 ppm in Ar) to study the effect of the induced irradiation damage on the dissolution of the UO 2 matrix with data collection capturing six minute intervals for several hours. These time-resolved data showed that the irradiated samples showed a higher initial release of uranium than unirradiated samples, but that the uranium concentrations converged towards ~10 -9 mol/l after a few hours. And apart from the initial spike in uranium concentration, attributed to irradiation induced surficial micro-structural changes, no noticeable difference in uranium chemistry as measured by X-ray electron spectroscopy or ‘effective solubility’ was observed between the irradiated, doped and undoped samples in this work. Some secondary phase formation was observed on the surface of UO 2 samples after the dissolution experiment.« less

The effect of ion irradiation on the dissolution of UO 2 and UO 2 -based simulant fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Popel, Aleksej J.; Wietsma, Thomas W.; Engelhard, Mark H.

Our aim is to study the separate effect of fission fragment damage on the dissolution of simulant UK advanced gas-cooled reactor nuclear fuel in water. Plain UO 2 and UO 2 samples, doped with inactive fission products to simulate 43 GWd/tU of burn-up, were fabricated. A set of these samples were then irradiated with 92 MeV 129Xe 23+ ions to a fluence of 4.8 × 10 15 ions/cm 2 to simulate the fission damage that occurs within nuclear fuels. The primary effect of the irradiation on the UO 2 samples, observed by scanning electron microscopy, was to induce a smootheningmore » of the surface features and formation of hollow blisters, which was attributed to multiple overlap of ion tracks. Dissolution experiments were conducted in single-pass flow-through (SPFT) mode under anoxic conditions (<0.1 O 2 ppm in Ar) to study the effect of the induced irradiation damage on the dissolution of the UO 2 matrix with data collection capturing six minute intervals for several hours. These time-resolved data showed that the irradiated samples showed a higher initial release of uranium than unirradiated samples, but that the uranium concentrations converged towards ~10 -9 mol/l after a few hours. And apart from the initial spike in uranium concentration, attributed to irradiation induced surficial micro-structural changes, no noticeable difference in uranium chemistry as measured by X-ray electron spectroscopy or ‘effective solubility’ was observed between the irradiated, doped and undoped samples in this work. Some secondary phase formation was observed on the surface of UO 2 samples after the dissolution experiment.« less

Effect of Al(OH)3 on the sintering of UO2-Gd2O3 fuel pellets with addition of U3O8 from recycle

NASA Astrophysics Data System (ADS)

dos Santos, Lauro Roberto; Durazzo, Michelangelo; Urano de Carvalho, Elita Fontenele; Riella, Humberto Gracher

2017-09-01

The incorporation of gadolinium as burnable poison directly into nuclear fuel is important for reactivity compensation, which enables longer fuel cycles. The function of the burnable poison fuel is to control the neutron population in the reactor core during its startup and the beginning of the fuel burning cycle to extend the use of the fuel. The implementation of UO2-Gd2O3 poisoned fuel in Brazil has been proposed according to the future requirements established for the Angra-2 nuclear power plant. The UO2 powder used is produced from the Ammonium Uranyl Carbonate (AUC). The incorporation of Gd2O3 powder directly into the AUC-derived UO2 powder by dry mechanical blending is the most attractive process, because of its simplicity. Nevertheless, processing by this method leads to difficulties while obtaining sintered pellets with the minimum required density. The cause of the low densities is the bad sintering behavior of the UO2-Gd2O3 mixed fuel, which shows a blockage in the sintering process that hinders the densification. This effect has been overcome by microdoping of the fuel with small quantities of aluminum. The process for manufacturing the fuel inevitably generates uranium-rich scraps from various sources. This residue is reincorporated into the production process in the form of U3O8 powder additions. The addition of U3O8 also hinders densification in sintering. This study was carried out to investigate the influence of both aluminum and U3O8 additives on the density of fuel pellets after sintering. As the effects of these additives are counterposed, this work studied the combined effect thereof, seeking to find an applicable composition for the production process. The experimental results demonstrated the effectiveness of aluminum, in the form of Al(OH)3, as an additive to promote increase in the densification of the (U,Gd)O2 pellets during sintering, even with high additions of U3O8 recycled from the manufacturing process.

Synthesis and sintering of UN-UO 2 fuel composites

DOE PAGES

Jaques, Brian J.; Watkins, Jennifer; Croteau, Joseph R.; ...

2015-06-17

In this study, the design and development of an economical, accident tolerant fuel (ATF) for use in the current light water reactor (LWR) fleet is highly desirable for the future of nuclear power. Uranium mononitride has been identified as an alternative fuel with higher uranium density and thermal conductivity when compared to the benchmark, UO 2, which could also provide significant economic benefits. However, UN by itself reacts with water at reactor operating temperatures. In order to reduce its reactivity, the addition of UO 2 to UN has been suggested. In order to avoid carbon impurities, UN was synthesized frommore » elemental uranium using a hydride-dehydride-nitride thermal synthesis route prior to mixing with up to 10 wt% UO 2 in a planetary ball mill. UN and UN – UO 2 composite pellets were sintered in Ar – (0–1 at%) N 2 to study the effects of nitrogen concentration on the evolved phases and microstructure. UN and UN-UO 2 composite pellets were also sintered in Ar – 100 ppm N 2 to assess the effects of temperature (1700–2000 °C) on the final grain morphology and phase concentration.« less

Sequestration of radioactive iodine in silver-palladium phases in commercial spent nuclear fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Buck, Edgar C.; Mausolf, Edward J.; McNamara, Bruce K.

Radioactive iodine is the Achilles’ heel in the design for the safe geological disposal of spent UO2 nuclear fuel. Iodine’s high solubility and anticipated instant release during waste package compromise jeopardize performance assessment calculations. However, dissolution studies have indicated that the instant release fraction (IRF) of radioiodine (I) does not correlate with increasing fuel burn-up. In fact, there is a peak in the release iodine at around 50-60 Mwd/kgU and with increasing burn-up the instant release of iodine decreases. Detailed electron microscopy analysis of high burn-up fuel (~80 MWd/kgU) has revealed the presence of (Pd,Ag)(I,Br) nano-particles. As UO2 fuels aremore » irradiated, the Ag and Pd content increases, from 239Pu fission, enabling radioiodine to be retained. The occurrence of these phases in nuclear fuels may have significant implications for the long-term behavior of iodine.« less

Summary report on UO 2 thermal conductivity model refinement and assessment studies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiang-Yang; Cooper, Michael William Donald; Mcclellan, Kenneth James

Uranium dioxide (UO 2) is the most commonly used fuel in light water nuclear reactors and thermal conductivity controls the removal of heat produced by fission, therefore, governing fuel temperature during normal and accident conditions. The use of fuel performance codes by the industry to predict operational behavior is widespread. A primary source of uncertainty in these codes is thermal conductivity, and optimized fuel utilization may be possible if existing empirical models were replaced with models that incorporate explicit thermal conductivity degradation mechanisms during fuel burn-up. This approach is able to represent the degradation of thermal conductivity due to eachmore » individual defect type, rather than the overall burn-up measure typically used which is not an accurate representation of the chemical or microstructure state of the fuel that actually governs thermal conductivity and other properties. To generate a mechanistic thermal conductivity model, molecular dynamics (MD) simulations of UO 2 thermal conductivity including representative uranium and oxygen defects and fission products are carried out. These calculations employ a standard Buckingham type interatomic potential and a potential that combines the many-body embedded atom method potential with Morse-Buckingham pair potentials. Potential parameters for UO 2+x and ZrO 2 are developed for the latter potential. Physical insights from the resonant phonon-spin scattering mechanism due to spins on the magnetic uranium ions have been introduced into the treatment of the MD results, with the corresponding relaxation time derived from existing experimental data. High defect scattering is predicted for Xe atoms compared to that of La and Zr ions. Uranium defects reduce the thermal conductivity more than oxygen defects. For each defect and fission product, scattering parameters are derived for application in both a Callaway model and the corresponding high-temperature model typically used in fuel performance codes. The model is validated by comparison to low-temperature experimental measurements on single crystal hyper-stoichiometric UO 2+x samples and high-temperature literature data. Ongoing works include investigation of the effect of phase separation to UO 2+U 4O 9 on the low temperature thermal conductivity of UO 2+x, and modeling of thermal conductivity using the Green-Kubo method. Ultimately, this work will enable more accurate fuel performance simulations as well as extension to new fuel types and operating conditions, all of which improve the fuel economics of nuclear energy and maintain high fuel reliability and safety.« less

Characterization of Actinides Complexed to Nuclear Fuel Constituents Using ESI-MS

DOE PAGES

McDonald, Luther W.; Campbell, James A.; Vercouter, Thomas; ...

2016-03-01

Electrospray ionization-mass spectrometry (ESI-MS) was tested for its use in monitoring spent nuclear fuel (SNF) constituents including U, Pu, dibutyl phosphate (DBP), and tributyl phosphate (TBP). Both positive and negative ion modes were used to evaluate the speciation of U and Pu with TBP and DBP. Furthermore, apparent stability constants were determined for U complexed to TBP and DBP. In positive ion mode, TBP produced a strong signal with and without complexation to U or Pu, but, in negative ion mode, no TBP, U-TBP, or Pu-TBP complexes were observed. Apparent stability constants were determined for [UO 2(NO 3) 2(TBP) 2],more » [UO 2(NO 3) 2(H 2O)(TBP) 2], and [UO 2(NO 3) 2(TBP) 3]. In contrast DBP, U-DBP, and Pu-DBP complexes were observed in both positive and negative ion modes. Apparent stability constants were determined for the species [UO 2(DBP)], [UO 2(DBP) 3], and [UO 2(DBP) 4]. Analyzing mixtures of U or Pu with TBP and DBP yielded the formation of ternary complexes whose stoichiometry was directly related to the ratio of TBP to DBP. The ESI-MS protocols used in this study will further demonstrate the utility of ESI-MS and its applicability to process control monitoring in SNF reprocessing facilities.« less

Revisiting the diffusion mechanism of helium in UO2: A DFT+U study

NASA Astrophysics Data System (ADS)

Liu, X.-Y.; Andersson, D. A.

2018-01-01

The understanding of migration properties of helium atoms after their generation through α-decay of actinides in spent nuclear fuels is important for the safety of nuclear fuel storage and disposal. The diffusion of helium in UO2 is revisited by using the DFT+U simulation methodology employing the "U-ramping" method to address the issue of metastable energy states. A novel diffusion mechanism by helium interstitials, the "asymmetric hop" mechanism, is reported and compared to other diffusion mechanisms including an oxygen vacancy mediated mechanism and available experimental diffusion data. The new mechanism is shown to be the dominant one over a wide temperature range.

Experiments on the high-temperature behaviour of neutron-irradiated uranium dioxide and fission products, volume 8, number 1

NASA Astrophysics Data System (ADS)

Tanke, R. H. J.

The release rate of fission products from overheated UO2, the chemical form of these fission products, and the transport mechanism inside the nuclear fuel are determined. UO spheres of approximately 1 mm diameter, irradiated in a high-flux reactor were used for the experiments. The chemical forms of the particles released from the spheres during evaporation were determined by mass spectrometry and the release rate of the mission products was determined by gamma spectrometry. A gamma topographer was developed to determine the change with temperature in the three dimensional distribution of radioactive fission products in the spheres. No clear relationship between the stoichiometry of the spheres and uranium consumption were shown. A diffusion model was used to determine the activation energy for the diffusion of fission products. It is concluded that the microstructure of the nuclear fuel greatly affects the number of free oxygen atoms, the release rate and the chemical form of the fission products. The evaporation of the UO2 matrix is the main mechanism for the release of all fission products at temperatures above 2300 K. Barium can be as volatile as iodine. Niobium and lanthenum can be volatile. Molecular combinations of the fission products, iodine, cesium and tellurium, are highly unlikely to be present inside the fuel. Barium and nobium may form compounds with oxygen and are then released as simple oxides. Fission products are released from overheated UO2 or as oxides. A new model is proposed for describing the behavior of oxygen in irradiated nuclear fuel.

A Historical Review of Cermet Fuel Development and the Engine Performance Implications

NASA Technical Reports Server (NTRS)

Stewart, Mark E. M.

2015-01-01

This paper reviews test data for cermet fuel samples developed in the 1960's to better quantify Nuclear Thermal Propulsion (NTP) cermet engine performance, and to better understand contemporary fuel testing results. Over 200 cermet (W-UO2) samples were tested by thermally cycling to 2500 deg (2770 K) in hydrogen. The data indicates two issues at high temperatures: the vaporization rate of UO2 and the chemical stability of UO2. The data show that cladding and chemical stabilizers each result in large, order of magnitude improvements in high temperature performance, while other approaches yield smaller, incremental improvements. Data is very limited above 2770 K, and this complicates predictions of engine performance at high Isp. The paper considers how this material performance data translates into engine performance. In particular, the location of maximum temperature within the fuel element and the effect of heat deposition rate are examined.

Status of Fuel Development and Manufacturing for Space Nuclear Reactors at BWX Technologies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carmack, W.J.; Husser, D.L.; Mohr, T.C.

2004-02-04

New advanced nuclear space propulsion systems will soon seek a high temperature, stable fuel form. BWX Technologies Inc (BWXT) has a long history of fuel manufacturing. UO2, UCO, and UCx have been fabricated at BWXT for various US and international programs. Recent efforts at BWXT have focused on establishing the manufacturing techniques and analysis capabilities needed to provide a high quality, high power, compact nuclear reactor for use in space nuclear powered missions. To support the production of a space nuclear reactor, uranium nitride has recently been manufactured by BWXT. In addition, analytical chemistry and analysis techniques have been developedmore » to provide verification and qualification of the uranium nitride production process. The fabrication of a space nuclear reactor will require the ability to place an unclad fuel form into a clad structure for assembly into a reactor core configuration. To this end, BWX Technologies has reestablished its capability for machining, GTA welding, and EB welding of refractory metals. Specifically, BWX Technologies has demonstrated GTA welding of niobium flat plate and EB welding of niobium and Nb-1Zr tubing. In performing these demonstration activities, BWX Technologies has established the necessary infrastructure to manufacture UO2, UCx, or UNx fuel, components, and complete reactor assemblies in support of space nuclear programs.« less

XPS studies of UO 2 oxidation by alpha radiolysis of water at 100°C

NASA Astrophysics Data System (ADS)

Sunder, S.; Boyer, G. D.; Miller, N. H.

1990-12-01

The effect of alpha radiolysis of water on the oxidation and dissolution of UO 2 was studied at 100°C as a function of alpha-field strength and water chemistry using X-ray photoelectron spectroscopy. In N 2-purged solutions the oxidation of UO 2 increases with the strength of the alpha flux; an alpha flux greater than or equal to that from a 250-μ Ci americium-241 source leads to oxidation of UO 2 beyond the UO 2.33 (U 3O 7) stage, and an alpha flux equal to that from a 5-μ Ci source does not result in UO 2 oxidation beyond the UO 2.33 stage. The presence of dissolved H 2 in water, at a concentration ≥ 1.6 × 10 -4moldm-3, reduces the oxidation and dissolution of UO 2 due to alpha radiolysis at temperatures ≥ 100° C. It is concluded that the radiolysis of groundwater at ~ 100°C, due to the alpha flux associated with used CANDU fuel, is unlikely to make a significant contribution to its oxidative dissolution in the geological disposal vault planned in the Canadian Nuclear Fuel Waste Management Program. CANada Deuterium Uranium. Registered trademark.

Safety and Regulatory Issues of the Thorium Fuel Cycle

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ade, Brian; Worrall, Andrew; Powers, Jeffrey

2014-02-01

Thorium has been widely considered an alternative to uranium fuel because of its relatively large natural abundance and its ability to breed fissile fuel (233U) from natural thorium (232Th). Possible scenarios for using thorium in the nuclear fuel cycle include use in different nuclear reactor types (light water, high temperature gas cooled, fast spectrum sodium, molten salt, etc.), advanced accelerator-driven systems, or even fission-fusion hybrid systems. The most likely near-term application of thorium in the United States is in currently operating light water reactors (LWRs). This use is primarily based on concepts that mix thorium with uranium (UO2 + ThO2),more » add fertile thorium (ThO2) fuel pins to LWR fuel assemblies, or use mixed plutonium and thorium (PuO2 + ThO2) fuel assemblies. The addition of thorium to currently operating LWRs would result in a number of different phenomenological impacts on the nuclear fuel. Thorium and its irradiation products have nuclear characteristics that are different from those of uranium. In addition, ThO2, alone or mixed with UO2 fuel, leads to different chemical and physical properties of the fuel. These aspects are key to reactor safety-related issues. The primary objectives of this report are to summarize historical, current, and proposed uses of thorium in nuclear reactors; provide some important properties of thorium fuel; perform qualitative and quantitative evaluations of both in-reactor and out-of-reactor safety issues and requirements specific to a thorium-based fuel cycle for current LWR reactor designs; and identify key knowledge gaps and technical issues that need to be addressed for the licensing of thorium LWR fuel in the United States.« less

Low temperature synthesis and sintering of d-UO2 nanoparticles.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nenoff, Tina Maria; Ferreira, Summer Rhodes; Robinson, David B.

We report on the novel room temperature method of synthesizing advanced nuclear fuels; a method that virtually eliminates any volatility of components. This process uses radiolysis to form stable nanoparticle (NP) nuclear transuranic (TRU) fuel surrogates and in-situ heated stage TEM to sinter the NPs. The radiolysis is performed at Sandia's Gamma Irradiation Facility (GIF) 60Co source (3 x 10{sup 6} rad/hr). Using this method, sufficient quantities of fuels for research purposes can be produced for accelerated advanced nuclear fuel development. We are focused on both metallic and oxide alloy nanoparticles of varying compositions, in particular d-U, d-U/La alloys andmore » d-UO2 NPs. We present detailed descriptions of the synthesis procedures, the characterization of the NPs, the sintering of the NPs, and their stability with temperature. We have employed UV-vis, HRTEM, HAADF-STEM imaging, single particle EDX and EFTEM mapping characterization techniques to confirm the composition and alloying of these NPs.« less

Characterization Report on Fuels for NEAMS Model Validation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gofryk, Krzysztof

Nearly 20% of the world’s electricity today is generated by nuclear energy from uranium dioxide (UO 2) fuel. The thermal conductivity of UO 2 governs the conversion of heat produced from fission events into electricity and it is an important parameter in reactor design and safety. While nuclear fuel operates at high to very high temperatures, thermal conductivity and other materials properties lack sensitivity to temperature variations and to material variations at reactor temperatures. As a result, both the uncertainties in laboratory measurements at high temperatures and the small differences in properties of different materials inevitably lead to large uncertaintiesmore » in models and little predictive power. Conversely, properties measured at low to moderate temperatures have more sensitivity, less uncertainty, and have larger differences in properties for different materials. These variations need to be characterized as they will afford the highest predictive capability in modeling and offer best assurances for validation and verification at all temperatures. This is well emphasized in the temperature variation of the thermal conductivity of UO 2.« less

A U-bearing composite waste form for electrochemical processing wastes

NASA Astrophysics Data System (ADS)

Chen, X.; Ebert, W. L.; Indacochea, J. E.

2018-04-01

Metallic/ceramic composite waste forms are being developed to immobilize combined metallic and oxide waste streams generated during electrochemical recycling of used nuclear fuel. Composites were made for corrosion testing by reacting HT9 steel to represent fuel cladding, Zr and Mo to simulate metallic fuel waste, and a mixture of ZrO2, Nd2O3, and UO2 to represent oxide wastes. More than half of the added UO2 was reduced to metal and formed Fe-Zr-U intermetallics and most of the remaining UO2 and all of the Nd2O3 reacted to form zirconates. Fe-Cr-Mo intermetallics were also formed. Microstructure characterization of the intermetallic and ceramic phases that were generated and tests conducted to evaluate their corrosion behaviors indicate composite waste forms can accommodate both metallic and oxidized waste streams in durable host phases.

A U-bearing composite waste form for electrochemical processing wastes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, X.; Ebert, W. L.; Indacochea, J. E.

Metallic/ceramic composite waste forms are being developed to immobilize combined metallic and oxide waste streams generated during electrochemical recycling of used nuclear fuel. Composites were made for corrosion testing by reacting HT9 steel to represent fuel cladding, Zr and Mo to simulate metallic fuel waste, and a mixture of ZrO2, Nd2O3, and UO2 to represent oxide wastes. More than half of the added UO2 was reduced to metal and formed Fe-Zr-U intermetallics and most of the remaining UO2 and all of the Nd2O3 reacted to form zirconates. Fe-Cr-Mo intermetallics were also formed. Microstructure characterization of the intermetallic and ceramic phasesmore » that were generated and tests conducted to evaluate their corrosion behaviors indicate composite waste forms can accommodate both metallic and oxidized waste streams in durable host phases. (c) 2018 Elsevier B.V. All rights reserved.« less

UO{sub 2} and PuO{sub 2} utilization in high temperature engineering test reactor with helium coolant

DOE Office of Scientific and Technical Information (OSTI.GOV)

Waris, Abdul, E-mail: awaris@fi.itb.ac.id; Novitrian,; Pramuditya, Syeilendra

High temperature engineering test reactor (HTTR) is one of high temperature gas cooled reactor (HTGR) types which has been developed by Japanese Atomic Energy Research Institute (JAERI). The HTTR is a graphite moderator, helium gas coolant, 30 MW thermal output and 950 °C outlet coolant temperature for high temperature test operation. Original HTTR uses UO{sub 2} fuel. In this study, we have evaluated the use of UO{sub 2} and PuO{sub 2} in form of mixed oxide (MOX) fuel in HTTR. The reactor cell calculation was performed by using SRAC 2002 code, with nuclear data library was derived from JENDL3.2. Themore » result shows that HTTR can obtain its criticality condition if the enrichment of {sup 235}U in loaded fuel is 18.0% or above.« less

Revisiting the diffusion mechanism of helium in UO 2 : A DFT+ U study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, X. -Y.; Andersson, D. A.

The understanding of migration properties of helium atoms after their generation through α-decay of actinides in spent nuclear fuels is important for the safety of nuclear fuel storage and disposal. The diffusion of helium in UO 2 is revisited by using the DFT+U simulation methodology employing the “U-ramping” method to address the issue of metastable energy states. A novel diffusion mechanism by helium interstitials, the “asymmetric hop” mechanism, is reported and compared to other diffusion mechanisms including an oxygen vacancy mediated mechanism and available experimental diffusion data. We show that the new mechanism is the dominant one over a widemore » temperature range.« less

Revisiting the diffusion mechanism of helium in UO 2 : A DFT+ U study

DOE PAGES

Liu, X. -Y.; Andersson, D. A.

2017-11-03

The understanding of migration properties of helium atoms after their generation through α-decay of actinides in spent nuclear fuels is important for the safety of nuclear fuel storage and disposal. The diffusion of helium in UO 2 is revisited by using the DFT+U simulation methodology employing the “U-ramping” method to address the issue of metastable energy states. A novel diffusion mechanism by helium interstitials, the “asymmetric hop” mechanism, is reported and compared to other diffusion mechanisms including an oxygen vacancy mediated mechanism and available experimental diffusion data. We show that the new mechanism is the dominant one over a widemore » temperature range.« less

Gas emission from the UO2 samples, containing fission products and burnable absorber

NASA Astrophysics Data System (ADS)

Kopytin, V. P.; Baranov, V. G.; Burlakova, M. A.; Tenishev, A. V.; Kuzmin, R. S.; Pokrovskiy, S. A.; Mikhalchik, V. V.

2016-04-01

The process gas released from the fuel pellets of uranium fuel during fuel burn-up reduces the thermal conductivity of the rod-shell gap, enhances hydrogen embrittlement of the cladding material, causes it's carbonization, as well as transport processes in the fuel. In this study a technique of investigating the thermal desorption of gases from the UO2 fuel material were perfected in the temperature range 300-2000 K for uniform sample heating rate of 15 K/min in vacuum. The characteristic kinetic dependences are acquired for the gas emission from UO2 samples, containing simulators of fission products (SFP) and the burnable neutron absorber (BNA). Depending on the amount of SFP and BNA contained in the sample thermal desorption gas spectra (TDGS) vary. The composition of emitted gas varies, as well as the number of peaks in the TDGS and the peaks shift to higher temperatures. This indicates that introduction of SFPs and BNA alters the sample material structure and cause the creation of so- called traps which have different bonding energies to the gases. The traps can be a grid of dislocations, voids, and contained in the UO2 matrix SFP and BNA. Similar processes will occur in the fuel pellets in the real conditions of the Nuclear Power Plant as well.

Molecular dynamics simulation of thermal transport in UO 2 containing uranium, oxygen, and fission-product defects

DOE PAGES

Liu, Xiang -Yang; Cooper, Michael William D.; McClellan, Kenneth James; ...

2016-10-25

Uranium dioxide (UO 2) is the most commonly used fuel in light-water nuclear reactors and thermal conductivity controls the removal of heat produced by fission, thereby governing fuel temperature during normal and accident conditions. The use of fuel performance codes by the industry to predict operational behavior is widespread. A primary source of uncertainty in these codes is thermal conductivity, and optimized fuel utilization may be possible if existing empirical models are replaced with models that incorporate explicit thermal-conductivity-degradation mechanisms during fuel burn up. This approach is able to represent the degradation of thermal conductivity due to each individual defectmore » type, rather than the overall burn-up measure typically used, which is not an accurate representation of the chemical or microstructure state of the fuel that actually governs thermal conductivity and other properties. To generate a mechanistic thermal conductivity model, molecular dynamics (MD) simulations of UO 2 thermal conductivity including representative uranium and oxygen defects and fission products are carried out. These calculations employ a standard Buckingham-type interatomic potential and a potential that combines the many-body embedded-atom-method potential with Morse-Buckingham pair potentials. Potential parameters for UO 2+x and ZrO 2 are developed for the latter potential. Physical insights from the resonant phonon-spin-scattering mechanism due to spins on the magnetic uranium ions are introduced into the treatment of the MD results, with the corresponding relaxation time derived from existing experimental data. High defect scattering is predicted for Xe atoms compared to that of La and Zr ions. Uranium defects reduce the thermal conductivity more than oxygen defects. For each defect and fission product, scattering parameters are derived for application in both a Callaway model and the corresponding high-temperature model typically used in fuel-performance codes. The model is validated by comparison to low-temperature experimental measurements on single-crystal hyperstoichiometric UO 2+x samples and high-temperature literature data. Furthermore, this work will enable more accurate fuel-performance simulations and will extend to new fuel types and operating conditions, all of which improve the fuel economics of nuclear energy and maintain high fuel reliability and safety.« less

Molecular dynamics simulation of thermal transport in UO 2 containing uranium, oxygen, and fission-product defects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiang -Yang; Cooper, Michael William D.; McClellan, Kenneth James

Uranium dioxide (UO 2) is the most commonly used fuel in light-water nuclear reactors and thermal conductivity controls the removal of heat produced by fission, thereby governing fuel temperature during normal and accident conditions. The use of fuel performance codes by the industry to predict operational behavior is widespread. A primary source of uncertainty in these codes is thermal conductivity, and optimized fuel utilization may be possible if existing empirical models are replaced with models that incorporate explicit thermal-conductivity-degradation mechanisms during fuel burn up. This approach is able to represent the degradation of thermal conductivity due to each individual defectmore » type, rather than the overall burn-up measure typically used, which is not an accurate representation of the chemical or microstructure state of the fuel that actually governs thermal conductivity and other properties. To generate a mechanistic thermal conductivity model, molecular dynamics (MD) simulations of UO 2 thermal conductivity including representative uranium and oxygen defects and fission products are carried out. These calculations employ a standard Buckingham-type interatomic potential and a potential that combines the many-body embedded-atom-method potential with Morse-Buckingham pair potentials. Potential parameters for UO 2+x and ZrO 2 are developed for the latter potential. Physical insights from the resonant phonon-spin-scattering mechanism due to spins on the magnetic uranium ions are introduced into the treatment of the MD results, with the corresponding relaxation time derived from existing experimental data. High defect scattering is predicted for Xe atoms compared to that of La and Zr ions. Uranium defects reduce the thermal conductivity more than oxygen defects. For each defect and fission product, scattering parameters are derived for application in both a Callaway model and the corresponding high-temperature model typically used in fuel-performance codes. The model is validated by comparison to low-temperature experimental measurements on single-crystal hyperstoichiometric UO 2+x samples and high-temperature literature data. Furthermore, this work will enable more accurate fuel-performance simulations and will extend to new fuel types and operating conditions, all of which improve the fuel economics of nuclear energy and maintain high fuel reliability and safety.« less

Hot Hydrogen Testing of Tungsten-Uranium Dioxide (W-UO2) CERMET Fuel Materials for Nuclear Thermal Propulsion

NASA Technical Reports Server (NTRS)

Hickman, Robert; Broadway, Jeramie

2014-01-01

CERMET fuel materials are being developed at the NASA Marshall Space Flight Center for a Nuclear Cryogenic Propulsion Stage. Recent work has resulted in the development and demonstration of a Compact Fuel Element Environmental Test (CFEET) System that is capable of subjecting depleted uranium fuel material samples to hot hydrogen. A critical obstacle to the development of an NCPS engine is the high-cost and safety concerns associated with developmental testing in nuclear environments. The purpose of this testing capability is to enable low-cost screening of candidate materials, fabrication processes, and further validation of concepts. The CERMET samples consist of depleted uranium dioxide (UO2) fuel particles in a tungsten metal matrix, which has been demonstrated on previous programs to provide improved performance and retention of fission products1. Numerous past programs have utilized hot hydrogen furnace testing to develop and evaluate fuel materials. The testing provides a reasonable simulation of temperature and thermal stress effects in a flowing hydrogen environment. Though no information is gained about radiation damage, the furnace testing is extremely valuable for development and verification of fuel element materials and processes. The current work includes testing of subscale W-UO2 slugs to evaluate fuel loss and stability. The materials are then fabricated into samples with seven cooling channels to test a more representative section of a fuel element. Several iterations of testing are being performed to evaluate fuel mass loss impacts from density, microstructure, fuel particle size and shape, chemistry, claddings, particle coatings, and stabilizers. The fuel materials and forms being evaluated on this effort have all been demonstrated to control fuel migration and loss. The objective is to verify performance improvements of the various materials and process options prior to expensive full scale fabrication and testing. Post test analysis will include weight percent fuel loss, microscopy, dimensional tolerance, and fuel stability.

PREPARATION OF SPHERICAL URANIUM DIOXIDE PARTICLES

DOEpatents

Levey, R.P. Jr.; Smith, A.E.

1963-04-30

This patent relates to the preparation of high-density, spherical UO/sub 2/ particles 80 to 150 microns in diameter. Sinterable UO/sub 2/ powder is wetted with 3 to 5 weight per cent water and tumbled for at least 48 hours. The resulting spherical particles are then sintered. The sintered particles are useful in dispersion-type fuel elements for nuclear reactors. (AEC)

Microscopic Fuel Particles Produced by Self-Assembly of Actinide Nanoclusters on Carbon Nanomaterials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Na, Chongzheng

2016-10-17

Many consider further development of nuclear power to be essential for sustained development of society; however, the fuel forms currently used are expensive to recycle. In this project, we sought to create the knowledge and knowhow that are needed to produce nanocomposite materials by directly depositing uranium nanoclusters on networks of carbon-­ based nanomaterials. The objectives of the proposed work were to (1) determine the control of uranium nanocluster surface chemistry on nanocomposite formation, (2) determine the control of carbon nanomaterial surface chemistry on nanocomposite formation, and (3) develop protocols for synthesizing uranium-­carbon nanomaterials. After examining a wide variety ofmore » synthetic methods, we show that synthesizing graphene-­supported UO 2 nanocrystals in polar ethylene glycol compounds by polyol reduction under boiling reflux can enable the use of an inexpensive graphene precursor graphene oxide in the production of uranium-carbon nanocomposites in a one-­pot process. We further show that triethylene glycol is the most suitable solvent for producing nanometer-­sized UO 2 crystals compared to monoethylene glycol, diethylene glycol, and polyethylene glycol. Graphene-­supported UO 2 nanocrystals synthesized with triethylene glycol show evidence of heteroepitaxy, which can be beneficial for facilitating heat transfer in nuclear fuel particles. Furthermore, we show that graphene-supported UO 2 nanocrystals synthesized by polyol reduction can be readily stored in alcohols, preventing oxidation from the prevalent oxygen in air. Together, these methods provide a facile approach for preparing and storing graphene-supported UO nanocrystals for further investigation and development under ambient conditions.« less

A ``NEW'' Solid-Core Reactor Fuel Form that Maximizes the Performance of Nuclear Thermal and Electric Rockets

NASA Astrophysics Data System (ADS)

Rom, Frank E.; Finnegan, Patrick M.

1994-07-01

The ``NEW'' solid-core fuel form is the old Vapor Transport (VT) fuel pin investigated at NASA about 30 years ago. It is simply a tube sealed at both ends partially filled with UO2. During operation the UO2 forms an annular layer on the inside of the tube by vaporization and condensation. This form is an ideal structure for overall strength and retention of fission products. All of the structural material lies between the fuel (including fission products) and the reactor coolant. The isothermal inside fuel surface temperature that results from the vaporization and condensation of fuel during operation eliminates hotspots, significantly increasing the design fuel pin surface temperature. For NTP, W-UO2 fuel pins yield higher operating temperatures than for other fuel forms, because W has about a ten-fold lower vaporization rate compared to any other known material. The use of perigee propulsion using W-UO2 fuel pins can result in a more than ten-fold reduction in reactor power. Lower reactor power, together with zero fission product release potential, and the simplicity of fabrication of VT fuel pins should greatly simplify and reduce the cost of development of NTP. For NEP, VT fuel pins can increase fast neutron spectrum reactor life with no fission product release. Thermal spectrum NEP reactors using W184 or Mo VT fuel pins, with only small amounts of high neutron absorbing additives, offer benefits because of much lower fissionable fuel requirements. The VT fuel pin has application to commercial power reactors with similar benefits.

Experimental studies of Micro- and Nano-grained UO 2: Grain Growth Behavior, Sufrace Morphology, and Fracture Toughness

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miao, Yinbin; Mo, Kun; Jamison, Laura M.

This activity is supported by the US Nuclear Energy Advanced Modeling and Simulation (NEAMS) Fuels Product Line (FPL) and aims at providing experimental data for the validation of the mesoscale simulation code MARMOT. MARMOT is a mesoscale multiphysics code that predicts the coevolution of microstructure and properties within reactor fuel during its lifetime in the reactor. It is an important component of the Moose-Bison-Marmot (MBM) code suite that has been developed by Idaho National Laboratory (INL) to enable next generation fuel performance modeling capability as part of the NEAMS Program FPL. In order to ensure the accuracy of the microstructure-basedmore » materials models being developed within the MARMOT code, extensive validation efforts must be carried out. In this report, we summarize the experimental efforts in FY16 including the following important experiments: (1) in-situ grain growth measurement of nano-grained UO 2; (2) investigation of surface morphology in micrograined UO 2; (3) Nano-indentation experiments on nano- and micro-grained UO 2. The highlight of this year is: we have successfully demonstrated our capability to in-situ measure grain size development while maintaining the stoichiometry of nano-grained UO 2 materials; the experiment is, for the first time, using synchrotron X-ray diffraction to in-situ measure grain growth behavior of UO 2.« less

Thermal reactions of uranium metal, UO 2, U 3O 8, UF 4, and UO 2F 2 with NF 3 to produce UF 6

NASA Astrophysics Data System (ADS)

McNamara, Bruce; Scheele, Randall; Kozelisky, Anne; Edwards, Matthew

2009-11-01

This paper demonstrates that NF 3 fluorinates uranium metal, UO 2, UF 4, UO 3, U 3O 8, and UO 2F 2·2H 2O to produce the volatile UF 6 at temperatures between 100 and 550 °C. Thermogravimetric and differential thermal analysis reaction profiles are described that reflect changes in the uranium fluorination/oxidation state, physiochemical effects, and instances of discrete chemical speciation. Large differences in the onset temperatures for each system investigated implicate changes in mode of the NF 3 gas-solid surface interaction. These studies also demonstrate that NF 3 is a potential replacement fluorinating agent in the existing nuclear fuel cycle and in actinide volatility reprocessing.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaques, Brian J.; Watkins, Jennifer; Croteau, Joseph R.

In this study, the design and development of an economical, accident tolerant fuel (ATF) for use in the current light water reactor (LWR) fleet is highly desirable for the future of nuclear power. Uranium mononitride has been identified as an alternative fuel with higher uranium density and thermal conductivity when compared to the benchmark, UO 2, which could also provide significant economic benefits. However, UN by itself reacts with water at reactor operating temperatures. In order to reduce its reactivity, the addition of UO 2 to UN has been suggested. In order to avoid carbon impurities, UN was synthesized frommore » elemental uranium using a hydride-dehydride-nitride thermal synthesis route prior to mixing with up to 10 wt% UO 2 in a planetary ball mill. UN and UN – UO 2 composite pellets were sintered in Ar – (0–1 at%) N 2 to study the effects of nitrogen concentration on the evolved phases and microstructure. UN and UN-UO 2 composite pellets were also sintered in Ar – 100 ppm N 2 to assess the effects of temperature (1700–2000 °C) on the final grain morphology and phase concentration.« less

Modelling the radiolytic corrosion of α-doped UO2 and spent nuclear fuel

NASA Astrophysics Data System (ADS)

Liu, Nazhen; Qin, Zack; Noël, James J.; Shoesmith, David W.

2017-10-01

A model previously developed to predict the corrosion rate of spent fuel (UO2) inside a failed waste container has been adapted to simulate the rates measured on a wide range of α-doped UO2 and spent fuel specimens. This simulation confirms the validity of the model and demonstrates that the steady-state corrosion rate is controlled by the radiolytic production of H2O2 (which has been shown to be the primary oxidant driving fuel corrosion), irrespective of the reactivity of the UO2 matrix. The model was then used to determine the consequences of corrosion inside a failed container resealed by steel corrosion products. The possible accumulation of O2, produced by H2O2 decomposition, was found to accelerate the corrosion rate in a closed system. However, the simultaneous accumulation of radiolytic H2, which is activated as a reductant on the noble metal (ε) particles in the spent fuel, rapidly overcame this acceleration leading to the eventual suppression of the corrosion rate to insignificant values. Calculations also showed that, while the radiation dose rate, the H2O2 decomposition ratio, and the surface coverage of ε particles all influenced the short term corrosion rate, the influence of the radiolytically produced H2 was the overwhelming influence in reducing the rate to negligible level (i.e., <10-20 mol m-2 s-1).

Modelling oxygen self-diffusion in UO 2 under pressure

DOE PAGES

Cooper, Michael William D.; Grimes, R. W.; Fitzpatrick, M. E.; ...

2015-10-22

Access to values for oxygen self-diffusion over a range of temperatures and pressures in UO 2 is important to nuclear fuel applications. Here, elastic and expansivity data are used in the framework of a thermodynamic model, the cBΩ model, to derive the oxygen self-diffusion coefficient in UO 2 over a range of pressures (0–10 GPa) and temperatures (300–1900 K). Furthermore, the significant reduction in oxygen self-diffusion as a function of increasing hydrostatic pressure, and the associated increase in activation energy, is identified.

YUCCA Mountain Project - Argonne National Laboratory, Annual Progress Report, FY 1997 for activity WP 1221 unsaturated drip condition testing of spent fuel and unsaturated dissolution tests of glass.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bates, J. K.; Buck, E. C.; Emery, J. W.

1998-09-18

This document reports on the work done by the Nuclear Waste Management Section of the Chemical Technology Division of Argonne National Laboratory in the period of October 1996 through September 1997. Studies have been performed to evaluate the behavior of nuclear waste glass and spent fuel samples under the unsaturated conditions (low-volume water contact) that are likely to exist in the Yucca Mountain environment being considered as a potential site for a high-level waste repository. Tests with actinide-doped waste glasses, in progress for over 11 years, indicate that the transuranic element release is dominated by colloids that continuously form andmore » span from the glass surface. The nature of the colloids that form in the glass and spent fuel testing programs is being investigated by dynamic light scattering to determine the size distribution, by autoradiography to determine the chemistry, and by zeta potential to measure the electrical properties of the colloids. Tests with UO{sub 2} have been ongoing for 12 years. They show that the oxidation of UO{sub 2} occurs rapidly, and the resulting paragenetic sequence of secondary phases forming on the sample surface is similar to that observed for uranium found in natural oxidizing environments. The reaction of spent fuel samples in conditions similar to those used with UO{sub 2} have been in progress for over six years, and the results suggest that spent fuel forms many of the same alteration products as UO{sub 2}. With spent fuel, the bulk of the reaction occurs via a through-grain reaction process, although grain boundary attack is sufficient to have reacted all of the grain boundary regions in the samples. New test methods are under development to evaluate the behavior of spent fuel samples with intact cladding: the rate at which alteration and radionuclide release occurs when water penetrates fuel sections and whether the reaction causes the cladding to split. Alteration phases have been formed on fine grains of UO{sub 2} in contact with small volumes of water within a several month period when the radiolysis product H{sub 2}O{sub 2} is added to the groundwater solution. The test setup has been mocked up for operation with spent fuel in the hot-cell.« less

The UO2 ex-ADU powder preparation and pellet sintering for optimum efficiency: experimental and modeling studies

NASA Astrophysics Data System (ADS)

Hung, Nguyen Trong; Thuan, Le Ba; Van Tung, Nguyen; Thuy, Nguyen Thanh; Lee, Jin-Young; Jyothi, Rajesh Kumar

2017-12-01

The UO2 nuclear fuel pellet process for light water reactors (LWR) includes the conversion of uranium hexafluoride (UF6) into UO2 powder and the fabrication of UO2 pellets from such UO2 powder. In the paper, studies on UO2 pellet process from ammonium diuranate-derived uranium dioxide powder (UO2 ex-ADU powder) were reported. The UO2 ex-ADU powders were converted from ADU at various temperatures of 973 K, 1023 K and 1073 K and then UO2 pellets prepared from the powders were sintered at temperatures of 1923 K, 1973 K and 2023 K for times of 4 h, 6 h and 8 h. Response surface methodology (RSM) based on quadratic central composite design (CCD) type of face centered (CCF) improved by Box and Hunter was used to model the UO2 pellet process, using MODDE 5.0 software as an assessing tool. On the base of the proposed model, the relationship between the technological parameters and density of the UO2 pellet product was suggested to control the UO2 ex-ADU pellet process as desired levels.

Molten uranium dioxide structure and dynamics

DOE PAGES

Skinner, L. B.; Parise, J. B.; Benmore, C. J.; ...

2014-11-21

Uranium dioxide (UO 2) is the major nuclear fuel component of fission power reactors. A key concern during severe accidents is the melting and leakage of radioactive UO 2 as it corrodes through its zirconium cladding and steel containment. Yet, the very high temperatures (>3140 kelvin) and chemical reactivity of molten UO 2 have prevented structural studies. In this work, we combine laser heating, sample levitation, and synchrotron x-rays to obtain pair distribution function measurements of hot solid and molten UO 2. The hot solid shows a substantial increase in oxygen disorder around the lambda transition (2670 K) but negligiblemore » U-O coordination change. On melting, the average U-O coordination drops from 8 to 6.7 ± 0.5. Molecular dynamics models refined to this structure predict higher U-U mobility than 8-coordinated melts.« less

Comparative Studies on UO2 Fueled HTTR Several Nuclear Data Libraries

NASA Astrophysics Data System (ADS)

Hidayati, Anni N.; Prastyo, Puguh A.; Waris, Abdul; Irwanto, Dwi

2017-07-01

HTTR (High Temperature Engineering Test Reactor) is one of Generation IV nuclear reactors that has been developed by JAERI (former name of JAEA, JAPAN). HTTR uses graphite moderator, helium gas coolant with UO2 fuel and outlet coolant temperature of 900°C or higher than that. Several studies regarding HTTR have been performed by employing JENDL 3.2 nuclear data libraries. In this paper, comparative evaluation of HTTR with several nuclear data libraries (JENDL 3.3, JENDL 4.0, and JEF 3.1) have been conducted.. The 3-D calculation was performed by using CITATION module of SRAC 2006 code. The result shows some differences between those nuclear data libraries result. K-eff or core effective multiplication factor results are about 1.17, 1,18 and 1,19 (JENDL 3.3, JENDL 4.0, and JEF 3.1) at Begin of Life, also at the End of Life (after two years operation) are 1.16, 1.17 and 1.17 for each nuclear data libraries. There are some different result of K-eff but for neutron spectra results, those nuclear data libraries show the same result.

Galvanic cell for processing of used nuclear fuel

DOEpatents

Garcia-Diaz, Brenda L.; Martinez-Rodriguez, Michael J.; Gray, Joshua R.; Olson, Luke C.

2017-02-07

A galvanic cell and methods of using the galvanic cell is described for the recovery of uranium from used nuclear fuel according to an electrofluorination process. The galvanic cell requires no input energy and can utilize relatively benign gaseous fluorinating agents. Uranium can be recovered from used nuclear fuel in the form of gaseous uranium compound such as uranium hexafluoride, which can then be converted to metallic uranium or UO.sub.2 and processed according to known methodology to form a useful product, e.g., fuel pellets for use in a commercial energy production system.

Electrochemical fluorination for processing of used nuclear fuel

DOEpatents

Garcia-Diaz, Brenda L.; Martinez-Rodriguez, Michael J.; Gray, Joshua R.; Olson, Luke C.

2016-07-05

A galvanic cell and methods of using the galvanic cell is described for the recovery of uranium from used nuclear fuel according to an electrofluorination process. The galvanic cell requires no input energy and can utilize relatively benign gaseous fluorinating agents. Uranium can be recovered from used nuclear fuel in the form of gaseous uranium compound such as uranium hexafluoride, which can then be converted to metallic uranium or UO.sub.2 and processed according to known methodology to form a useful product, e.g., fuel pellets for use in a commercial energy production system.

Molecular Dynamics Simulation of Fission Fragment Damage in Nuclear Fuel and Surrogate Material

DOE Office of Scientific and Technical Information (OSTI.GOV)

Devanathan, Ram

ABSTRACT We have performed classical molecular dynamics simulations of swift heavy ion damage, typical of fission fragments, in nuclear fuel (UO 2) for energy deposition per unit length of 3.9 keV/nm. We did not observe amorphization. The damage mainly consisted of isolated point defects. Only about 1% of the displacements occur on the uranium sublattice. Oxygen Frenkel pairs are an order of magnitude more numerous than uranium Frenkel pairs in the primary damage state. In contrast, previous results show that the ratio of Frenkel pairs on the two sublattices is close to the stoichiometric ratio in ceria. These differences inmore » the primary damage state may lead to differences in radiation response of UO 2and CeO 2.« less

Phase discrimination of uranium oxides using laser-induced breakdown spectroscopy

NASA Astrophysics Data System (ADS)

Campbell, Keri R.; Wozniak, Nicholas R.; Colgan, James P.; Judge, Elizabeth J.; Barefield, James E.; Kilcrease, David P.; Wilkerson, Marianne P.; Czerwinski, Ken R.; Clegg, Samuel M.

2017-08-01

Nuclear forensics goals for characterizing samples of interest include qualitative and quantitative analysis of major and trace elements, isotopic analysis, phase identification, and physical analysis. These samples may include uranium oxides UO2, U3O8, and UO3, which play an important role in the front end of the nuclear fuel cycle, from mining to fuel fabrication. The focus of this study is to compare the ratios of the intensities of uranium and oxygen emission lines which can be used to distinguish between different uranium oxide materials using Laser-Induced Breakdown Spectroscopy (LIBS). Measurements at varying laser powers were made under an argon atmosphere at 585 Torr to ensure the oxygen emission intensity was originating from the sample, and not from the atmosphere. Fifteen uranium emission lines were used to compare experimental results with theoretical calculations in order to determine the plasma conditions. Using a laser energy of 26 mJ, the uranium lines 591.539 and 682.692 nm provide the highest degree of discrimination between the uranium oxides. The study presented here suggests that LIBS is useful for discriminating uranium oxide phases, UO2, U3O8, and UO3.

Fuel Fabrication and Nuclear Reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Karpius, Peter Joseph

2017-02-02

The uranium from the enrichment plant is still in the form of UF 6. UF 6 is not suitable for use in a reactor due to its highly corrosive chemistry as well as its phase diagram. UF 6 is converted into UO 2 fuel pellets, which are in turn placed in fuel rods and assemblies. Reactor designs are variable in moderators, coolants, fuel, performance etc.The dream of energy ‘too-cheap to meter’ is no more, and now the nuclear power industry is pushing ahead with advanced reactor designs.

Screening of advanced cladding materials and UN-U3Si5 fuel

NASA Astrophysics Data System (ADS)

Brown, Nicholas R.; Todosow, Michael; Cuadra, Arantxa

2015-07-01

In the aftermath of Fukushima, a focus of the DOE-NE Advanced Fuels Campaign has been the development of advanced nuclear fuel and cladding options with the potential for improved performance in an accident. Uranium dioxide (UO2) fuels with various advanced cladding materials were analyzed to provide a reference for cladding performance impacts. For advanced cladding options with UO2 fuel, most of the cladding materials have some reactivity and discharge burn-up penalty (in GWd/t). Silicon carbide is one exception in that the reactor physics performance is predicted to be very similar to zirconium alloy cladding. Most candidate claddings performed similar to UO2-Zr fuel-cladding in terms of safety coefficients. The clear exception is that Mo-based materials were identified as potentially challenging from a reactor physics perspective due to high resonance absorption. This paper also includes evaluation of UN-U3Si5 fuels with Kanthal AF or APMT cladding. The objective of the U3Si5 phase in the UN-U3Si5 fuel concept is to shield the nitride phase from water. It was shown that UN-U3Si5 fuels with Kanthal AF or APMT cladding have similar reactor physics and fuel management performance over a wide parameter space of phase fractions when compared to UO2-Zr fuel-cladding. There will be a marginal penalty in discharge burn-up (in GWd/t) and the sensitivity to 14N content in UN ceramic composites is high. Analysis of the rim effect due to self-shielding in the fuel shows that the UN-based ceramic fuels are not expected to have significantly different relative burn-up distributions at discharge relative to the UO2 reference fuel. However, the overall harder spectrum in the UN ceramic composite fuels increases transuranic build-up, which will increase long-term activity in a once-thru fuel cycle but is expected to be a significant advantage in a fuel cycle with continuous recycling of transuranic material. It is recognized that the fuel and cladding properties assumed in these assessments are preliminary, and that additional data are necessary for these materials, most significantly under irradiation.

Thermal transport in UO 2 with defects and fission products by molecular dynamics simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiang-Yang; Cooper, Michael William Donald; Mcclellan, Kenneth James

2015-10-14

The importance of the thermal transport in nuclear fuel has motivated a wide range of experimental and modelling studies. In this report, the reduction of thermal transport in UO 2 due to defects and fission products has been investigated using non-equilibrium MD simulations, with two sets of empirical potentials for studying the degregation of UO 2 thermal conductivity including a Buckingham type interatomic potential and a recently developed EAM type interatomic potential. Additional parameters for U 5+ and Zr 4+ in UO 2 have been developed for the EAM potential. The thermal conductivity results from MD simulations are then correctedmore » for the spin-phonon scattering through Callaway model formulations. To validate the modelling results, comparison was made with experimental measurements on single crystal hyper-stoichiometric UO 2+x samples.« less

Uncertainties for Swiss LWR spent nuclear fuels due to nuclear data

NASA Astrophysics Data System (ADS)

Rochman, Dimitri A.; Vasiliev, Alexander; Dokhane, Abdelhamid; Ferroukhi, Hakim

2018-05-01

This paper presents a study of the impact of the nuclear data (cross sections, neutron emission and spectra) on different quantities for spent nuclear fuels (SNF) from Swiss power plants: activities, decay heat, neutron and gamma sources and isotopic vectors. Realistic irradiation histories are considered using validated core follow-up models based on CASMO and SIMULATE. Two Pressurized and one Boiling Water Reactors (PWR and BWR) are considered over a large number of operated cycles. All the assemblies at the end of the cycles are studied, being reloaded or finally discharged, allowing spanning over a large range of exposure (from 4 to 60 MWd/kgU for ≃9200 assembly-cycles). Both UO2 and MOX fuels were used during the reactor cycles, with enrichments from 1.9 to 4.7% for the UO2 and 2.2 to 5.8% Pu for the MOX. The SNF characteristics presented in this paper are calculated with the SNF code. The calculated uncertainties, based on the ENDF/B-VII.1 library are obtained using a simple Monte Carlo sampling method. It is demonstrated that the impact of nuclear data is relatively important (e.g. up to 17% for the decay heat), showing the necessity to consider them for safety analysis of the SNF handling and disposal.

Atomistic modeling of the solid-state chemistry of actinide materials

NASA Astrophysics Data System (ADS)

Shuller, Lindsay C.

Materials that incorporate actinides are critical to the nuclear fuel cycle, either as nuclear fuels or nuclear waste forms. In this thesis, I examine four materials: i) ThO2-UO2 solid solutions, ii) binary ThO2-CeO2-ZrO2 solid solutions, iii) Np-doped studtite, iv) Np-doped boltwoodite. Computational methods, particularly density functional theory (DFT) calculations and Monte-Carlo (MC) simulations, are used to determine the energetics and structures of these actinide-bearing materials. The solid-solution behavior of nuclear fuels and nuclear waste forms indicate the thermodynamic stability of the material, which is important for understanding the in-reactor fuel properties and long-term stability of used fuel. The ThxU1-xO2 and ThxCe 1-xO2 binaries are almost completely miscible; however, DeltaGmix reveals a small tendency for the systems to exsolve (e.g., DeltaEexsoln(Th xU1-xO2) = 0.13 kJ/(mol cations) at 750 K). Kinetic hindrances (e.g., interfacial energy) may inhibit exsolution, especially at the low temperatures necessary to stabilize the nanoscale exsolution lamellae observed in the ThxU1-xO2 and Ce xZr1-xO2 binaries. Miscibility in the Zr-bearing binaries is limited. At 1400 °C, only 3.6 and 0.09 mol% ZrO2 is miscible in CeO2 and ThO2, respectively. The incorporation of minor amounts of Np5+,6+ into uranium alteration phases, e.g., studtite [UO2O2 (H2O)4] or boltwoodite [K(UO2)(SiO 3OH)(H2O)1.5] , may limit the mobility of aqueous neptunyl complexes released from oxidized nuclear fuels. Np6+-incorporation into studtite requires less energy than Np5+-incorporation (e.g., with source/sink = Np2O5/UO 3 DeltaEincorp(Np6+) = 0.42 eV and DeltaEincorp(Np5+) = 1.12 eV). In addition, Np6+ is completely miscible in studtite at room temperature with respect to a hypothetical Np6+-studtite. Electronic structure calculations provide insight into Np-bonding in studtite. The Np 5f orbitals are within the band gap of studtite, resulting in the narrowing of the band gap from 2.29 eV for studtite to 1.09 eV for Np-incorporated studtite. Three charge-balancing mechanisms for the substitution of Np5+ for U6+ were compared: i) addition of H+ [DeltaEincorp(bolt) = 0.79 eV; DeltaEincorp(stud) = 1.12 eV], ii) interlayer coupled substitution [DeltaEincorp (bolt) = 1.40 eV], iii) intra-layer coupled-substitution [DeltaEincorp(bolt) = 0.86 eV]. Solid-solution calculations of the intra-layer coupled-substitution mechanism, where Np 5+ and P5+ substitute for U6+ and Si 4+, predict an incorporation limit of 585 ppm at 300 °C.

Coupled thermochemical, isotopic evolution and heat transfer simulations in highly irradiated UO2 nuclear fuel

NASA Astrophysics Data System (ADS)

Piro, M. H. A.; Banfield, J.; Clarno, K. T.; Simunovic, S.; Besmann, T. M.; Lewis, B. J.; Thompson, W. T.

2013-10-01

Predictive capabilities for simulating irradiated nuclear fuel behavior are enhanced in the current work by coupling thermochemistry, isotopic evolution and heat transfer. Thermodynamic models that are incorporated into this framework not only predict the departure from stoichiometry of UO2, but also consider dissolved fission and activation products in the fluorite oxide phase, noble metal inclusions, secondary oxides including uranates, zirconates, molybdates and the gas phase. Thermochemical computations utilize the spatial and temporal evolution of the fission and activation product inventory in the pellet, which is typically neglected in nuclear fuel performance simulations. Isotopic computations encompass the depletion, decay and transmutation of more than 2000 isotopes that are calculated at every point in space and time. These computations take into consideration neutron flux depression and the increased production of fissile plutonium near the fuel pellet periphery (i.e., the so-called “rim effect”). Thermochemical and isotopic predictions are in very good agreement with reported experimental measurements of highly irradiated UO2 fuel with an average burnup of 102 GW d t(U)-1. Simulation results demonstrate that predictions are considerably enhanced when coupling thermochemical and isotopic computations in comparison to empirical correlations. Notice: This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes.

Microstructure and mechanical properties of eutectic B2O3-UO2 ceramic composites solidified at different cooling rates

NASA Astrophysics Data System (ADS)

Yusufu, Aikebaier; Uno, Masayoshi

2018-02-01

The removal of nuclear debris from damaged reactors by drilling or cutting requires an understanding of various properties of the solidified debris, such as mechanical properties (hardness, fractural features, strength, etc.) and microstructural properties like porosity, which have a significant impact on the mechanical properties. In this study, B2O3-UO2 composites were prepared by the eutectic reaction as solidified samples of mock fuel debris with a wide variety of porosities, and the porosity dependence of the mechanical properties under compression were characterized to obtain fundamental data on the complicated fuel debris. The porous eutectic B2O3-UO2 (B2O3/UO2 atomic ratio = 0.225:0.775) samples were successfully prepared by solidification of the molten phase below 2073 K, and the porosity increased as the pore network developed as the cooling rate was decreased. The nano- and microhardness as well as Young's moduli of the eutectic B2O3-UO2 samples were higher than those of UO2. However, the compressive strengths of the eutectic B2O3-UO2 samples were lower than that of UO2, and they decreased as the porosity increased. All samples showed typical brittle fracturing behavior. The low-porosity samples showed a linear elastic step up to a sudden rupture, whereas the high-porosity samples exhibited two main regimes: a linear elastic region that can be attributed to pore-edge bending or face stretching; a zigzag step that is related to the progression of pore collapse.

Thermodynamic and kinetic aspects of UO 2 fuel oxidation in air at 400-2000 K

NASA Astrophysics Data System (ADS)

Taylor, Peter

2005-09-01

Most nuclear fuel oxidation research has addressed either low-temperature (<700 K) air oxidation related to fuel storage or high-temperature (>1500 K) steam oxidation linked to reactor safety. This paper attempts to unify modelling for air oxidation of UO 2 fuel over a wide range of temperature, and thus to assist future improvement of the ASTEC code, co-developed by IRSN and GRS. Phenomenological correlations for different temperature ranges distinguish between oxidation on the scale of individual grains to U 3O 7 and U 3O 8 below ˜700 K and individual fragments to U 3O 8 via UO 2+ x and/or U 4O 9 above ˜1200 K. Between about 700 and 1200 K, empirical oxidation rates slowly decline as the U 3O 8 product becomes coarser-grained and more coherent, and fragment-scale processes become important. A more mechanistic approach to high-temperature oxidation addresses questions of oxygen supply, surface reaction kinetics, thermodynamic properties, and solid-state oxygen diffusion. Experimental data are scarce, however, especially at low oxygen partial pressures and high temperatures.

Radiation induced dissolution of UO 2 based nuclear fuel - A critical review of predictive modelling approaches

NASA Astrophysics Data System (ADS)

Eriksen, Trygve E.; Shoesmith, David W.; Jonsson, Mats

2012-01-01

Radiation induced dissolution of uranium dioxide (UO 2) nuclear fuel and the consequent release of radionuclides to intruding groundwater are key-processes in the safety analysis of future deep geological repositories for spent nuclear fuel. For several decades, these processes have been studied experimentally using both spent fuel and various types of simulated spent fuels. The latter have been employed since it is difficult to draw mechanistic conclusions from real spent nuclear fuel experiments. Several predictive modelling approaches have been developed over the last two decades. These models are largely based on experimental observations. In this work we have performed a critical review of the modelling approaches developed based on the large body of chemical and electrochemical experimental data. The main conclusions are: (1) the use of measured interfacial rate constants give results in generally good agreement with experimental results compared to simulations where homogeneous rate constants are used; (2) the use of spatial dose rate distributions is particularly important when simulating the behaviour over short time periods; and (3) the steady-state approach (the rate of oxidant consumption is equal to the rate of oxidant production) provides a simple but fairly accurate alternative, but errors in the reaction mechanism and in the kinetic parameters used may not be revealed by simple benchmarking. It is essential to use experimentally determined rate constants and verified reaction mechanisms, irrespective of whether the approach is chemical or electrochemical.

The thermal conductivity of mixed fuel U xPu 1-xO 2: molecular dynamics simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiang-Yang; Cooper, Michael William Donald; Stanek, Christopher Richard

2015-10-16

Mixed oxides (MOX), in the context of nuclear fuels, are a mixture of the oxides of heavy actinide elements such as uranium, plutonium and thorium. The interest in the UO 2-PuO 2 system arises from the fact that these oxides are used both in fast breeder reactors (FBRs) as well as in pressurized water reactors (PWRs). The thermal conductivity of UO 2 fuel is an important material property that affects fuel performance since it is the key parameter determining the temperature distribution in the fuel, thus governing, e.g., dimensional changes due to thermal expansion, fission gas release rates, etc. Formore » this reason it is important to understand the thermal conductivity of MOX fuel and how it differs from UO 2. Here, molecular dynamics (MD) simulations are carried out to determine quantitatively, the effect of mixing on the thermal conductivity of U xPu 1-xO 2, as a function of PuO 2 concentrations, for a range of temperatures, 300 – 1500 K. The results will be used to develop enhanced continuum thermal conductivity models for MARMOT and BISON by INL. These models express the thermal conductivity as a function of microstructure state-variables, thus enabling thermal conductivity models with closer connection to the physical state of the fuel.« less

Sensitivity Analysis of Fuel Centerline Temperatures in SuperCritical Water-cooled Reactors (SCWRs)

NASA Astrophysics Data System (ADS)

Abdalla, Ayman

SuperCritical Water-cooled Reactors (SCWRs) are one of the six nuclear-reactor concepts currently being developed under the Generation-IV International Forum (GIF). A main advantage of SCW Nuclear Power Plants (NPPs) is that they offer higher thermal efficiencies compared to those of current conventional NPPs. Unlike today's conventional NPPs, which have thermal efficiencies between 30 - 35%, SCW NPPs will have thermal efficiencies within a range of 45 - 50%, owing to high operating temperatures and pressures (i.e., coolant temperatures as high as 625°C at 25 MPa pressure). The use of current fuel bundles with UO2 fuel at the high operating parameters of SCWRs may cause high fuel centerline temperatures, which could lead to fuel failure and fission gas release. Studies have shown that when the Variant-20 (43-element) fuel bundle was examined at SCW conditions, the fuel centerline temperature industry limit of 1850°C for UO2 and the sheath temperature design limit of 850°C might be exceeded. Therefore, new fuel-bundle designs, which comply with the design requirements, are required for future use in SCWRs. The main objective of this study to conduct a sensitivity analysis in order to identify the main factors that leads to fuel centerline temperature reduction. Therefore, a 54-element fuel bundle with smaller diameter of fuel elements compared to that of the 43-element bundle was designed and various nuclear fuels are examined for future use in a generic Pressure Tube (PT) SCWR. The 54-element bundle consists of 53 heated fuel elements with an outer diameter of 9.5 mm and one central unheated element of 20-mm outer diameter which contains burnable poison. The 54-element fuel bundle has an outer diameter of 103.45 mm, which is the same as the outer diameter of the 43-element fuel bundle. After developing the 54-element fuel bundle, one-dimensional heat-transfer analysis was conducted using MATLAB and NIST REFPROP programs. As a result, the Heat Transfer Coefficient (HTC), bulk-fluid, sheath and fuel centerline temperature profiles were generated along the heated length of 5.772 m for a generic fuel channel. The fuel centerline and sheath temperature profiles have been determined at four Axial Heat Flux Profiles (AHFPs) using an average thermal power per channel of 8.5 MWth. The four examined AHFPs are the uniform, cosine, upstream-skewed and downstream-skewed profiles. Additionally, this study focuses on investigating a possibility of using low, enhanced and high thermal-conductivity fuels. The low thermal-conductivity fuels, which have been examined in this study, are uranium dioxide (UO 2), Mixed Oxide (MOX) and Thoria (ThO2) fuels. The examined enhanced thermal-conductivity fuels are uranium dioxide - silicon carbide (UO2 - SiC) and uranium dioxide - beryllium oxide (UO2 - BeO). Lastly, uranium carbide (UC), uranium dicarbide (UC2) and uranium nitride (UN) are the selected high thermal-conductivity fuels, which have been proposed for use in SCWRs. A comparison has been made between the low, enhanced and high thermal-conductivity fuels in order to identify the fuel centerline temperature behaviour when different nuclear fuels are used. Also, in the process of conducting the sensitivity analysis, the HTC was calculated using the Mokry et al. correlation, which is the most accurate supercritical water heat-transfer correlation so far. The sheath and the fuel centerline temperature profiles were determined for two cases. In Case 1, the HTC was calculated based on the Mokry et al. correlation, while in Case 2, the HTC values calculated for Case 1 were multiplied by a factor of 2. This factor was used in order to identify the amount of decrease in temperatures if the heat transfer is enhanced with appendages. Results of this analysis indicate that the use of the newly developed 54-element fuel bundle along with the proposed fuels is promising when compared with the Variant-20 (43-element) fuel bundle. Overall, the fuel centerline and sheath temperatures were below the industry and design limits when most of the proposed fuels were examined in the 54-element fuel bundle, however, the fuel centerline temperature limit was exceeded while MOX fuel was examined. Keywords: SCWRs, Fuel Centerline Temperature, Sheath Temperature, High Thermal Conductivity Fuels, Low Thermal Conductivity Fuels, HTC.

Fission products and nuclear fuel behaviour under severe accident conditions part 2: Fuel behaviour in the VERDON-1 sample

NASA Astrophysics Data System (ADS)

Geiger, E.; Le Gall, C.; Gallais-During, A.; Pontillon, Y.; Lamontagne, J.; Hanus, E.; Ducros, G.

2017-11-01

Within the framework of the International Source Term Programme (ISTP), the VERDON programme aims at quantifying the source term of radioactive materials in case of a hypothetical severe accident in a light water reactor (LWR). Tests were performed in a new experimental laboratory (VERDON) built in the LECA-STAR facility (CEA Cadarache). The VERDON-1 test was devoted to the study of a high burn-up UO2 fuel and FP releases at very high temperature (≈2873 K) in a reducing atmosphere. Post-test qualitative and quantitative characterisations of the VERDON-1 sample led to the proposal of a scenario explaining the phenomena occurring during the experimental sequence. Hence, the fuel and the cladding may have interacted which led to the melting of UO2-ZrO2 alloy. Although no relocation was observed during the test, it may have been imminent.

Development of UO2/PuO2 dispersed in uranium matrix CERMET fuel system for fast reactors

NASA Astrophysics Data System (ADS)

Sinha, V. P.; Hegde, P. V.; Prasad, G. J.; Pal, S.; Mishra, G. P.

2012-08-01

CERMET fuel with either PuO2 or enriched UO2 dispersed in uranium metal matrix has a strong potential of becoming a fuel for the liquid metal cooled fast breeder reactors (LMR's). In fact it may act as a bridge between the advantages and disadvantages associated with the two extremes of fuel systems (i.e. ceramic fuel and metallic fuel) for fast reactors. At Bhabha Atomic Research Centre (BARC), R & D efforts are on to develop this CERMET fuel by powder metallurgy route. This paper describes the development of flow sheet for preparation of UO2 dispersed in uranium metal matrix pellets for three different compositions i.e. U-20 wt%UO2, U-25 wt%UO2 and U-30 wt%UO2. It was found that the sintered pellets were having excellent integrity and their linear mass was higher than that of carbide fuel pellets used in Fast Breeder Test Reactor programme (FBTR) in India. The pellets were characterized by X-ray diffraction (XRD) technique for phase analysis and lattice parameter determination. The optical microstructures were developed and reported for all the three different U-UO2 compositions.

Development of Innovative Accident Tolerant High Thermal Conductivity UO 2-Diamond Composite Fuel Pellets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tulenko, James; Subhash, Ghatu

2016-01-01

The University of Florida (UF) evaluated a composite fuel consisting of UO 2 powder mixed with diamond micro particles as a candidate as an accident-tolerant fuel (ATF). The research group had previous extensive experience researching with diamond micro particles as an addition to reactor coolant for improved plant thermal performance. The purpose of this research work was to utilize diamond micro particles to develop UO 2-Diamond composite fuel pellets with significantly enhanced thermal properties, beyond that already being measured in the previous UF research projects of UO 2 – SiC and UO 2 – Carbon Nanotube fuel pins. UF ismore » proving with the current research results that the addition of diamond micro particles to UO 2 may greatly enhanced the thermal conductivity of the UO 2 pellets producing an accident-tolerant fuel. The Beginning of life benefits have been proven and fuel samples are being irradiated in the ATR reactor to confirm that the thermal conductivity improvements are still present under irradiation.« less

High Frequency Acoustic Microscopy for the Determination of Porosity and Young's Modulus in High Burnup Uranium Dioxide Nuclear Fuel

NASA Astrophysics Data System (ADS)

Marchetti, Mara; Laux, Didier; Cappia, Fabiola; Laurie, M.; Van Uffelen, P.; Rondinella, V. V.; Wiss, T.; Despaux, G.

2016-06-01

During irradiation UO2 nuclear fuel experiences the development of a non-uniform distribution of porosity which contributes to establish varying mechanical properties along the radius of the pellet. Radial variations of both porosity and elastic properties in high burnup UO2 pellet can be investigated via high frequency acoustic microscopy. For this purpose ultrasound waves are generated by a piezoelectric transducer and focused on the sample, after having travelled through a coupling liquid. The elastic properties of the material are related to the velocity of the generated Rayleigh surface wave (VR). A UO2 pellet with a burnup of 67 GWd/tU was characterized using the acoustic microscope installed in the hot cells of the JRC-ITU at a 90 MHz frequency, with methanol as coupling liquid. VR was measured at different radial positions. A good agreement was found, when comparing the porosity values obtained via acoustic microscopy with those determined using SEM image analysis, especially in the areas close to the centre. In addition, Young's modulus was calculated and its radial profile was correlated to the corresponding burnup profile and to the hardness radial profile data obtained by Vickers micro-indentation.

A thermal conductivity model for U-­Si compounds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Yongfeng; Andersson, Anders David Ragnar

U 3Si 2 is a candidate for accident tolerant nuclear fuel being developed as an alternative to UO 2 in commercial light water reactors (LWRs). One of its main benefits compared to UO 2 is higher thermal conductivity that increases with temperature. This increase is contrary to UO 2, for which the thermal conductivity decreases with temperature. The reason for the difference is the electronic origin of thermal conductivity in U 3Si 2, as compared to the phonon mechanism responsible for thermal transport in UO 2. The phonon thermal conductivity in UO 2 is unusually low for a fluorite oxidemore » due to the strong interaction with the spins in the paramagnetic phase. The thermal conductivity of U 3Si 2 as well as other U-­Si compounds has been measured experimentally [1-­4]. However, for fuel performance simulations it is also critical to model the degradation of the thermal conductivity due to damage and microstructure evolution caused by the reactor environment (irradiation and high temperature). For UO 2 this reduction is substantial and it has been the topic of extensive NEAMS research resulting in several publications [5, 6]. There are no data or models for the evolution of the U 3Si 2 thermal conductivity under irradiation. We know that the intrinsic thermal conductivities of UO 2 (semi-conductor) and U 3Si 2 (metal) are very different, and we do not necessarily expect the dependence on damage to be the same either, which could present another advantage for the silicide fuel. In this report we summarize the first step in developing a model for the thermal conductivity of U-­Si compounds with the goal of capturing the effect of damage in U 3Si 2. Next year, we will focus on lattice damage. We will also attempt to assess the impact of fission gas bubbles.« less

Nuclear fuels for very high temperature applications

NASA Astrophysics Data System (ADS)

Lundberg, L. B.; Hobbins, R. R.

The success of the development of nuclear thermal propulsion devices and thermionic space nuclear power generation systems depends on the successful utilization of nuclear fuel materials at temperatures in the range 2000 to 3500 K. Problems associated with the utilization of uranium bearing fuel materials at these very high temperatures while maintaining them in the solid state for the required operating times are addressed. The critical issues addressed include evaporation, melting, reactor neutron spectrum, high temperature chemical stability, fabrication, fission induced swelling, fission product release, high temperature creep, thermal shock resistance, and fuel density, both mass and fissile atom. Candidate fuel materials for this temperature range are based on UO2 or uranium carbides. Evaporation suppression, such as a sealed cladding, is required for either fuel base. Nuclear performance data needed for design are sparse for all candidate fuel forms in this temperature range, especially at the higher temperatures.

Dissolution process for ZrO.sub.2 -UO.sub.2 -CaO fuels

DOEpatents

Paige, Bernice E.

1976-06-22

The present invention provides an improved dissolution process for ZrO.sub.2 -UO.sub.2 -CaO-type pressurized water reactor fuels. The zirconium cladding is dissolved with hydrofluoric acid, immersing the ZrO.sub.2 -UO.sub.2 -CaO fuel wafers in the resulting zirconium-dissolver-product in the dissolver vessel, and nitric acid is added to the dissolver vessel to facilitate dissolution of the uranium from the ZrO.sub.2 -UO.sub.2 -CaO fuel wafers.

PREPARATION OF UO$sub 2$ FOR NUCLEAR REACTOR FUEL PELLETS

DOEpatents

Googin, J.M.

1962-06-01

A method is given for preparing high-density UO/sub 2/ compacts. An aqueous uranyl fluoride solution is contacted with an aqueous ammonium hydroxide solution at an ammonium to-uranium ratio of 25: 1 to 30:1 to form a precipitate. The precipitate is separated from the- mother liquor, dried, and contacted with steam at a uniform temperature within the range of 400 to 650 deg C to produce U/ sub 3/O/sub 8/. The U/sub 3/O/sub 8/ is red uced to UO/sub 2/ with hydrogen at a uniform temperature within the range of 550 to 600 deg C. The UO/sub 2/ is then compressed into compacts and sintered. High-density compacts are fabricated to close tolerances without use of a binder and without machining or grinding. (AEC)

Non-stoichiometry in U 3Si 2

DOE PAGES

Middleburgh, Simon C.; Grimes, Robin W.; Lahoda, Ed J.; ...

2016-10-08

Uranium silicides, in particular U 3Si 2, are being explored as an advanced nuclear fuel with increased accident tolerance as well as competitive economics compared to the baseline UO 2 fuel. Here we use density functional theory calculations and thermochemical analysis to assess the stability of U 3Si 2 with respect to non-stoichiometry reactions in both the hypo- and hyper-stoichiometric regimes. We find that the degree of non-stoichiometry in U 3Si 2 is much smaller than in UO 2 and at most reaches a few percent at high temperature. Non-stoichiometry impacts fuel performance by determining whether the loss of uraniummore » due to fission leads to a non-stoichiometric U 3Si 2±x phase or precipitation of a second U-Si phase. Lastly, we also investigate the U 5Si 4 phase as a candidate for the equilibrium phase diagram.« less

Thermodynamic studies of studtite thermal decomposition pathways via amorphous intermediates UO 3, U 2O 7, and UO 4

DOE PAGES

Guo, Xiaofeng; Wu, Di; Xu, Hongwu; ...

2016-09-01

The thermal decomposition of studtite (UO 2)O 2(H 2O) 2·2H 2O results in a series of intermediate X-ray amorphous materials with general composition UO 3+x (x = 0, 0.5, 1). As an extension of a structural study on U 2O 7, this work provides detailed calorimetric data on these amorphous oxygen-rich materials since their energetics and thermal stability are unknown. These were characterized in situ by thermogravimetry, and mass spectrometry. Ex situ X-ray diffraction and infrared spectroscopy characterized their chemical bonding and local structures. This detailed characterization formed the basis for obtaining formation enthalpies by high temperature oxide melt solutionmore » calorimetry. The thermodynamic data demonstrate the metastability of the amorphous UO 3+x materials, and explain their irreversible and spontaneous reactions to generate oxygen and form metaschoepite. Thus, formation of studtite in the nuclear fuel cycle, followed by heat treatment, can produce metastable amorphous UO 3+x materials that pose the risk of significant O 2 gas. Quantitative knowledge of the energy landscape of amorphous UO 3+x was provided for stability analysis and assessment of conditions for decomposition.« less

Design of a uranium-dioxide powder spheroidization system by plasma processing

NASA Astrophysics Data System (ADS)

Cavender, Daniel

The plasma spheroidization system (PSS) is the first process in the development of a tungsten-uranium dioxide (W-UO2) ceramic-metallic (cermet) fuel for nuclear thermal rocket (NTR) propulsion. For the purposes of fissile fuel retention, UO2 spheroids ranging in size from 50 - 100 micrometers (μm) in diameter will be encapsulated in a tungsten shell. The PSS produces spherical particles by melting angular stock particles in an argon-hydrogen plasma jet where they become spherical due to surface tension. Surrogate CeO 2 powder was used in place of UO2 for system and process parameter development. Stock and spheroidized powders were micrographed using optical and scanning electron microscopy and evaluated by statistical methods to characterize and compare the spherocity of pre and post process powders. Particle spherocity was determined by irregularity parameter. Processed powders showed a statistically significant improvement in spherocity, with greater that 60% of the examined particles having an irregularity parameter of equal to or lower than 1.2, compared to stock powder.

Characterisation of high temperature refractory ceramics for nuclear applications

NASA Astrophysics Data System (ADS)

Bottomley, P. D. W.; Wiss, Th; Janssen, A.; Cremer, B.; Thiele, H.; Manara, D.; Scheindlin, M.; Murray-Farthing, M.; Lajarge, P.; Menna, M.; Bouexière, D.; Rondinella, V. V.

2012-03-01

The ternary oxide ceramic system UO2-ZrO2-FeO is a refractory system that is of great relevance to the nuclear industry as it represents one of the main systems resulting from the interaction of the Zircaloy cladding, the UO2 fuel and the structural elements of a nuclear reactor. It is particularly the high temperature properties that require investigation; that is, when substantial overheating of the nuclear core occurs and interactions can lead to its degradation, melting and result in a severe nuclear accident. There has been much work on the UO2-ZrO2 system and also on the ternary system with FeO but there is still a need to examine 2 further aspects; firstly the effect of sub-oxidized systems, the UO2-Zr and FeO-Zr systems, and secondly the effect of Fe/Zr or Fe/U ratios on the melting point of the U-Zr-Fe oxide system. Samples of UO2-Zr and UO2-ZrO2-FeO were fabricated at ITU and then characterized by optical microscopy (OM) and X-ray diffraction to determine the ceramic's structure and verify the composition. Thereafter the samples are to be melted by laser flash heating and their liquidus and solidus temperatures determined by pyrometry. This programme is currently ongoing. The frozen samples, after testing, were then sectioned, polished and the molten zone micro-analytically examined by OM & SEM-EDS in order to determine its structure and composition and to compare with the existing phase diagrams. Examples of results from these systems will be given. Finally, a reacted Zr-FeO thermite mixture was examined, which had been used to generate high temperatures during tests of reactor melt-concrete interactions. The aim was to assess the reaction and estimate the heat generation from this novel technique. These results allow verification or improvement of the phase diagram and are of primary importance as input to models used to predict materials interactions in a severe nuclear accident.

Nuclear forensic analysis of uranium oxide powders interdicted in Victoria, Australia

DOE PAGES

Kristo, Michael Joseph; Keegan, Elizabeth; Colella, Michael; ...

2015-04-13

Nuclear forensic analysis was conducted on two uranium samples confiscated during a police investigation in Victoria, Australia. The first sample, designated NSR-F-270409-1, was a depleted uranium powder of moderate purity (~1000 μg/g total elemental impurities). The chemical form of the uranium was a compound similar to K 2(UO 2) 3O 4·4H 2O. While aliquoting NSR-F-270409-1 for analysis, the body and head of a Tineid moth was discovered in the sample. The second sample, designated NSR-F-270409-2, was also a depleted uranium powder. It was of reasonably high purity (~380 μg/g total elemental impurities). The chemical form of the uranium was primarilymore » UO 3·2H 2O, with minor phases of U 3O 8 and UO 2. While aliquoting NSR-F-270409-2 for analysis, a metal staple of unknown origin was discovered in the sample. The presence of 236U and 232U in both samples indicates that the uranium feed stocks for these samples experienced a neutron flux at some point in their history. The reactor burn-up calculated from the isotopic composition of the uranium is consistent with that of spent fuel from natural uranium (NU) fueled Pu production. These nuclear forensic conclusions allow us to categorically exclude Australia as the origin of the material and greatly reduce the number of candidate sources.« less

Effect of High Si Content on U3Si2 Fuel Microstructure

NASA Astrophysics Data System (ADS)

Rosales, Jhonathan; van Rooyen, Isabella J.; Meher, Subhashish; Hoggan, Rita; Parga, Clemente; Harp, Jason

2018-02-01

The development of U3Si2 as an accident-tolerant nuclear fuel has gained research interest because of its promising high uranium density and improved thermal properties. In the present study, three samples of U3Si2 fuel with varying silicon content have been fabricated by a conventional powder metallurgical route. Microstructural characterization via scanning and transmission electron microscopy reveals the presence of other stoichiometry of uranium silicide such as USi and UO2 in both samples. The detailed phase analysis by x-ray diffraction shows the presence of secondary phases, such as USi, U3Si, and UO2. The samples with higher concentrations of silicon content of 7.5 wt.% display additional elemental Si. These samples also possess an increased amount of the USi phase as compared to that in the conventional sample with 7.3 wt.% silicon. The optimization of U3Si2 fuel performance through the understanding of the role of Si content on its microstructure has been discussed.

On the condition of UO2 nuclear fuel irradiated in a PWR to a burn-up in excess of 110 MWd/kgHM

NASA Astrophysics Data System (ADS)

Restani, R.; Horvath, M.; Goll, W.; Bertsch, J.; Gavillet, D.; Hermann, A.; Martin, M.; Walker, C. T.

2016-12-01

Post-irradiation examination results are presented for UO2 fuel from a PWR fuel rod that had been irradiated to an average burn-up of 105 MWd/kgHM and showed high fission gas release of 42%. The radial distribution of xenon and the partitioning of fission gas between bubbles and the fuel matrix was investigated using laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) and electron probe microanalysis. It is concluded that release from the fuel at intermediate radial positions was mainly responsible for the high fission gas release. In this region thermal release had occurred from the high burn-up structure (HBS) at some point after the sixth irradiation cycle. The LA-ICP-MS results indicate that gas release had also occurred from the HBS in the vicinity of the pellet periphery. It is shown that the gas pressure in the HBS pores is well below the pressure that the fuel can sustain.

Evaluation of Non-Oxide Fuel for Fission-based Nuclear Reactors on Spacecraft

DTIC Science & Technology

smaller and potentially lighter core, whichis a significant advantage. The results of this study indicate that use of both UC and UN may result in significant weight savings due tohigher uranium loading density....The goal of this project was to study the performance of atypical uranium-based fuels in a nuclear reactor capable of producing 1 megawattof thermal...UN), or uranium carbide (UC) and compared their performance to uranium oxide (UO2) which is thefuel form used in the vast majority of commercial

Oxide particle size distribution from shearing irradiated and unirradiated LWR fuels in Zircaloy and stainless steel cladding: significance for risk assessment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davis, W. Jr.; West, G.A.; Stacy, R.G.

1979-03-22

Sieve fractionation was performed with oxide particles dislodged during shearing of unirradiated or irradiated fuel bundles or single rods of UO/sub 2/ or 96 to 97% ThO/sub 2/--3 to 4% UO/sub 2/. Analyses of these data by nonlinear least-squares techniques demonstrated that the particle size distribution is lognormal. Variables involved in the numerical analyses include lognormal median size, lognormal standard deviation, and shear cut length. Sieve-fractionation data are presented for unirradiated bundles of stainless-steel-clad or Zircaloy-2-clad UO/sub 2/ or ThO/sub 2/--UO/sub 2/ sheared into lengths from 0.5 to 2.0 in. Data are also presented for irradiated single rods (sheared intomore » lengths of 0.25 to 2.0 in.) of Zircaloy-2-clad UO/sub 2/ from BWRs and of Zircaloy-4-clad UO/sub 2/ from PWRs. Median particle sizes of UO/sub 2/ from shearing irradiated stainless-steel-clad fuel ranged from 103 to 182 ..mu..m; particle sizes of ThO/sub 2/--UO/sub 2/, under these same conditions, ranged from 137 to 202 ..mu..m. Similarly, median particle sizes of UO/sub 2/ from shearing unirradiated Zircaloy-2-clad fuel ranged from 230 to 957 ..mu..m. Irradiation levels of fuels from reactors ranged from 9,000 to 28,000 MWd/MTU. In general, particle sizes from shearing these irradiated fuels are larger than those from the unirradiated fuels; however, unirradiated fuel from vendors was not available for performing comparative shearing experiments. In addition, variations in particle size parameters pertaining to samples of a single vendor varied as much as those between different vendors. The fraction of fuel dislodged from the cladding is nearly proportional to the reciprocal of the shear cut length, until the cut length attains some minimum value below which all fuel is dislodged. Particles of fuel are generally elongated with a long-to-short axis ratio usually less than 3. Using parameters of the lognormal distribution estimates can be made of fractions of dislodged fuel having dimensions less than specified values.« less

Argentina-LLNL-LANL Comparative Sample Analysis on UO2 fuel pellet CRM-125A for Nuclear Forensics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kips, R.

The recent workshop on analytical plan development provided context and background for the next step in this engagement, i.e. a comparative sample analysis on CRM 125-A. This is a commercially available certified low-enriched uranium oxide fuel pellet material from New Brunswick National Laboratory (NBL) (see certificate in Annex 1).

Phenomenological model of sintering of oxide nuclear fuel with doping admixtures

NASA Astrophysics Data System (ADS)

Baranov, V. G.; Devyatko, Yu. N.; Tenishev, A. V.; Khomyakov, O. V.

2015-12-01

It is shown that a change in the linear dimension of compacted UO2 in the sintering process is associated with its plastic yielding under the action of the forces of residual stress and capillary forces. From the curves of sintering of a fuel with doping admixtures in various gaseous media, its rate of creep is reduced.

FASTGRASS implementation in BISON and Fission gas behavior characterization in UO 2 and connection to validating MARMOT

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yun, Di; Mo, Kun; Ye, Bei

2015-09-30

This activity is supported by the US Nuclear Energy Advanced Modeling and Simulation (NEAMS) Fuels Product Line (FPL). Two major accomplishments in FY 15 are summarized in this report: (1) implementation of the FASTGRASS module in the BISON code; and (2) a Xe implantation experiment for large-grained UO 2. Both BISON AND MARMOT codes have been developed by Idaho National Laboratory (INL) to enable next generation fuel performance modeling capability as part of the NEAMS Program FPL. To contribute to the development of the Moose-Bison-Marmot (MBM) code suite, we have implemented the FASTGRASS fission gas model as a module inmore » the BISON code. Based on rate theory formulations, the coupled FASTGRASS module in BISON is capable of modeling LWR oxide fuel fission gas behavior and fission gas release. In addition, we conducted a Xe implantation experiment at the Argonne Tandem Linac Accelerator System (ATLAS) in order to produce the needed UO 2 samples with desired bubble morphology. With these samples, further experiments to study the fission gas diffusivity are planned to provide validation data for the Fission Gas Release Model in MARMOT codes.« less

Thermal Aspects of Using Alternative Nuclear Fuels in Supercritical Water-Cooled Reactors

NASA Astrophysics Data System (ADS)

Grande, Lisa Christine

A SuperCritical Water-cooled Nuclear Reactor (SCWR) is a Generation IV concept currently being developed worldwide. Unique to this reactor type is the use of light-water coolant above its critical point. The current research presents a thermal-hydraulic analysis of a single fuel channel within a Pressure Tube (PT)-type SCWR with a single-reheat cycle. Since this reactor is in its early design phase many fuel-channel components are being investigated in various combinations. Analysis inputs are: steam cycle, Axial Heat Flux Profile (AHFP), fuel-bundle geometry, and thermophysical properties of reactor coolant, fuel sheath and fuel. Uniform and non-uniform AHFPs for average channel power were applied to a variety of alternative fuels (mixed oxide, thorium dioxide, uranium dicarbide, uranium nitride and uranium carbide) enclosed in an Inconel-600 43-element bundle. The results depict bulk-fluid, outer-sheath and fuel-centreline temperature profiles together with the Heat Transfer Coefficient (HTC) profiles along the heated length of fuel channel. The objective is to identify the best options in terms of fuel, sheath material and AHFPS in which the outer-sheath and fuel-centreline temperatures will be below the accepted temperature limits of 850°C and 1850°C respectively. The 43-element Inconel-600 fuel bundle is suitable for SCWR use as the sheath-temperature design limit of 850°C was maintained for all analyzed cases at average channel power. Thoria, UC2, UN and UC fuels for all AHFPs are acceptable since the maximum fuel-centreline temperature does not exceed the industry accepted limit of 1850°C. Conversely, the fuel-centreline temperature limit was exceeded for MOX at all AHFPs, and UO2 for both cosine and downstream-skewed cosine AHFPs. Therefore, fuel-bundle modifications are required for UO2 and MOX to be feasible nuclear fuels for SCWRs.

The effect of fission products on the rate of U3O8 formation in SIMFUEL oxidized in air at 250°C

NASA Astrophysics Data System (ADS)

Choi, Jong-Won; McEachern, Rod J.; Taylor, Peter; Wood, Donald D.

1996-06-01

The effect of fission products on the rate of U3O8 formation was investigated by oxidizing UO2-based SIMFUEL (simulated high burnup nuclear fuel) and unirradiated UO2 fuel specimens in air at 250°C for different times (1-317 days). The progress of oxidation was monitored by X-ray diffraction, revealing that the rate of U3O8 formation declines with increasing burnup. An expression was derived to describe quantitatively the time for U3O8 powder formation as a function of simulated burnup. These findings were supported by additional isochronal oxidation experiments conducted between 200 and 300°C.

Instant release fraction corrosion studies of commercial UO2 BWR spent nuclear fuel

NASA Astrophysics Data System (ADS)

Martínez-Torrents, Albert; Serrano-Purroy, Daniel; Sureda, Rosa; Casas, Ignasi; de Pablo, Joan

2017-05-01

The instant release fraction of a spent nuclear fuel is a matter of concern in the performance assessment of a deep geological repository since it increases the radiological risk. Corrosion studies of two different spent nuclear fuels were performed using bicarbonate water under oxidizing conditions to study their instant release fraction. From each fuel, cladded segments and powder samples obtained at different radial positions were used. The results were normalised using the specific surface area to permit a comparison between fuels and samples. Different radionuclide dissolution patterns were studied in terms of water contact availability and radial distribution in the spent nuclear fuel. The relationship between the results of this work and morphological parameters like the grain size or irradiation parameters such as the burn-up or the linear power density was studied in order to increase the understanding of the instant release fraction formation.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kristo, Michael Joseph; Keegan, Elizabeth; Colella, Michael

Nuclear forensic analysis was conducted on two uranium samples confiscated during a police investigation in Victoria, Australia. The first sample, designated NSR-F-270409-1, was a depleted uranium powder of moderate purity (~1000 μg/g total elemental impurities). The chemical form of the uranium was a compound similar to K 2(UO 2) 3O 4·4H 2O. While aliquoting NSR-F-270409-1 for analysis, the body and head of a Tineid moth was discovered in the sample. The second sample, designated NSR-F-270409-2, was also a depleted uranium powder. It was of reasonably high purity (~380 μg/g total elemental impurities). The chemical form of the uranium was primarilymore » UO 3·2H 2O, with minor phases of U 3O 8 and UO 2. While aliquoting NSR-F-270409-2 for analysis, a metal staple of unknown origin was discovered in the sample. The presence of 236U and 232U in both samples indicates that the uranium feed stocks for these samples experienced a neutron flux at some point in their history. The reactor burn-up calculated from the isotopic composition of the uranium is consistent with that of spent fuel from natural uranium (NU) fueled Pu production. These nuclear forensic conclusions allow us to categorically exclude Australia as the origin of the material and greatly reduce the number of candidate sources.« less

Dissolution of spent nuclear fuel in carbonate-peroxide solution

NASA Astrophysics Data System (ADS)

Soderquist, Chuck; Hanson, Brady

2010-01-01

This study shows that spent UO2 fuel can be completely dissolved in a room temperature carbonate-peroxide solution apparently without attacking the metallic Mo-Tc-Ru-Rh-Pd fission product phase. In parallel tests, identical samples of spent nuclear fuel were dissolved in nitric acid and in an ammonium carbonate, hydrogen peroxide solution. The resulting solutions were analyzed for strontium-90, technetium-99, cesium-137, europium-154, plutonium, and americium-241. The results were identical for all analytes except technetium, where the carbonate-peroxide dissolution had only about 25% of the technetium that the nitric acid dissolution had.

Biokinetics of nuclear fuel compounds and biological effects of nonuniform radiation.

PubMed Central

Lang, S; Servomaa, K; Kosma, V M; Rytömaa, T

1995-01-01

Environmental releases of insoluble nuclear fuel compounds may occur at nuclear power plants during normal operation, after nuclear power plant accidents, and as a consequence of nuclear weapons testing. For example, the Chernobyl fallout contained extensive amounts of pulverized nuclear fuel composed of uranium and its nonvolatile fission products. The effects of these highly radioactive particles, also called hot particles, on humans are not well known due to lack of reliable data on the extent of the exposure. However, the biokinetics and biological effects of nuclear fuel compounds have been investigated in a number of experimental studies using various cellular systems and laboratory animals. In this article, we review the biokinetic properties and effects of insoluble nuclear fuel compounds, with special reference to UO2, PuO2, and nonvolatile, long-lived beta-emitters Zr, Nb, Ru, and Ce. First, the data on hot particles, including sources, dosimetry, and human exposure are discussed. Second, the biokinetics of insoluble nuclear fuel compounds in the gastrointestinal tract and respiratory tract are reviewed. Finally, short- and long-term biological effects of nonuniform alpha- and beta-irradiation on the gastrointestinal tract, lungs, and skin are discussed. Images p920-a Figure 1. PMID:8529589

Neutronics Benchmarks for the Utilization of Mixed-Oxide Fuel: Joint U.S./Russian Progress Report for Fiscal Year 1997

DOE Office of Scientific and Technical Information (OSTI.GOV)

Akkurt, H

2001-01-11

In 1967, a series of critical experiments were conducted at the Westinghouse Reactor Evaluation Center (WREC) using mixed-oxide (MOX) PuO{sub 2}-UO{sub 2} and/or UO{sub 2} fuels in various lattices and configurations . These experiments were performed under the joint sponsorship of the Empire State Atomic Development Associates (ESADA) plutonium program and Westinghouse . The purpose of these experiments was to develop experimental data to validate analytical methods used in the design of a plutonium-bearing replacement fuel for water reactors. Three different fuels were used during the experimental program: two MOX fuels and a low-enriched UO{sub 2} fuel. The MOX fuelsmore » were distinguished by their {sup 240}Pu content: 8 wt% {sup 240}Pu and 24 wt% {sup 240}Pu. Both MOX fuels contained 2.0 wt % PuO{sub 2} in natural UO{sub 2} . The UO{sub 2} fuel with 2.72 wt % enrichment was used for comparison with the plutonium data and for use in multiregion experiments.« less

Irradiation effects and micro-structural changes in large grain uranium dioxide fuel investigated by micro-beam X-ray diffraction

NASA Astrophysics Data System (ADS)

Mieszczynski, C.; Kuri, G.; Degueldre, C.; Martin, M.; Bertsch, J.; Borca, C. N.; Grolimund, D.; Delafoy, Ch.; Simoni, E.

2014-01-01

Microstructural changes in a set of commercial grade UO2 fuel samples have been investigated using synchrotron based micro-focused X-ray fluorescence (μ-XRF) and X-ray diffraction (μ-XRD) techniques. The results are associated with conventional UO2 materials and relatively larger grain chromia-doped UO2 fuels, irradiated in a commercial light water reactor plant (average burn-up: 40 MW d kg-1). The lattice parameters of UO2 in fresh and irradiated specimens have been measured and compared with theoretical predictions. In the pristine state, the doped fuel has a somewhat smaller lattice parameter than the standard UO2 as a result of chromia doping. Increase in micro-strain and lattice parameter in irradiated materials is highlighted. All irradiated samples behave in a similar manner with UO2 lattice expansion occurring upon irradiation, where any Cr induced effect seems insignificant and accumulated lattice defects prevail. Elastic strain energy densities in the irradiated fuels are also evaluated based on the UO2 crystal lattice strain and non-uniform strain. The μ-XRD patterns further allow the evaluation of the crystalline domain size and sub-grain formation at different locations of the irradiated UO2 pellets.

Thermodynamic and kinetic modelling of fuel oxidation behaviour in operating defective fuel

NASA Astrophysics Data System (ADS)

Lewis, operating defective fuel B. J.; Thompson, W. T.; Akbari, F.; Thompson, D. M.; Thurgood, C.; Higgs, J.

2004-07-01

A theoretical treatment has been developed to predict the fuel oxidation behaviour in operating defective nuclear fuel elements. The equilibrium stoichiometry deviation in the hyper-stoichiometric fuel has been derived from thermodynamic considerations using a self-consistent set of thermodynamic properties for the U-O system, which emphasizes replication of solubilities and three-phase invariant conditions displayed in the U-O binary phase diagram. The kinetics model accounts for multi-phase transport including interstitial oxygen diffusion in the solid and gas-phase transport of hydrogen and steam in the fuel cracks. The fuel oxidation model is further coupled to a heat conduction model to account for the feedback effect of a reduced thermal conductivity in the hyper-stoichiometric fuel. A numerical solution has been developed using a finite-element technique with the FEMLAB software package. The model has been compared to available data from several in-reactor X-2 loop experiments with defective fuel conducted at the Chalk River Laboratories. The model has also been benchmarked against an O/U profile measurement for a spent defective fuel element discharged from a commercial reactor.

Effect of metallic iron on the oxidative dissolution of UO2 doped with a radioactive alpha emitter in synthetic Callovian-Oxfordian groundwater

NASA Astrophysics Data System (ADS)

Odorowski, Mélina; Jegou, Christophe; De Windt, Laurent; Broudic, Véronique; Jouan, Gauthier; Peuget, Sylvain; Martin, Christelle

2017-12-01

In the hypothesis of direct disposal of spent fuel in a geological nuclear waste repository, interactions between the fuel mainly composed of UO2 and its environment must be understood. The dissolution rate of the UO2 matrix, which depends on the redox conditions on the fuel surface, will have a major impact on the release of radionuclides into the environment. The reducing conditions expected for a geological disposal situation would appear to be favorable as regards the solubility and stability of the UO2 matrix, but may be disturbed on the surface of irradiated fuel. In particular, the local redox conditions will result from a competition between the radiolysis effects of water under alpha irradiation (simultaneously producing oxidizing species like H2O2, hydrogen peroxide, and reducing species like H2, hydrogen) and those of redox active species from the environment. In particular, Fe2+, a strongly reducing aqueous species coming from the corrosion of the iron canister or from the host rock, could influence the dissolution of the fuel matrix. The effect of iron on the oxidative dissolution of UO2 was thus investigated under the conditions of the French disposal site, a Callovian-Oxfordian clay formation chosen by the French National Radioactive Waste Management Agency (Andra), here tested under alpha irradiation. For this study, UO2 fuel pellets doped with a radioactive alpha emitter (238/239Pu) were leached in synthetic Callovian-Oxfordian groundwater (representative of the French waste disposal site groundwater) in the presence of a metallic iron foil to simulate the steel canister. The pellets had varying levels of alpha activity, in order to modulate the concentrations of species produced by water radiolysis on the surface and to simulate the activity of aged spent fuel after 50 and 10,000 years of alpha radioactivity decay. The experimental data showed that whatever the sample alpha radioactivity, the presence of iron inhibits the oxidizing dissolution of UO2 and leads to low uranium concentrations (between 4 × 10-10 and 4 × 10-9 M), through a reactional mechanism located in the very first microns of the UO2/water reactional interface. The mechanism involves consumption of oxidizing species, in particular of H2O2 by Fe2+ at the precise place where these species are produced, and is accompanied by the precipitation of an akaganeite-type Fe3+ hydroxide on the surface. The higher the radioactivity of the samples, the greater the precipitation induced. Modeling has been developed, coupling chemistry with transport and based on the main reactional mechanisms identified, which enables accurate reproduction of the mineralogy of the system under study, giving the nature of the phases under observation as well as the location of their precipitation. Obviously without excluding a potential contribution from the hydrogen produced by the anoxic corrosion of the iron foil, this study has shown that iron plays a major role in this oxidizing dissolution inhibition process for the system investigated (localized alpha radiolysis). This inhibitor effect associated with iron is therefore strongly dependent on the location of the redox front, which is found on the surface in the case of alpha irradiation UO2/water reactional interface.

Development of Xe and Kr empirical potentials for CeO 2, ThO 2, UO 2 and PuO 2, combining DFT with high temperature MD

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cooper, M. W. D.; Kuganathan, N.; Burr, P. A.

In this study, the development of embedded atom method (EAM) many-body potentials for actinide oxides and associated mixed oxide (MOX) systems has motivated the development of a complementary parameter set for gas-actinide and gas-oxygen interactions. A comprehensive set of density functional theory (DFT) calculations were used to study Xe and Kr incorporation at a number of sites in CeO 2, ThO 2, UO 2 and PuO 2. These structures were used to fit a potential, which was used to generate molecular dynamics (MD) configurations incorporating Xe and Kr at 300 K, 1500 K, 3000 K and 5000 K. Subsequent matchingmore » to the forces predicted by DFT for these MD configurations was used to refine the potential set. This fitting approach ensured weighted fitting to configurations that are thermodynamically significant over a broad temperature range, while avoiding computationally expensive DFT-MD calculations. The resultant gas potentials were validated against DFT trapping energies and are suitable for simulating combinations of Xe and Kr in solid solutions of CeO 2, ThO 2, UO 2 and PuO 2, providing a powerful tool for the atomistic simulation of conventional nuclear reactor fuel UO 2 as well as advanced MOX fuels.« less

Development of Xe and Kr empirical potentials for CeO 2, ThO 2, UO 2 and PuO 2, combining DFT with high temperature MD

DOE PAGES

Cooper, M. W. D.; Kuganathan, N.; Burr, P. A.; ...

2016-08-23

In this study, the development of embedded atom method (EAM) many-body potentials for actinide oxides and associated mixed oxide (MOX) systems has motivated the development of a complementary parameter set for gas-actinide and gas-oxygen interactions. A comprehensive set of density functional theory (DFT) calculations were used to study Xe and Kr incorporation at a number of sites in CeO 2, ThO 2, UO 2 and PuO 2. These structures were used to fit a potential, which was used to generate molecular dynamics (MD) configurations incorporating Xe and Kr at 300 K, 1500 K, 3000 K and 5000 K. Subsequent matchingmore » to the forces predicted by DFT for these MD configurations was used to refine the potential set. This fitting approach ensured weighted fitting to configurations that are thermodynamically significant over a broad temperature range, while avoiding computationally expensive DFT-MD calculations. The resultant gas potentials were validated against DFT trapping energies and are suitable for simulating combinations of Xe and Kr in solid solutions of CeO 2, ThO 2, UO 2 and PuO 2, providing a powerful tool for the atomistic simulation of conventional nuclear reactor fuel UO 2 as well as advanced MOX fuels.« less

METHOD OF PREPARING A CERAMIC FUEL ELEMENT

DOEpatents

Ross, W.T.; Bloomster, C.H.; Bardsley, R.E.

1963-09-01

A method is described for preparing a fuel element from -325 mesh PuO/ sub 2/ and -20 mesh UO/sub 2/, and the steps of screening --325 mesh UO/sub 2/ from the -20 mesh UO/sub 2/, mixing PuO/sub 2/ with the --325 mesh UO/sub 2/, blending this mixture with sufficient --20 mesh UO/sub 2/ to obtain the desired composition, introducing the blend into a metal tube, repeating the procedure until the tube is full, and vibrating the tube to compact the powder are included. (AEC)

Milestone report: The simulation of radiation driven gas diffusion in UO 2 at low temperature

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cooper, Michael William; Kuganathan, Navaratnarajah; Burr, Patrick A

2016-10-24

Below 1000 K it is thought that fission gas diffusion in nuclear fuel during irradiation occurs through atomic mixing due to radiation damage. This is an important process for nuclear reactor performance as it affects fission gas release, particularly from the periphery of the pellet where such temperatures are normal. Here we present a molecular dynamics study of Xe and Kr diffusion due to irradiation. Thermal spikes and cascades have been used to study the electronic stopping and ballistic phases of damage, respectively. Our results predict that O and Kr exhibit the greatest diffusivity and U the least, while Xemore » lies in between. It is concluded that the ballistic phase does not sufficiently account for the experimentally observed diffusion. Preliminary thermal spike calculations indicate that the electronic stopping phase generates greater fission gas displacement than the ballistic phase, although further calculation must be carried out to confirm this. A good description of the system by the empirical potentials is important over the very wide temperatures induced during thermal spike and damage cascade simulations. This has motivated the development of a parameter set for gas-actinide and gas-oxygen interactions that is complementary for use with a recent many-body potential set. A comprehensive set of density functional theory (DFT) calculations were used to study Xe and Kr incorporation at a number of sites in CeO 2, ThO 2, UO 2 and PuO 2. These structures were used to fit a potential, which was used to generate molecular dynamics (MD) configurations incorporating Xe and Kr at 300 K, 1500 K, 3000 K and 5000 K. Subsequent matching to the forces predicted by DFT for these MD configurations was used to refine the potential set. This fitting approach ensured weighted fitting to configurations that are thermodynamically significant over a broad temperature range, while avoiding computationally expensive DFT-MD calculations. The resultant gas potentials were validated against DFT binding energies and are suitable for simulating combinations of Xe and Kr in solid solutions of CeO 2, ThO 2, UO 2 and PuO 2, providing a powerful tool for the atomistic simulation of conventional nuclear reactor fuel UO 2 as well as advanced MOX fuels.« less

A multiphase interfacial model for the dissolution of spent nuclear fuel

NASA Astrophysics Data System (ADS)

Jerden, James L.; Frey, Kurt; Ebert, William

2015-07-01

The Fuel Matrix Dissolution Model (FMDM) is an electrochemical reaction/diffusion model for the dissolution of spent uranium oxide fuel. The model was developed to provide radionuclide source terms for use in performance assessment calculations for various types of geologic repositories. It is based on mixed potential theory and consists of a two-phase fuel surface made up of UO2 and a noble metal bearing fission product phase in contact with groundwater. The corrosion potential at the surface of the dissolving fuel is calculated by balancing cathodic and anodic reactions occurring at the solution interfaces with UO2 and NMP surfaces. Dissolved oxygen and hydrogen peroxide generated by radiolysis of the groundwater are the major oxidizing agents that promote fuel dissolution. Several reactions occurring on noble metal alloy surfaces are electrically coupled to the UO2 and can catalyze or inhibit oxidative dissolution of the fuel. The most important of these is the oxidation of hydrogen, which counteracts the effects of oxidants (primarily H2O2 and O2). Inclusion of this reaction greatly decreases the oxidation of U(IV) and slows fuel dissolution significantly. In addition to radiolytic hydrogen, large quantities of hydrogen can be produced by the anoxic corrosion of steel structures within and near the fuel waste package. The model accurately predicts key experimental trends seen in literature data, the most important being the dramatic depression of the fuel dissolution rate by the presence of dissolved hydrogen at even relatively low concentrations (e.g., less than 1 mM). This hydrogen effect counteracts oxidation reactions and can limit fuel degradation to chemical dissolution, which results in radionuclide source term values that are four or five orders of magnitude lower than when oxidative dissolution processes are operative. This paper presents the scientific basis of the model, the approach for modeling used fuel in a disposal system, and preliminary calculations to demonstrate the application and value of the model.

Environmental modeling of uranium interstitial compositions of non-stoichiometric oxides: experimental and theoretical analysis.

PubMed

Ivanova, Bojidarka

2016-10-01

Study of uranium interstitial compositions of non-stoichiometric oxides UO2+x (x ∈ 0.1-0.02) in gas and condense phases has been presented, using various soft-ionization mass spectrometric methods such as ESI-, APCI-, and MALDI-MS at a wide dynamic temperature gradient (∈ 25-300 °C). Linearly polarized vibrational spectroscopy has been utilized in order to assign unambiguously, the vibrational frequencies of uranium non-stoichiometric oxides. Experimental design has involved xUO2.66·yUO2.33, xUO2.66·yUO2.33/SiO2, xUO2.66·yUO2.33/SiO2 (NaOH) and SiO2/x'NaOH·y'UO2(NO3)2·6H2O, multicomponent systems (x = 1, y ∈ 0.1-1.0 and x' = 1, y' ∈ 0.1-0.6) as well as phase transitions UO2(NO3)2·6H2O → {U4O9(UO2.25)} → U3O7(UO2.33) → U3O8(UO2.66) → {UO3}, thus ensuring a maximal representativeness to real environmental conditions, where diverse chemical, geochemical and biochemical reactions, including complexation and sorption onto minerals have occurred. Experimental factors such as UV-irradiation, pH, temperature, concentration levels, solvent types and ion strength have been taken into consideration, too. As far as uranium speciation represents a challenging analytical task in terms of chemical identification diverse coordination species, mechanistic aspects relating incorporation of oxygen into UO 2+x form the shown full methods validation significantly impacts the field of environmental radioanalytical chemistry. UO2 is the most commonly used fuel in nuclear reactors around the globe; however, a large non-stoichiometric range ∈ UO1.65-UO2.25 has occurred due to radiolysis of water on UO2 surface yielding to H2O2, OH(·), and more. Each of those compositions has different oxygen diffusion. And in this respect enormous effort has been concentrated to study the potential impact of hazardous radionuclide on the environment, encompassing from the reprocessing to the disposal stages of the fuel waste, including the waste itself, the processes in the waste containers, the clay around the containers, and geological processes. In a broader sense, thereby, this study contributes to field of environmental analysis highlighting the great ability of various soft-ionization MS methods, particularly, MALDI-MS one, for direct assay of complex multicomponent heterogeneous mixtures at fmol-attomol concentration ranges, along with it the great instrumental features allowing, not only meaningful quantitative, but also structural information of the analytes, thus making the method indispensable for environmental speciation of radionuclides, generally.

Issues in the use of Weapons-Grade MOX Fuel in VVER-1000 Nuclear Reactors: Comparison of UO2 and MOX Fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carbajo, J.J.

2005-05-27

The purpose of this report is to quantify the differences between mixed oxide (MOX) and low-enriched uranium (LEU) fuels and to assess in reasonable detail the potential impacts of MOX fuel use in VVER-1000 nuclear power plants in Russia. This report is a generic tool to assist in the identification of plant modifications that may be required to accommodate receiving, storing, handling, irradiating, and disposing of MOX fuel in VVER-1000 reactors. The report is based on information from work performed by Russian and U.S. institutions. The report quantifies each issue, and the differences between LEU and MOX fuels are describedmore » as accurately as possible, given the current sources of data.« less

Thermophysical properties of liquid UO2, ZrO2 and corium by molecular dynamics and predictive models

NASA Astrophysics Data System (ADS)

Kim, Woong Kee; Shim, Ji Hoon; Kaviany, Massoud

2017-08-01

Predicting the fate of accident-melted nuclear fuel-cladding requires the understanding of the thermophysical properties which are lacking or have large scatter due to high-temperature experimental challenges. Using equilibrium classical molecular dynamics (MD), we predict the properties of melted UO2 and ZrO2 and compare them with the available experimental data and the predictive models. The existing interatomic potential models have been developed mainly for the polymorphic solid phases of these oxides, so they cannot be used to predict all the properties accurately. We compare and decipher the distinctions of those MD predictions using the specific property-related autocorrelation decays. The predicted properties are density, specific heat, heat of fusion, compressibility, viscosity, surface tension, and the molecular and electronic thermal conductivities. After the comparisons, we provide readily usable temperature-dependent correlations (including UO2-ZrO2 compounds, i.e. corium melt).

Synchrotron characterization of nanograined UO 2 grain growth

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mo, Kun; Miao, Yinbin; Yun, Di

2015-09-30

This activity is supported by the US Nuclear Energy Advanced Modeling and Simulation (NEAMS) Fuels Product Line (FPL) and aims at providing experimental data for the validation of the mesoscale simulation code MARMOT. MARMOT is a mesoscale multiphysics code that predicts the coevolution of microstructure and properties within reactor fuel during its lifetime in the reactor. It is an important component of the Moose-Bison-Marmot (MBM) code suite that has been developed by Idaho National Laboratory (INL) to enable next generation fuel performance modeling capability as part of the NEAMS Program FPL. In order to ensure the accuracy of the microstructuremore » based materials models being developed within the MARMOT code, extensive validation efforts must be carried out. In this report, we summarize our preliminary synchrotron radiation experiments at APS to determine the grain size of nanograin UO 2. The methodology and experimental setup developed in this experiment can directly apply to the proposed in-situ grain growth measurements. The investigation of the grain growth kinetics was conducted based on isothermal annealing and grain growth characterization as functions of duration and temperature. The kinetic parameters such as activation energy for grain growth for UO 2 with different stoichiometry are obtained and compared with molecular dynamics (MD) simulations.« less

Supplying materials needed for grain growth characterizations of nano-grained UO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mo, Kun; Miao, Yinbin; Yun, Di

2015-09-30

This activity is supported by the US Nuclear Energy Advanced Modeling and Simulation (NEAMS) Fuels Product Line (FPL) and aims at providing experimental data for the validation of the mesoscale simulation code MARMOT. MARMOT is a mesoscale multiphysics code that predicts the coevolution of microstructure and properties within reactor fuel during its lifetime in the reactor. It is an important component of the Moose-Bison-Marmot (MBM) code suite that has been developed by Idaho National Laboratory (INL) to enable next generation fuel performance modeling capability as part of the NEAMS Program FPL. In order to ensure the accuracy of the microstructuremore » based materials models being developed within the MARMOT code, extensive validation efforts must be carried out. In this report, we summarize our preliminary synchrotron radiation experiments at APS to determine the grain size of nanograin UO 2. The methodology and experimental setup developed in this experiment can directly apply to the proposed in-situ grain growth measurements. The investigation of the grain growth kinetics was conducted based on isothermal annealing and grain growth characterization as functions of duration and temperature. The kinetic parameters such as activation energy for grain growth for UO 2 with different stoichiometry are obtained and compared with molecular dynamics (MD) simulations.« less

Identification of the fragmentation of brittle particles during compaction process by the acoustic emission technique.

PubMed

Favretto-Cristini, Nathalie; Hégron, Lise; Sornay, Philippe

2016-04-01

Some nuclear fuels are currently manufactured by a powder metallurgy process that consists of three main steps, namely preparation of the powders, powder compaction, and sintering of the compact. An optimum between size, shape and cohesion of the particles of the nuclear fuels must be sought in order to obtain a compact with a sufficient mechanical strength, and to facilitate the release of helium and fission gases during irradiation through pores connected to the outside of the pellet after sintering. Being simple to adapt to nuclear-oriented purposes, the Acoustic Emission (AE) technique is used to control the microstructure of the compact by monitoring the compaction of brittle Uranium Dioxide (UO2) particles of a few hundred micrometers. The objective is to identify in situ the mechanisms that occur during the UO2 compaction, and more specifically the particle fragmentation that is linked to the open porosity of the nuclear matter. Three zones of acoustic activity, strongly related to the applied stress, can be clearly defined from analysis of the continuous signals recorded during the compaction process. They correspond to particle rearrangement and/or fragmentation. The end of the noteworthy fragmentation process is clearly defined as the end of the significant process that increases the compactness of the material. Despite the fact that the wave propagation strongly evolves during the compaction process, the acoustic signature of the fragmentation of a single UO2 particle and a bed of UO2 particles under compaction is well identified. The waveform, with a short rise time and an exponential-like decay of the signal envelope, is the most reliable descriptor. The impact of the particle size and cohesion on the AE activity, and then on the fragmentation domain, is analyzed through the discrete AE signals. The maximum amplitude of the burst signals, as well as the mean stress corresponding to the end of the recorded AE, increase with increasing mean diameter of the particles. Moreover, the maximum burst amplitude increases with increasing particle cohesion. Copyright © 2015 Elsevier B.V. All rights reserved.

K 2x Sn 4-x S 8-x (x = 0.65–1): a new metal sulfide for rapid and selective removal of Cs + , Sr 2+ and UO 2 2+ ions

DOE PAGES

Sarma, Debajit; Malliakas, Christos D.; Subrahmanyam, K. S.; ...

2015-10-27

The fission of uranium produces radionuclides, 137Cs and 90Sr, which are major constituents of spent nuclear fuel. The half-life of 137Cs and 90Sr is nearly 30 years and thus that makes them harmful to human life and the environment. The selective removal of these radionuclides in the presence of high salt concentrations from industrial nuclear waste is necessary for safe storage. We report the synthesis and crystal structure of K 2xSn 4-xS 8-x (x = 0.65–1, KTS-3) a material which exhibits excellent Cs +, Sr 2+ and UO 2 2+ ion exchange properties in varying conditions. Furthermore, the compound adoptsmore » a layered structure which consists of exchangeable potassium ions sandwiched between infinite layers of octahedral and tetrahedral tin centers. K 2xSn 4-xS 8-x (x = 0.65–1, KTS-3) crystallizes in the monoclinic space group P2 1/c with cell parameters a = 13.092(3) Å, b = 16.882(2) Å, c = 7.375(1) Å and β = 98.10(1)°. Refinement of the single crystal diffraction data revealed the presence of Sn vacancies in the tetrahedra that are long range ordered. The interlayer potassium ions of KTS-3 can be exchanged for Cs +, Sr 2+ and UO 2 2+. KTS-3 exhibits rapid and efficient ion exchange behavior in a broad pH range. The distribution coefficients (K d) for KTS-3 are high for Cs + (5.5 × 10 4), Sr 2+ (3.9 × 10 5) and UO 2 2+ (2.7 × 10 4) at neutral pH (7.4, 6.9, 5.7 ppm Cs +, Sr 2+ and UO 2 2+, respectively; V/m ~ 1000 mL g -1). KTS-3 exhibits impressive Cs +, Sr 2+ and UO 2 2+ ion exchange properties in high salt concentration and over a broad pH range, which coupled with the low cost, environmentally friendly nature and facile synthesis underscores its potential in treating nuclear waste.« less

Neptunium incorporation into select uranyl phases and thermal analysis of select uranyl phases

NASA Astrophysics Data System (ADS)

Klingensmith, Amanda Leigh

Alteration of spent nuclear fuel in a geological repository under oxidizing conditions is likely to result in abundant uranyl compounds. The proposed repository at Yucca Mountain, Nevada is intended to store about 70,000 metric tons of spent nuclear fuel in the unsaturated zone of a welded tuff sequence. Following failure of canisters that encapsulate the waste, contents may be exposed both to air and water and undergo repetitive wetting and drying events. Incorporation of radionuclides into the uranyl alteration phases may significantly reduce their mobility, thereby impacting repository performance. Of particular interest is 237Np owing to its long half-life (2.14 x 106 years) and potential mobility in groundwater. Powders of the synthetic uranyl phase soddyite, (UO2) 2(SiO4)(H2O)2, a framework type structure, and uranophane, Ca[(UO2)(SiO3OH)]2(H 2O)5, kasolite, Pb[(UO2)(SiO4)]H 2O, Na compreignacite, Na2[(UO2)3O 2(OH)3]2(H2O)7, and becquerelite, Ca[(UO2)3O2(OH)3]2(H 2O)8, all of which are sheet type structures, were synthesized in the presence of Np5+ under varying temperature and pH conditions. Uranophane, kasolite, boltwoodite K[(UO2)(SiO3OH)](H 2O)1.5, and Na boltwoodite K,Na[(UO2)(SiO 3OH)](H2O)1.5 were synthesized in the presence of Np as well as P, Ca and/or Mg. Single crystals of Na metaschoepite, Na[(UO 2)4O2(OH)5]˙5H2O were synthesized in the presence of Np5+ and laser ablation verified that Np can be incorporated within the structure of a uranyl phase. Incorporation of Np5+ into soddyite increased steadily with synthesis temperature. Np incorporation into uranophane, becquerelite, and kasolite was not dependent on synthesis temperature. Np uptake in uranophane and kasolite was found to be dependent on synthesis pH, with an increase in Np uptake with higher pH. Uranophane, boltwoodite and Na boltwoodite showed an increase in Np incorporation in the presence of P. Boltwoodite showed an even higher Np uptake when Mg and P were both present in the synthesis. Thermal analysis was completed for the uranyl phases soddyite, becquerelite, Na compreignacite, uranophane, and kasolite. TGA curves for becquerelite, Na compreignacite and uranophane showed loss of interlayer water groups by 100°C. Soddyite and kasolite showed more gradual TGA curves and retention of water groups up to 400°C for soddyite and 550°C for kasolite, with agreement shown by high temperature powder XRD data.

The defect chemistry of UO2 ± x from atomistic simulations

NASA Astrophysics Data System (ADS)

Cooper, M. W. D.; Murphy, S. T.; Andersson, D. A.

2018-06-01

Control of the defect chemistry in UO2 ± x is important for manipulating nuclear fuel properties and fuel performance. For example, the uranium vacancy concentration is critical for fission gas release and sintering, while all oxygen and uranium defects are known to strongly influence thermal conductivity. Here the point defect concentrations in thermal equilibrium are predicted using defect energies from density functional theory (DFT) and vibrational entropies calculated using empirical potentials. Electrons and holes have been treated in a similar fashion to other charged defects allowing for structural relaxation around the localized electronic defects. Predictions are made for the defect concentrations and non-stoichiometry of UO2 ± x as a function of oxygen partial pressure and temperature. If vibrational entropy is omitted, oxygen interstitials are predicted to be the dominant mechanism of excess oxygen accommodation over only a small temperature range (1265 K-1350 K), in contrast to experimental observation. Conversely, if vibrational entropy is included oxygen interstitials dominate from 1165 K to 1680 K (Busker potential) or from 1275 K to 1630 K (CRG potential). Below these temperature ranges, excess oxygen is predicted to be accommodated by uranium vacancies, while above them the system is hypo-stoichiometric with oxygen deficiency accommodated by oxygen vacancies. Our results are discussed in the context of oxygen clustering, formation of U4O9, and issues for fuel behavior. In particular, the variation of the uranium vacancy concentrations as a function of temperature and oxygen partial pressure will underpin future studies into fission gas diffusivity and broaden the understanding of UO2 ± x sintering.

Methodology for Producing a Uniform Distribution of UO2 in a Tungsten Matrix

NASA Technical Reports Server (NTRS)

Tucker, Dennis S.; O'Conner, Andrew; Hickman, Rickman; Broadway, Jeramie; Belancik, Grace

2015-01-01

Current work at NASA's Marshall Space Flight Center (MSFC) is focused on the development CERMET fuel materials for Nuclear Thermal Propulsion (NTP). The CERMETs consist of uranium dioxide (UO2) fuel particles embedded in a tungsten (W) metal matrix. Initial testing of W-UO2 samples fabricated from fine angular powders performed reasonably well, but suffered from significant fuel loss during repeated thermal cycling due to agglomeration of the UO2 (1). The blended powder mixtures resulted in a non-uniform dispersion of the UO2 particles in the tungsten matrix, which allows rapid vaporization of the interconnected UO2 from the sample edges into the bulk material. Also, the angular powders create areas of stress concentrations due to thermal expansion mismatch, which eventually cracks the tungsten matrix. Evenly coating spherical UO2 particles with chemical vapor deposited (CVD) tungsten prior to consolidation was previously demonstrated to provide improved performance. However, the CVD processing technology is expensive and not currently available. In order to reduce cost and enhance performance, a powder coating process has been developed at MSFC to produce a uniform distribution of the spherical UO2 particles in a tungsten matrix. The method involves utilization of a polyethylene binder during mixing which leads to fine tungsten powders clinging to the larger UO2 spherical particles. This process was developed using HfO2 as a surrogate for UO2. Enough powder was mixed to make 8 discs (2cm diameter x 8mm thickness) using spark plasma sintering. A uniaxial pressure of 50 MPa was used at four different temperatures (2 samples at each temperature). The first two samples were heated to 1400C and 1500C respectively for 5 minutes. Densities for these samples were less than 85% of theoretical, so the time at temperature was increased to 20 minutes for the remaining samples. The highest densities were achieved for the two samples sintered at 1700C (approx. 92% of theoretical). Scanning electron microscopy (SEM) of the mixed powders and the sintered samples along with energy dispersive x-ray analysis was obtained. The SEM of the powders clearly show the fine W powder adhered to the larger HfO2 particles and a uniform distribution of HfO2 particles in a tungsten matrix upon densification. Vicker's Microhardness testing was also performed on all samples using 0.5, 1.0 and 2.0 kg loads. Five indents were made at each load level. All indents were placed in the tungsten matrix to assist as a proxy in measuring densification. The highest hardness value was obtained for the 1700C specimens. The hardness average for these samples was 312.14 MPa. This powder processing method has been applied to W/UO2 powders with the SEM of the powders appearing similar to the W/HfO2 powder images.

Thermal diffusivity and conductivity of thorium- uranium mixed oxides

NASA Astrophysics Data System (ADS)

Saoudi, M.; Staicu, D.; Mouris, J.; Bergeron, A.; Hamilton, H.; Naji, M.; Freis, D.; Cologna, M.

2018-03-01

Thorium-uranium oxide pellets with high densities were prepared at the Canadian Nuclear Laboratories (CNL) by co-milling, pressing, and sintering at 2023 K, with UO2 mass contents of 0, 1.5, 3, 8, 13, 30, 60 and 100%. At the Joint Research Centre, Karlsruhe (JRC-Karlsruhe), thorium-uranium oxide pellets were prepared using the spark plasma sintering (SPS) technique with 79 and 93 wt. % UO2. The thermal diffusivity of (Th1-xUx)O2 (0 ≤ x ≤ 1) was measured at CNL and at JRC-Karlsruhe using the laser flash technique. ThO2 and (Th,U)O2 with 1.5, 3, 8 and 13 wt. % UO2 were found to be semi-transparent to the infrared wavelength of the laser and were coated with graphite for the thermal diffusivity measurements. This semi-transparency decreased with the addition of UO2 and was lost at about 30 wt. % of UO2 in ThO2. The thermal conductivity was deduced using the measured density and literature data for the specific heat capacity. The thermal conductivity for ThO2 is significantly higher than for UO2. The thermal conductivity of (Th,U)O2 decreases rapidly with increasing UO2 content, and for UO2 contents of 60% and higher, the conductivity of the thorium-uranium oxide fuel is close to UO2. As the mass difference between the Th and U atoms is small, the thermal conductivity decrease is attributed to the phonon scattering enhanced by lattice strain due to the introduction of uranium in ThO2 lattice. The new results were compared to the data available in the literature and were evaluated using the classical phonon transport model for oxide systems.

Slave boson theory of orbital differentiation with crystal field effects: Application to UO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lanatà, Nicola; Yao, Yongxin; Deng, Xiaoyu

We derive an exact operatorial reformulation of the rotational invariant slave boson method, and we apply it to describe the orbital differentiation in strongly correlated electron systems starting from first principles. The approach enables us to treat strong electron correlations, spin-orbit coupling, and crystal field splittings on the same footing by exploiting the gauge invariance of the mean-field equations. Furthermore, we apply our theory to the archetypical nuclear fuel UO 2 and show that the ground state of this system displays a pronounced orbital differentiation within the 5f manifold, with Mott-localized Γ 8 and extended Γ 7 electrons.

Slave boson theory of orbital differentiation with crystal field effects: Application to UO 2

DOE PAGES

Lanatà, Nicola; Yao, Yongxin; Deng, Xiaoyu; ...

2017-03-23

We derive an exact operatorial reformulation of the rotational invariant slave boson method, and we apply it to describe the orbital differentiation in strongly correlated electron systems starting from first principles. The approach enables us to treat strong electron correlations, spin-orbit coupling, and crystal field splittings on the same footing by exploiting the gauge invariance of the mean-field equations. Furthermore, we apply our theory to the archetypical nuclear fuel UO 2 and show that the ground state of this system displays a pronounced orbital differentiation within the 5f manifold, with Mott-localized Γ 8 and extended Γ 7 electrons.

Slave Boson Theory of Orbital Differentiation with Crystal Field Effects: Application to UO_{2}.

PubMed

Lanatà, Nicola; Yao, Yongxin; Deng, Xiaoyu; Dobrosavljević, Vladimir; Kotliar, Gabriel

2017-03-24

We derive an exact operatorial reformulation of the rotational invariant slave boson method, and we apply it to describe the orbital differentiation in strongly correlated electron systems starting from first principles. The approach enables us to treat strong electron correlations, spin-orbit coupling, and crystal field splittings on the same footing by exploiting the gauge invariance of the mean-field equations. We apply our theory to the archetypical nuclear fuel UO_{2} and show that the ground state of this system displays a pronounced orbital differentiation within the 5f manifold, with Mott-localized Γ_{8} and extended Γ_{7} electrons.

The Development of Models to Optimize Selection of Nuclear Fuels through Atomic-Level Simulation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Prof. Simon Phillpot; Prof. Susan B. Sinnott; Prof. Hans Seifert

2009-01-26

Demonstrated that FRAPCON can be modified to accept data generated from first principles studies, and that the result obtained from the modified FRAPCON make sense in terms of the inputs. Determined the temperature dependence of the thermal conductivity of single crystal UO2 from atomistic simulation.

Design, fabrication, and testing of an external fuel (UO2), full-length thermionic converter

NASA Technical Reports Server (NTRS)

Schock, A.; Raab, B.

1971-01-01

The development of a full-length external-fuel thermionic converter for in-pile testing is described. The development program includes out-of-pile performance testing of the fully fueled-converter, using RF-induction heating, before its installation in the in-pile test capsule. The external-fuel converter is cylindrical in shape, and consists of an inner, centrally cooled collector, and an outer emitter surrounded by nuclear fuel. The term full-length denotes that the converter is long enough to extend over the full height of the reactor core. Thus, the converter is not a scaled-down test device, but a full-scale fuel element of the thermionic reactor. The external-fuel converter concept permits a number of different design options, particularly with respect to the fuel composition and shape, and the collector cooling arrangement. The converter described was developed for the Jet Propulsion Laboratory, and is based on their concept for a thermionic reactor with uninsulated collector cooling as previously described. The converter is double-ended, with through-flow cooling, and with ceramic seals and emitter and collector power take-offs at both ends. The design uses a revolver-shaped tungsten emitter body, with the central emitter hole surrounded by six peripheral fuel holes loaded with cylindrical UO2 pellets.

Energetics of metastudtite and implications for nuclear waste alteration

PubMed Central

Guo, Xiaofeng; Ushakov, Sergey V.; Labs, Sabrina; Curtius, Hildegard; Bosbach, Dirk; Navrotsky, Alexandra

2014-01-01

Metastudtite, (UO2)O2(H2O)2, is one of two known natural peroxide minerals, but little is established about its thermodynamic stability. In this work, its standard enthalpy of formation, −1,779.6 ± 1.9 kJ/mol, was obtained by high temperature oxide melt drop solution calorimetry. Decomposition of synthetic metastudtite was characterized by thermogravimetry and differential scanning calorimetry (DSC) with ex situ X-ray diffraction analysis. Four decomposition steps were observed in oxygen atmosphere: water loss around 220 °C associated with an endothermic heat effect accompanied by amorphization; another water loss from 400 °C to 530 °C; oxygen loss from amorphous UO3 to crystallize orthorhombic α-UO2.9; and reduction to crystalline U3O8. This detailed characterization allowed calculation of formation enthalpy from heat effects on decomposition measured by DSC and by transposed temperature drop calorimetry, and both these values agree with that from drop solution calorimetry. The data explain the irreversible transformation from studtite to metastudtite, the conditions under which metastudtite may form, and its significant role in the oxidation, corrosion, and dissolution of nuclear fuel in contact with water. PMID:25422465

Energetics of metastudtite and implications for nuclear waste alteration

DOE PAGES

Guo, Xiaofeng; Ushakov, Sergey V.; Labs, Sabrina; ...

2014-11-24

Metastudtite, (UO 2)O 2(H 2O) 2, is one of two known natural peroxide minerals, but little is established about its thermodynamic stability. In this work, its standard enthalpy of formation, $-$1,779.6 ± 1.9 kJ/mol, was obtained by high temperature oxide melt drop solution calorimetry. Decomposition of synthetic metastudtite was characterized by thermogravimetry and differential scanning calorimetry (DSC) with ex situ X-ray diffraction analysis. We observed four decomposition steps in oxygen atmosphere: water loss around 220 °C associated with an endothermic heat effect accompanied by amorphization; another water loss from 400 °C to 530 °C; oxygen loss from amorphous UO 3more » to crystallize orthorhombic α-UO 2.9; and reduction to crystalline U 3O 8. This detailed characterization allowed calculation of formation enthalpy from heat effects on decomposition measured by DSC and by transposed temperature drop calorimetry, and both these values agree with that from drop solution calorimetry. The data explain the irreversible transformation from studtite to metastudtite, the conditions under which metastudtite may form, and its significant role in the oxidation, corrosion, and dissolution of nuclear fuel in contact with water.« less

Molybdenum-UO2 cerment irradiation at 1145 K

NASA Technical Reports Server (NTRS)

Mcdonald, G.

1971-01-01

Two molybdenum-UO2 cermet fuel pins were fission heated in a helium-cooled loop at a temperature of 1145 K and to a total burnup of 5.3 % of the U-235. After irradiation the fuel pins were measured to check dimensional stability, punctured at the plenums to determine fission gas release, and examined metallographically to determine the effect of irradiation. Burnup was determined in several sections of the fuel pin. The results of the postirradiation examination indicated: (1) There was no visible change in the fuel pins on irradiation under the above conditions. (2) The maximum swelling of the fuel pins was less than 1%. (3) There was no migration of UO2 and no visible interaction between the molybdenum and the UO2. (4) Approximately 12% of the fission gas formed was released from the cermet cone into the gas plenum.

Mechanism for transient migration of xenon in UO{sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, X.-Y.; Uberuaga, B. P.; Andersson, D. A.

2011-04-11

In this letter, we report recent work on atomistic modeling of diffusion migration events of the fission gas product xenon in UO{sub 2} nuclear fuel. Under nonequilibrium conditions, Xe atoms can occupy the octahedral interstitial site, in contrast to the thermodynamically most stable uranium substitutional site. A transient migration mechanism involving Xe and two oxygen atoms is identified using basin constrained molecular dynamics employing a Buckingham type interatomic potential. This mechanism is then validated using density functional theory calculations using the nudged elastic band method. An overall reduction in the migration barrier of 1.6-2.7 eV is obtained compared to vacancy-mediatedmore » diffusion on the uranium sublattice.« less

A semi-empirical model for the formation and depletion of the high burnup structure in UO 2

DOE PAGES

Pizzocri, D.; Cappia, F.; Luzzi, L.; ...

2017-01-31

In the rim zone of UO 2 nuclear fuel pellets, the combination of high burnup and low temperature drives a microstructural change, leading to the formation of the high burnup structure (HBS). In this work, we propose a semi-empirical model to describe the formation of the HBS, which embraces the polygonisation/recrystallization process and the depletion of intra-granular fission gas, describing them as inherently related. To this end, we per-formed grain-size measurements on samples at radial positions in which the restructuring was incomplete. Moreover, based on these new experimental data, we assume an exponential reduction of the average grain size withmore » local effective burnup, paired with a simultaneous depletion of intra-granular fission gas driven by diffusion. The comparison with currently used models indicates the applicability of the herein developed model within integral fuel performance codes.« less

Simulation of radiation driven fission gas diffusion in UO 2, ThO 2 and PuO 2

DOE PAGES

Cooper, Michael William D.; Stanek, Christopher Richard; Turnbull, James Anthony; ...

2016-12-01

Below 1000 K it is thought that fission gas diffusion in nuclear fuel during irradiation occurs through atomic mixing due to radiation damage. Here we present a molecular dynamics (MD) study of Xe, Kr, Th, U, Pu and O diffusion due to irradiation. It is concluded that the ballistic phase does not sufficiently account for the experimentally observed diffusion. Thermal spike simulations are used to confirm that electronic stopping remedies the discrepancy with experiment and the predicted diffusivities lie within the scatter of the experimental data. Here, our results predict that the diffusion coefficients are ordered such that D* 0more » > D* Kr > D* Xe > D* U. For all species >98.5% of diffusivity is accounted for by electronic stopping. Fission gas diffusivity was not predicted to vary significantly between ThO 2, UO 2 and PuO 2, indicating that this process would not change greatly for mixed oxide fuels.« less

Fission products behaviour during a power transient: Their inventory in an intragranular bubble

NASA Astrophysics Data System (ADS)

Desgranges, L.; Blay, Th.; Lamontagne, J.; Roure, I.; Bienvenu, Ph.

2017-09-01

The behaviour of fission products is a key issue during Anticipated Operational Occurrences (AOOs) or Condition II transients or accidental sequence for nuclear fuel. Here we characterized how fission products behaved inside chromium doped UO2 pellet during a power ramp. At the pellet centre fission products have left the UO2 lattice and can be found in bubbles. The composition of the bubbles was determined using an original experimental methodology. The existence of separated precipitates made of metallic fission products for the one, and volatile fission products for the other, was evidenced. This result is discussed with regards to the behaviour of fission products during a power ramp.

Experimental evaluation of thermal ratcheting behavior in UO2 fuel elements

NASA Technical Reports Server (NTRS)

Phillips, W. M.

1973-01-01

The effects of thermal cycling of UO2 at high temperatures has been experimentally evaluated to determine the rates of distortion of UO2/clad fuel elements. Two capsules were rested in the 1500 C range, one with a 50 C thermal cycle, the other with a 100 C thermal cycle. It was observed that eight hours at the lower cycle temperature produced sufficient UO2 redistribution to cause clad distortion. The amount of distortion produced by the 100 C cycle was less than double that produced by the 50 C, indicating smaller thermal cycles would result in clad distortion. An incubation period was observed to occur before the onset of distortion with cycling similar to fuel swelling observed in-pile at these temperatures.

PROCESS OF MAKING A NEUTRONIC REACTOR FUEL ELEMENT COMPOSITION

DOEpatents

Alter, H.W.; Davidson, J.K.; Miller, R.S.; Mewherter, J.L.

1959-01-13

A process is presented for making a ceramic-like material suitable for use as a nuclear fuel. The material consists of a solid solution of plutonium dioxide in uranium dioxide and is produced from a uranyl nitrate -plutonium nitrate solution containing uraniunm and plutonium in the desired ratio. The uranium and plutonium are first precipitated from the solution by addition of NH/ sub 4/OH and the dried precipitate is then calcined at 600 C in a hydrogen atmosphere to yield the desired solid solution of PuO/sub 2/ in UO/sub 2/.

Study of phonons in irradiated epitaxial thin films of UO2

NASA Astrophysics Data System (ADS)

Rennie, S.; Lawrence Bright, E.; Darnbrough, J. E.; Paolasini, L.; Bosak, A.; Smith, A. D.; Mason, N.; Lander, G. H.; Springell, R.

2018-06-01

We report experiments to determine the effect of radiation damage on the phonon spectra of the most common nuclear fuel, UO2. We irradiated thin (˜300 nm) epitaxial films of UO2 with 2.1 MeV He2 + ions to 0.15 displacements per atom and a lattice swelling of Δ a /a ˜0.6 % and then used grazing-incidence inelastic x-ray scattering to measure the phonon spectrum. We succeeded in observing the acoustic modes, both transverse and longitudinal, across the Brillouin zone. The phonon energies, in both the pristine and irradiated samples, are unchanged from those observed in bulk material. On the other hand, the phonon linewidths (inversely proportional to the phonon lifetimes) show a significant broadening when comparing the pristine and irradiated samples. This effect is shown to increase with phonon energy across the Brillouin zone. The decreases in the phonon lifetimes of the acoustic modes are roughly consistent with a 50% reduction in the thermal conductivity.

Mini-MITEE: Ultra Small, Ultra Light NTP Engines for Robotic Science and Manned Exploration Missions

NASA Astrophysics Data System (ADS)

Powell, James; Maise, George; Paniagua, John

2006-01-01

A compact, ultra lightweight Nuclear Thermal Propulsion (NTP) engine design is described with the capability to carry out a wide range of unique and important robotic science missions that are not possible using chemical or Nuclear Electric Propulsion (NEP). The MITEE (MInature ReacTor EnginE) reactor uses hydrogeneous moderator, such as solid lithium-7 hydride, and high temperature cermet tungsten/UO2 nuclear fuel. The reactor is configured as a modular pressure tube assembly, with each pressure tube containing an outer annual shell of moderator with an inner annular region of W/UO2 cermet fuel sheets. H2 propellant flows radially inwards through the moderator and fuel regions, exiting at ~3000 K into a central channel that leads to a nozzle at the end of the pressure tube. Power density in the fuel region is 10 to 20 megawatts per liter, depending on design, producing a thrust output on the order of 15,000 Newtons and an Isp of ~1000 seconds. 3D Monte Carlo neutronic analyses are described for MITEE reactors utilizing various fissile fuel options (U-235, U-233, and Am242m) and moderators (7LiH and BeH2). Reactor mass ranges from a maximum of 100 kg for the 7LiH/U-235 option to a minimum of 28 kg for the BeH2/Am-242 m option. Pure thrust only and bi-modal (thrust plus electric power generation) MITEE designs are described. Potential unique robotic science missions enabled by the MITEE engine are described, including landing on Europa and exploring the ice sheet interior with return of samples to Earth, hopping to and exploring multiple sites on Mars, unlimited ramjet flight in the atmospheres of Jupiter, Saturn, Uranus, and Neptune and landing on, and sample return from Pluto.

Mini-MITEE: Ultra Small, Ultra Light NTP Engines for Robotic Science and Manned Exploration Missions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Powell, James; Maise, George; Paniagua, John

2006-01-20

A compact, ultra lightweight Nuclear Thermal Propulsion (NTP) engine design is described with the capability to carry out a wide range of unique and important robotic science missions that are not possible using chemical or Nuclear Electric Propulsion (NEP). The MITEE (MInature ReacTor EnginE) reactor uses hydrogeneous moderator, such as solid lithium-7 hydride, and high temperature cermet tungsten/UO2 nuclear fuel. The reactor is configured as a modular pressure tube assembly, with each pressure tube containing an outer annual shell of moderator with an inner annular region of W/UO2 cermet fuel sheets. H2 propellant flows radially inwards through the moderator andmore » fuel regions, exiting at {approx}3000 K into a central channel that leads to a nozzle at the end of the pressure tube. Power density in the fuel region is 10 to 20 megawatts per liter, depending on design, producing a thrust output on the order of 15,000 Newtons and an Isp of {approx}1000 seconds. 3D Monte Carlo neutronic analyses are described for MITEE reactors utilizing various fissile fuel options (U-235, U-233, and Am242m) and moderators (7LiH and BeH2). Reactor mass ranges from a maximum of 100 kg for the 7LiH/U-235 option to a minimum of 28 kg for the BeH2/Am-242 m option. Pure thrust only and bi-modal (thrust plus electric power generation) MITEE designs are described. Potential unique robotic science missions enabled by the MITEE engine are described, including landing on Europa and exploring the ice sheet interior with return of samples to Earth, hopping to and exploring multiple sites on Mars, unlimited ramjet flight in the atmospheres of Jupiter, Saturn, Uranus, and Neptune and landing on, and sample return from Pluto.« less

Amoeba behavior of UO/sub 2/ coated particle fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wagner-Loeffler, M.

1977-09-01

The data extracted from numerous irradiation tests were used to derive amoeba endurance parameters for UO/sub 2/. The data do not yet allow an unambiguous definition of the controlling mechanism, which may be due to either gaseous or solid-state diffusion processes. Adequate data on the amoeba effect are available for design of a steam-raising high-temperature gas-cooled reactor using UO/sub 2/ fuel.

PRELIMINARY EVALUATION OF FeCrAl CLADDING AND U-Si FUEL FOR ACCIDENT TOLERANT FUEL CONCEPTS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hales, J. D.; Gamble, K. A.

2015-09-01

Since the accident at the Fukushima Daiichi Nuclear Power Station, enhancing the accident tolerance of light water reactors (LWRs) has become an important research topic. In particular, the community is actively developing enhanced fuels and cladding for LWRs to improve safety in the event of accidents in the reactor or spent fuel pools. Fuels with enhanced accident tolerance are those that, in comparison with the standard UO2-zirconium alloy system, can tolerate loss of active cooling in the reactor core for a considerably longer time period during design-basis and beyond design-basis events while maintaining or improving the fuel performance during normalmore » operations and operational transients. This paper presents early work in developing thermal and mechanical models for two materials that may have promise: U-Si for fuel, and FeCrAl for cladding. These materials would not necessarily be used together in the same fuel system, but individually have promising characteristics. BISON, the finite element-based fuel performance code in development at Idaho National Laboratory, was used to compare results from normal operation conditions with Zr-4/UO2 behavior. In addition, sensitivity studies are presented for evaluating the relative importance of material parameters such as ductility and thermal conductivity in FeCrAl and U-Si in order to provide guidance on future experiments for these materials.« less

Nuclear Energy Advanced Modeling and Simulation (NEAMS) Accident Tolerant Fuels High Impact Problem: Coordinate Multiscale U 3Si 2 Modeling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gamble, K. A.; Hales, J. D.; Miao, Y.

Since the events at the Fukushima-Daiichi nuclear power plant in March 2011 significant research has unfolded at national laboratories, universities and other institutions into alternative materials that have potential enhanced accident tolerance when compared to traditional \\uo~fuel zircaloy clad fuel rods. One of the potential replacement fuels is uranium silicide (\\usi) for its higher thermal conductivity and uranium density. The lower melting temperature is of potential concern during postulated accident conditions. Another disadvantage for \\usi~ is the lack of experimental data under power reactor conditions. Due to the aggressive development schedule for inserting some of the potential materials into leadmore » test assemblies or rods by 2022~\\cite{bragg-sitton_2014} multiscale multiphysics modeling approaches have been used to provide insight into these materials. \\\\ \

Nanoparticle Precipitation in Irradiated and Annealed Ceria Doped with Metals for Emulation of Spent Fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jiang, Weilin; Conroy, Michele A.; Kruska, Karen

Epsilon alloy precipitates have been observed with varied compositions and sizes in spent nuclear fuels, such as UO2. Presence of the inclusions, along with other oxide precipitates, gas bubbles and irradiation-induced structural defects, can significantly degrade the physical properties of the fuel. To predict fuel performance, a fundamental study of the precipitation processes is needed. This study uses ceria (CeO2) as a surrogate for UO2. Polycrystalline CeO2 films doped with Mo, Ru, Rh, Pd and Re (surrogate for Tc) were grown at 823 K using pulsed laser deposition, irradiated at 673 K with He+ ions, and subsequently annealed at highermore » temperatures. A number of methods, including transmission electron microscopy and atom probe tomography, were applied to characterize the samples. The results indicate that there is a uniform distribution of the doped metals in the as-grown CeO2 film. Pd particles of ~3 nm in size appear near dislocation edges after He+ ion irradiation to ~13 dpa. Thermal annealing at 1073 K in air leads to formation of precipitates with Mo and Pd around grain boundaries. Further annealing at 1373 K produces 70 nm sized precipitates with small grains at cavities.« less

Proliferation resistance of small modular reactors fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Polidoro, F.; Parozzi, F.; Fassnacht, F.

2013-07-01

In this paper the proliferation resistance of different types of Small Modular Reactors (SMRs) has been examined and classified with criteria available in the literature. In the first part of the study, the level of proliferation attractiveness of traditional low-enriched UO{sub 2} and MOX fuels to be used in SMRs based on pressurized water technology has been analyzed. On the basis of numerical simulations both cores show significant proliferation risks. Although the MOX core is less proliferation prone in comparison to the UO{sub 2} core, it still can be highly attractive for diversion or undeclared production of nuclear material. Inmore » the second part of the paper, calculations to assess the proliferation attractiveness of fuel in typical small sodium cooled fast reactor show that proliferation risks from spent fuel cannot be neglected. The core contains a highly attractive plutonium composition during the whole life cycle. Despite some aspects of the design like the sealed core that enables easy detection of unauthorized withdrawal of fissile material and enhances proliferation resistance, in case of open Non-Proliferation Treaty break-out, weapon-grade plutonium in sufficient quantities could be extracted from the reactor core.« less

Investigations of ion-irradiated uranium dioxide nuclear fuel with laser-assisted atom probe tomography

NASA Astrophysics Data System (ADS)

Valderrama, Billy

Performance in commercial light water reactors is dictated by the ability of its fuel material, uranium dioxide (UO2), to transport heat generated during the fission process. It is widely known that the service lifetime is limited by irradiation-induced microstructural changes that degrade the thermal performance of UO2. Studying the role of complex, often interacting mechanisms that occur during the early stages of microstructural evolution presents a challenge. Phenomena of particular interest are the segregation of fission products to form bubbles and their resultant effect on grain boundary (GB) mobility, and the effect of irradiation on fuel stoichiometry. Each mechanism has a profound consequence on fuel thermal conductivity. Several advanced analytical techniques, such as transmission electron microscopy, x-ray diffraction, x-ray photoelectron spectroscopy, etc. have been used to study these mechanisms. However, they each have limitations and cannot individually provide the necessary information for deeper understanding. One technique that has been under utilized is atom probe tomography (APT), which has a unique ability to spatially resolve small-scale chemical variations. APT uses the principle of field ionization to evaporate surface ions for chemical analysis. For low electrical conductivity systems, a pulsed laser is used to thermally assist in the evaporation process. One factor complicating the analysis is that laser-material interactions are poorly understood for oxide materials and literature using this technique with UO2 is lacking. Therefore, an initial systematic study to identify the optimal conditions for the analysis of UO2 using laser-assisted APT was conducted. A comparative study on the evaporation behavior between CeO2 and UO2 was followed. CeO2 was chosen due to its technological relevancy and availability of comparative studies with laser-assisted APT. Dissimilar evaporation behavior between these materials was identified and attributed to differences in laser absorption, oxide stability, and thermal conductivity between the two materials. After the conditions were identified, APT was utilized to study the role of temperature and GB structure on the segregation of Kr. Results indicate that high angle GBs contain more Kr relative to low angle GBs. The methodology presented can be applied to investigate small-scale chemical changes in other oxide materials.

High Pressure Low Temperature X-Ray Diffraction Studies of UO2 and UN single crystals.

NASA Astrophysics Data System (ADS)

Antonio, Daniel; Mast, Daniel; Lavina, Barbara; Gofryk, Krzysztof

Uranium dioxide is the most commonly used nuclear fuel material in commercial reactors, while uranium nitride also has many thermal and physical properties that make it attractive for potential use in reactors. Both have a cubic fcc lattice structure at ambient conditions and transition to antiferromagnetic order at low temperature. UO2 is a Mott insulator that orders in a complex non-collinear 3k magnetic structure at about 30 K, while UN has appreciable conductivity and orders in a simpler 1k magnetic structure below 52 K. Both compounds are characterized by strong magneto-structural interactions, understanding of which is vital for modeling their thermo-physical properties. While UO2 and UN have been extensively studied at and above room temperature, little work has been done to directly study the structure of these materials at low temperatures where magnetic interactions are dominant. In the course of our systematic studies on magneto vibrational behavior of UO2 and UN, here we present our recent results of high pressure X-Ray Diffraction (up to 35 GPa) measured below the Neel temperature using synchrotron radiation. Work supported by the Department of Energy, Office of Basic Energy Sciences, Materials Sciences, and Engineering Division.

Further observations on OCOM MOX fuel: microstructure in the vicinity of the pellet rim and fuel — cladding interaction

NASA Astrophysics Data System (ADS)

Walker, C. T.; Goll, W.; Matsumura, T.

1997-06-01

The fuel investigated was manufactured by Siemens-KWU and irradiated at low rating in the KWO reactor in Germany. The MOX agglomerates in the cold outer region of the fuel shared several common features with the high burn-up structure at the rim of UO 2 fuel. It is proposed that in both cases the mechanism producing the microstructure change is recrystallisation. Further, it is shown that surface MOX agglomerates do not noticeably retard cladding creepdown although they swell into the gap. The contracting cladding appears able to push the agglomerates back into the fuel. The thickness of the oxide layer on the inner cladding surface increased at points where contact with surface MOX agglomerates had occurred. Despite this, the mean thickness of the oxide did not differ significantly from that found in UO 2 fuel rods of like design. It is judged that the high burn-up structure will form in the UO 2 matrix when the local burn-up there reaches 60 to 80 GWd/tM. Limiting the MOX scrap addition in the UO 2 matrix will delay its formation.

AGR-2 Irradiation Test Final As-Run Report, Rev 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Collin, Blaise P.

2014-08-01

This document presents the as-run analysis of the AGR-2 irradiation experiment. AGR-2 is the second of the planned irradiations for the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program. Funding for this program is provided by the U.S. Department of Energy as part of the Very High Temperature Reactor (VHTR) Technical Development Office (TDO) program. The objectives of the AGR-2 experiment are to: (a) Irradiate UCO (uranium oxycarbide) and UO 2 (uranium dioxide) fuel produced in a large coater. Fuel attributes are based on results obtained from the AGR-1 test and other project activities. (b) Provide irradiated fuel samplesmore » for post-irradiation experiment (PIE) and safety testing. (c) Support the development of an understanding of the relationship between fuel fabrication processes, fuel product properties, and irradiation performance. The primary objective of the test was to irradiate both UCO and UO 2 TRISO (tri-structural isotropic) fuel produced from prototypic scale equipment to obtain normal operation and accident condition fuel performance data. The UCO compacts were subjected to a range of burnups and temperatures typical of anticipated prismatic reactor service conditions in three capsules. The test train also includes compacts containing UO 2 particles produced independently by the United States, South Africa, and France in three separate capsules. The range of burnups and temperatures in these capsules were typical of anticipated pebble bed reactor service conditions. The results discussed in this report pertain only to U.S. produced fuel. In order to achieve the test objectives, the AGR-2 experiment was irradiated in the B-12 position of the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) for a total irradiation duration of 559.2 effective full power days (EFPD). Irradiation began on June 22, 2010, and ended on October 16, 2013, spanning 12 ATR power cycles and approximately three and a half calendar years. The test contained six independently controlled and monitored capsules. Each U.S. capsule contained 12 compacts of either UCO or UO2 AGR coated fuel. No fuel particles failed during the AGR-2 irradiation. Final burnup values on a per compact basis ranged from 7.26 to 13.15% FIMA (fissions per initial heavy-metal atom) for UCO fuel, and 9.01 to 10.69% FIMA for UO 2 fuel, while fast fluence values ranged from 1.94 to 3.47 x 10 25 n/m 2 (E >0.18 MeV) for UCO fuel, and from 3.05 to 3.53 x 10 25 n/m 2 (E >0.18 MeV) for UO 2 fuel. Time-average volume-average (TAVA) temperatures on a capsule basis at the end of irradiation ranged from 987°C in Capsule 6 to 1296°C in Capsule 2 for UCO, and from 996 to 1062°C in UO 2-fueled Capsule 3. By the end of the irradiation, all of the installed thermocouples (TCs) had failed. Fission product release-to-birth (R/B) ratios were quite low. In the UCO capsules, R/B values during the first three cycles were below 10 -6 with the exception of the hotter Capsule 2, in which the R/Bs reached 2 x 10 -6. In the UO 2 capsule (Capsule 3), the R/B values during the first three cycles were below 10 -7. R/B values for all following cycles are not reliable due to gas flow and cross talk issues.« less

Safety Criticality Standards Using the French CRISTAL Code Package: Application to the AREVA NP UO{sub 2} Fuel Fabrication Plant

DOE Office of Scientific and Technical Information (OSTI.GOV)

Doucet, M.; Durant Terrasson, L.; Mouton, J.

2006-07-01

Criticality safety evaluations implement requirements to proof of sufficient sub critical margins outside of the reactor environment for example in fuel fabrication plants. Basic criticality data (i.e., criticality standards) are used in the determination of sub critical margins for all processes involving plutonium or enriched uranium. There are several criticality international standards, e.g., ARH-600, which is one the US nuclear industry relies on. The French Nuclear Safety Authority (DGSNR and its advising body IRSN) has requested AREVA NP to review the criticality standards used for the evaluation of its Low Enriched Uranium fuel fabrication plants with CRISTAL V0, the recentlymore » updated French criticality evaluation package. Criticality safety is a concern for every phase of the fabrication process including UF{sub 6} cylinder storage, UF{sub 6}-UO{sub 2} conversion, powder storage, pelletizing, rod loading, assembly fabrication, and assembly transportation. Until 2003, the accepted criticality standards were based on the French CEA work performed in the late seventies with the APOLLO1 cell/assembly computer code. APOLLO1 is a spectral code, used for evaluating the basic characteristics of fuel assemblies for reactor physics applications, which has been enhanced to perform criticality safety calculations. Throughout the years, CRISTAL, starting with APOLLO1 and MORET 3 (a 3D Monte Carlo code), has been improved to account for the growth of its qualification database and for increasing user requirements. Today, CRISTAL V0 is an up-to-date computational tool incorporating a modern basic microscopic cross section set based on JEF2.2 and the comprehensive APOLLO2 and MORET 4 codes. APOLLO2 is well suited for criticality standards calculations as it includes a sophisticated self shielding approach, a P{sub ij} flux determination, and a 1D transport (S{sub n}) process. CRISTAL V0 is the result of more than five years of development work focusing on theoretical approaches and the implementation of user-friendly graphical interfaces. Due to its comprehensive physical simulation and thanks to its broad qualification database with more than a thousand benchmark/calculation comparisons, CRISTAL V0 provides outstanding and reliable accuracy for criticality evaluations for configurations covering the entire fuel cycle (i.e. from enrichment, pellet/assembly fabrication, transportation, to fuel reprocessing). After a brief description of the calculation scheme and the physics algorithms used in this code package, results for the various fissile media encountered in a UO{sub 2} fuel fabrication plant will be detailed and discussed. (authors)« less

Diffusion of oxygen interstitials in UO2+x using kinetic Monte Carlo simulations: Role of O/M ratio and sensitivity analysis

NASA Astrophysics Data System (ADS)

Behera, Rakesh K.; Watanabe, Taku; Andersson, David A.; Uberuaga, Blas P.; Deo, Chaitanya S.

2016-04-01

Oxygen interstitials in UO2+x significantly affect the thermophysical properties and microstructural evolution of the oxide nuclear fuel. In hyperstoichiometric Urania (UO2+x), these oxygen interstitials form different types of defect clusters, which have different migration behavior. In this study we have used kinetic Monte Carlo (kMC) to evaluate diffusivities of oxygen interstitials accounting for mono- and di-interstitial clusters. Our results indicate that the predicted diffusivities increase significantly at higher non-stoichiometry (x > 0.01) for di-interstitial clusters compared to a mono-interstitial only model. The diffusivities calculated at higher temperatures compare better with experimental values than at lower temperatures (< 973 K). We have discussed the resulting activation energies achieved for diffusion with all the mono- and di-interstitial models. We have carefully performed sensitivity analysis to estimate the effect of input di-interstitial binding energies on the predicted diffusivities and activation energies. While this article only discusses mono- and di-interstitials in evaluating oxygen diffusion response in UO2+x, future improvements to the model will primarily focus on including energetic definitions of larger stable interstitial clusters reported in the literature. The addition of larger clusters to the kMC model is expected to improve the comparison of oxygen transport in UO2+x with experiment.

Uncertainty analysis on reactivity and discharged inventory for a pressurized water reactor fuel assembly due to {sup 235,238}U nuclear data uncertainties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Da Cruz, D. F.; Rochman, D.; Koning, A. J.

2012-07-01

This paper discusses the uncertainty analysis on reactivity and inventory for a typical PWR fuel element as a result of uncertainties in {sup 235,238}U nuclear data. A typical Westinghouse 3-loop fuel assembly fuelled with UO{sub 2} fuel with 4.8% enrichment has been selected. The Total Monte-Carlo method has been applied using the deterministic transport code DRAGON. This code allows the generation of the few-groups nuclear data libraries by directly using data contained in the nuclear data evaluation files. The nuclear data used in this study is from the JEFF3.1 evaluation, and the nuclear data files for {sup 238}U and {supmore » 235}U (randomized for the generation of the various DRAGON libraries) are taken from the nuclear data library TENDL. The total uncertainty (obtained by randomizing all {sup 238}U and {sup 235}U nuclear data in the ENDF files) on the reactor parameters has been split into different components (different nuclear reaction channels). Results show that the TMC method in combination with a deterministic transport code constitutes a powerful tool for performing uncertainty and sensitivity analysis of reactor physics parameters. (authors)« less

Spent nuclear fuel/water interface behavior: Alpha dose rate profile determination for model surfaces and microcracks by using Monte-Carlo methods

NASA Astrophysics Data System (ADS)

Tribet, M.; Mougnaud, S.; Jégou, C.

2017-05-01

This work aims to better understand the nature and evolution of energy deposits at the UO2/water reactional interface subjected to alpha irradiation, through an original approach based on Monte-Carlo-type simulations, using the MCNPX code. Such an approach has the advantage of describing the energy deposit profiles on both sides of the interface (UO2 and water). The calculations have been performed on simple geometries, with data from an irradiated UOX fuel (burnup of 47 GWd.tHM-1 and 15 years of alpha decay). The influence of geometric parameters such as the diameter and the calculation steps at the reactional interface are discussed, and the exponential laws to be used in practice are suggested. The case of cracks with various different apertures (from 5 to 35 μm) has also been examined and these calculations have also enabled new information on the mean range of radiolytic species in cracks, and thus on the local chemistry.

CHEMICAL ENGINEERING DIVISION SUMMARY REPORT, OCTOBER, NOVEMBER, DECEMBER 1960

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

1961-03-01

Chemical-metallurgical processing studies were made of pyrometallurgical development snd research, and fuel processing facilities for EBR-II. Fuel-cycle applications of fluidization and volatility techniques included laboratory investigations of fluoride volatility processes, engineeringscale development, and conversion of UF/sub 6/ to UO/sub 2/. Reactor safety studies consisted of metal oxidation and ignition kinetics, and metal-water reactions. Reactor chemistry investigations were conducted to determine nuclear constants and suitable reactor decontamination methods. Routine operations are summarized for the high-level gammairradiation facillty and waste processing. (B.O.G.)

Numerical characterization of micro-cell UO2sbnd Mo pellet for enhanced thermal performance

NASA Astrophysics Data System (ADS)

Lee, Heung Soo; Kim, Dong-Joo; Kim, Sun Woo; Yang, Jae Ho; Koo, Yang-Hyun; Kim, Dong Rip

2016-08-01

Metallic micro-cell UO2 pellet with high thermal conductivity has received attention as a promising accident-tolerant fuel. Although experimental demonstrations have been successful, studies on the potency of current metallic micro-cell UO2 fuels for further enhancement of thermal performance are lacking. Here, we numerically investigated the thermal conductivities of micro-cell UO2sbnd Mo pellets in terms of the amount of Mo content, the unit cell size, and the aspect ratio of the micro-cells. The results showed good agreement with experimental measurements, and more importantly, indicated the importance of optimizing the unit cell geometries of the micro-cell pellets for greater increases in thermal conductivity. Consequently, the micro-cell UO2sbnd Mo pellets (5 vol% Mo) with modified geometries increased the thermal conductivity of the current UO2 pellets by about 2.5 times, and lowered the temperature gradient within the pellets by 62.9% under a linear heat generation rate of 200 W/cm.

Implementation and evaluation of fuel creep using advanced light-water reactor materials in FRAPCON 3.5

NASA Astrophysics Data System (ADS)

Carroll, Spencer

As current reactors approach the end of their operable lifetime, new reactors are needed if nuclear power is to continue being generated in the United States. Some utilities have already began construction on newer, more advanced LWR reactors, which use the same fuel as current reactors and have a similar but updated design. Others are researching next generation (GEN-IV) reactors which have new designs that utilize alternative fuel, coolants and other reactor materials. Many of these alternative fuels are capable of achieving higher burnups and are designed to be more accident tolerant than the currently used UO2 fuel. However, before these new materials can be used, extensive research must be done in order to obtain a detailed understanding of how the new fuels and other materials will interact. New fuels, such as uranium nitride (UN) and uranium carbide (UC) have several advantages over UO2, such as increased burnup capabilities and higher thermal conductivities. However, there are issues with each that prevent UC and UN from being used as direct replacements for UO2. Both UC and UN swell at a significantly higher rate than UO2 and neither fuel reacts favorably when exposed to water. Due to this, UC and UN are being considered more for GEN-IV reactors that use alternative coolant rather than for current LWRs. In an effort to increase accident tolerance, silicon carbide (SiC) is being considered for use as an alternative cladding. The high strength, high melting point and low oxidation of SiC make it an attractive cladding choice, especially in an accident scenario. However, as a ceramic, SiC is not ductile and will not creep outwards upon pellet-clad mechanical interaction (PCMI) which can cause a large build up in interfacial pressure. In order to understand the interaction between the high swelling fuels and unyielding SiC cladding, data on the properties and behaviors of these materials must be gathered and incorporated into FRAPCON. FRAPCON is a fuel performance code developed by PNNL and used by the Nuclear Regulatory Commission (NRC) as a licensing code for US reactors. FRAPCON will give insight into how these new fuel-cladding combinations will affect cladding hoop stress and help determine if the new materials are feasible for use in a reactor. To accurately simulate the interaction between the new materials, a soft pellet model that allows for stresses on the pellet to affect pellet deformation will have to be implemented. Currently, FRAPCON uses a rigid pellet model that does not allow for feedback of the cladding onto the pellet. Since SiC does not creep at the temperatures being considered and is not ductile, any PCMI create a much higher interfacial pressure than is possible with Zircaloy. Because of this, it is necessary to implement a model that allows for pellet creep to alleviate some of these cladding stresses. These results will then be compared to FEMAXI-6, a Japanese fuel performance code that already calculates pellet stress and allows for cladding feedback onto the pellet. This research is intended to be a continuation and verification of previous work done by USC on the analysis of accident tolerant fuels with alternative claddings and is intended to prove that a soft pellet model is necessary to accurately model any fuel with SiC cladding.

Evaluation of refractory-metal-clad uranium nitride and uranium dioxide fuel pins after irradiation for times up to 10 450 hours at 990 C

NASA Technical Reports Server (NTRS)

Bowles, K. J.; Gluyas, R. E.

1975-01-01

The effects of some materials variables on the irradiation performance of fuel pins for a lithium-cooled space power reactor design concept were examined. The variables studied were UN fuel density, fuel composition, and cladding alloy. All pins were irradiated at about 990 C in a thermal neutron environment to the design fuel burnup. An 85-percent dense UN fuel gave the best overall results in meeting the operational goals. The T-111 cladding on all specimens was embrittled, possibly by hydrogen in the case of the UN fuel and by uranium and oxygen in the case of the UO2 fuel. Tests with Cb-1Zr cladding indicate potential use of this cladding material. The UO2 fueled specimens met the operational goals of less than 1 percent cladding strain, but other factors make UO2 less attractive than low-density UN for the contemplated space power reactor use.

Critical Safe Disposal of Spent Fuel: Behavior of Neutron Poisons

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kienzler, Bernhard; Gmal, Bernhard

2007-07-01

In contrast to Yucca Mountain, European repository concepts rely on deep underground conditions which guarantee permanently a reducing geochemical environment. As long as no water comes into contact with the disposed nuclear fuel, criticality is excluded by compliance with the disposal conditions (limitation of U/Pu in the canisters). Penetration of water into the canister may also be considered as a scenario. However, water in a disposal results in geochemical reactions proceeding over very long periods of time: (1) Presence of water allows the corrosion of the steel of the canister material forming hydrogen and iron corrosion products. (2) Hydrogen pressuresmore » affect the zircaloy cladding even at low temperatures. Failure of fuel cladding and spacers leads to changes in the geometrical configuration. (3) UO{sub 2} matrix corrosion results in geochemically controlled reformation of secondary phase. (4) Even if the dissolution rate of UO{sub 2} is low, elements accounting for burnup credit do not behave similar as uranium. Geochemical reactions are analyzed in detail and compositions are presented which have a high probability to be formed in the long-term needing to be analyzed with respect to K{sub eff}. (authors)« less

Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling

DOE PAGES

Burns, Jonathan D.; Moyer, Bruce A.

2016-08-17

Hexavalent Np, Pu, and Am individually, and as a group, have all been cocrystallized with UO 2(NO 3) 2∙ 6H 2O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO 2(NO 3) 2∙ 6H 2O in near proportion with a simple reduction in temperature, while the lower valence states, An(III) and An(IV), are only slightly removed from solution. A separation of An(VI) species from An(III) ions by crystallization has been demonstrated, with an observed separation factor of 14. Separation of An(VI) species from key fission products, 95Zr,more » 95Nb, 137Cs, and 144Ce, has also been demonstrated by crystallization, with separation factors ranging from 6.5 to 71 in the absence of Am(VI), while in the presence of Am(VI), the separation factors were reduced to 0.99 7.7. One interesting observation is that Am(VI) shows increased stability in the cocrystallized form, with no reduction observed after 13 days, as opposed to in solution, in which >50% is reduced after only 10 days. The ability to cocrystallize and stabilize hexavalent actinides from solution, especially Am(VI), introduces a new separations approach that can be applied to closing the nuclear fuel cycle.« less

Group Hexavalent Actinide Separations: A New Approach to Used Nuclear Fuel Recycling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Burns, Jonathan D.; Moyer, Bruce A.

Hexavalent Np, Pu, and Am individually, and as a group, have all been cocrystallized with UO 2(NO 3) 2∙ 6H 2O, constituting the first demonstration of an An(VI) group cocrystalliza- tion. The hexavalent dioxo cations of Np, Pu, and Am cocrystallize with UO 2(NO 3) 2∙ 6H 2O in near proportion with a simple reduction in temperature, while the lower valence states, An(III) and An(IV), are only slightly removed from solution. A separation of An(VI) species from An(III) ions by crystallization has been demonstrated, with an observed separation factor of 14. Separation of An(VI) species from key fission products, 95Zr,more » 95Nb, 137Cs, and 144Ce, has also been demonstrated by crystallization, with separation factors ranging from 6.5 to 71 in the absence of Am(VI), while in the presence of Am(VI), the separation factors were reduced to 0.99 7.7. One interesting observation is that Am(VI) shows increased stability in the cocrystallized form, with no reduction observed after 13 days, as opposed to in solution, in which >50% is reduced after only 10 days. The ability to cocrystallize and stabilize hexavalent actinides from solution, especially Am(VI), introduces a new separations approach that can be applied to closing the nuclear fuel cycle.« less

Uranium extraction from TRISO-coated fuel particles using supercritical CO2 containing tri-n-butyl phosphate.

PubMed

Zhu, Liyang; Duan, Wuhua; Xu, Jingming; Zhu, Yongjun

2012-11-30

High-temperature gas-cooled reactors (HTGRs) are advanced nuclear systems that will receive heavy use in the future. It is important to develop spent nuclear fuel reprocessing technologies for HTGR. A new method for recovering uranium from tristructural-isotropic (TRISO-) coated fuel particles with supercritical CO(2) containing tri-n-butyl phosphate (TBP) as a complexing agent was investigated. TRISO-coated fuel particles from HTGR fuel elements were first crushed to expose UO(2) pellet fuel kernels. The crushed TRISO-coated fuel particles were then treated under O(2) stream at 750°C, resulting in a mixture of U(3)O(8) powder and SiC shells. The conversion of U(3)O(8) into solid uranyl nitrate by its reaction with liquid N(2)O(4) in the presence of a small amount of water was carried out. Complete conversion was achieved after 60 min of reaction at 80°C, whereas the SiC shells were not converted by N(2)O(4). Uranyl nitrate in the converted mixture was extracted with supercritical CO(2) containing TBP. The cumulative extraction efficiency was above 98% after 20 min of online extraction at 50°C and 25 MPa, whereas the SiC shells were not extracted by TBP. The results suggest an attractive strategy for reprocessing spent nuclear fuel from HTGR to minimize the generation of secondary radioactive waste. Copyright © 2012 Elsevier B.V. All rights reserved.

Preliminary assessment of accident-tolerant fuels on LWR performance during normal operation and under DB and BDB accident conditions

NASA Astrophysics Data System (ADS)

Ott, L. J.; Robb, K. R.; Wang, D.

2014-05-01

Following the severe accidents at the Japanese Fukushima Daiichi Nuclear Power Station in 2011, the US Department of Energy initiated research and development on the enhancement of the accident tolerance of light water reactors by the development of fuels/cladding that, in comparison with the standard UO2/Zircaloy (Zr) system, can tolerate loss of active cooling in the core for a considerably longer time period while maintaining or improving the fuel performance during normal operations. Analyses are presented that illustrate the impact of these new candidate fuel/cladding materials on the fuel performance at normal operating conditions and on the reactor system under DB and BDB accident conditions.

Design Study of Modular Nuclear Power Plant with Small Long Life Gas Cooled Fast Reactors Utilizing MOX Fuel

NASA Astrophysics Data System (ADS)

Ilham, Muhammad; Su'ud, Zaki

2017-01-01

Growing energy needed due to increasing of the world’s population encourages development of technology and science of nuclear power plant in its safety and security. In this research, it will be explained about design study of modular fast reactor with helium gas cooling (GCFR) small long life reactor, which can be operated over 20 years. It had been conducted about neutronic design GCFR with Mixed Oxide (UO2-PuO2) fuel in range of 100-200 MWth NPPs of power and 50-60% of fuel fraction variation with cylindrical pin cell and cylindrical balance of reactor core geometry. Calculation method used SRAC-CITATION code. The obtained results are the effective multiplication factor and density value of core reactor power (with geometry optimalization) to obtain optimum design core reactor power, whereas the obtained of optimum core reactor power is 200 MWth with 55% of fuel fraction and 9-13% of percentages.

Separation of uranium from technetium in recovery of spent nuclear fuel

NASA Astrophysics Data System (ADS)

Friedman, H. A.

1984-06-01

A method for decontaminating uranium product from the Purex 5 process is described. Hydrazine is added to the product uranyl nitrate stream from the Purex process, which contains hexavalent (UO2(2+)) uranium and heptavalent technetius (TcO4-). Technetium in the product stream is reduced and then complexed by the addition of oxalic acid (H2O2O4), and the Tc-oxalate complex is readily separated from the 10 uranium by solvent extraction with 30 vol % tributyl phosphate in n-dodecane.

Uranium dioxide electrolysis

DOEpatents

Willit, James L [Batavia, IL; Ackerman, John P [Prescott, AZ; Williamson, Mark A [Naperville, IL

2009-12-29

This is a single stage process for treating spent nuclear fuel from light water reactors. The spent nuclear fuel, uranium oxide, UO.sub.2, is added to a solution of UCl.sub.4 dissolved in molten LiCl. A carbon anode and a metallic cathode is positioned in the molten salt bath. A power source is connected to the electrodes and a voltage greater than or equal to 1.3 volts is applied to the bath. At the anode, the carbon is oxidized to form carbon dioxide and uranium chloride. At the cathode, uranium is electroplated. The uranium chloride at the cathode reacts with more uranium oxide to continue the reaction. The process may also be used with other transuranic oxides and rare earth metal oxides.

Thermal property change of MOX and UO2 irradiated up to high burnup of 74 GWd/t

NASA Astrophysics Data System (ADS)

Nakae, Nobuo; Akiyama, Hidetoshi; Miura, Hiromichi; Baba, Toshikazu; Kamimura, Katsuichiro; Kurematsu, Shigeru; Kosaka, Yuji; Yoshino, Aya; Kitagawa, Takaaki

2013-09-01

Thermal property is important because it controls fuel behavior under irradiation. The thermal property change at high burnup of more than 70 GWd/t is examined. Two kinds of MOX fuel rods, which were fabricated by MIMAS and SBR methods, and one referenced UO2 fuel rod were used in the experiment. These rods were taken from the pre-irradiated rods (IFA 609/626, of which irradiation test were carried out by Japanese PWR group) and re-fabricated and re-irradiated in HBWR as IFA 702 by JNES. The specification of fuel corresponds to that of 17 × 17 PWR type fuel and the axially averaged linear heat rates (LHR) of MOX rods are 25 kW/m (BOL of IFA 702) and 20 kW/m (EOL of IFA 702). The axial peak burnups achieved are about 74 GWd/t for both of MOX and UO2. Centerline temperature and plenum gas pressure were measured in situ during irradiation. The measured centerline temperature is plotted against LHR at the position where thermocouples are fixed. The slopes of MOX are corresponded to each other, but that of UO2 is higher than those of MOX. This implies that the thermal conductivity of MOX is higher than that of UO2 at high burnup under the condition that the pellet-cladding gap is closed during irradiation. Gap closure is confirmed by the metallography of the postirradiation examinations. It is understood that thermal conductivity of MOX is lower than that of UO2 before irradiation since phonon scattering with plutonium in MOX becomes remarkable. A phonon scattering with plutonium decreases in MOX when burnup proceeds. Thus, thermal conductivity of MOX becomes close to that of UO2. A reverse phenomenon is observed at high burnup region. The phonon scattering with fission products such as Nd and Zr causes a degradation of thermal conductivity of burnt fuel. It might be speculated that this scattering effect causes the phenomenon and the mechanism is discussed here.

Development of burnup dependent fuel rod model in COBRA-TF

NASA Astrophysics Data System (ADS)

Yilmaz, Mine Ozdemir

The purpose of this research was to develop a burnup dependent fuel thermal conductivity model within Pennsylvania State University, Reactor Dynamics and Fuel Management Group (RDFMG) version of the subchannel thermal-hydraulics code COBRA-TF (CTF). The model takes into account first, the degradation of fuel thermal conductivity with high burnup; and second, the fuel thermal conductivity dependence on the Gadolinium content for both UO2 and MOX fuel rods. The modified Nuclear Fuel Industries (NFI) model for UO2 fuel rods and Duriez/Modified NFI Model for MOX fuel rods were incorporated into CTF and fuel centerline predictions were compared against Halden experimental test data and FRAPCON-3.4 predictions to validate the burnup dependent fuel thermal conductivity model in CTF. Experimental test cases from Halden reactor fuel rods for UO2 fuel rods at Beginning of Life (BOL), through lifetime without Gd2O3 and through lifetime with Gd 2O3 and a MOX fuel rod were simulated with CTF. Since test fuel rod and FRAPCON-3.4 results were based on single rod measurements, CTF was run for a single fuel rod surrounded with a single channel configuration. Input decks for CTF were developed for one fuel rod located at the center of a subchannel (rod-centered subchannel approach). Fuel centerline temperatures predicted by CTF were compared against the measurements from Halden experimental test data and the predictions from FRAPCON-3.4. After implementing the new fuel thermal conductivity model in CTF and validating the model with experimental data, CTF model was applied to steady state and transient calculations. 4x4 PWR fuel bundle configuration from Purdue MOX benchmark was used to apply the new model for steady state and transient calculations. First, one of each high burnup UO2 and MOX fuel rods from 4x4 matrix were selected to carry out single fuel rod calculations and fuel centerline temperatures predicted by CTF/TORT-TD were compared against CTF /TORT-TD /FRAPTRAN predictions. After confirming that the new fuel thermal conductivity model in CTF worked and provided consistent results with FRAPTRAN predictions for a single fuel rod configuration, the same type of analysis was carried out for a bigger system which is the 4x4 PWR bundle consisting of 15 fuel pins and one control guide tube. Steady- state calculations at Hot Full Power (HFP) conditions for control guide tube out (unrodded) were performed using the 4x4 PWR array with CTF/TORT-TD coupled code system. Fuel centerline, surface and average temperatures predicted by CTF/TORT-TD with and without the new fuel thermal conductivity model were compared against CTF/TORT-TD/FRAPTRAN predictions to demonstrate the improvement in fuel centerline predictions when new model was used. In addition to that constant and CTF dynamic gap conductance model were used with the new thermal conductivity model to show the performance of the CTF dynamic gap conductance model and its impact on fuel centerline and surface temperatures. Finally, a Rod Ejection Accident (REA) scenario using the same 4x4 PWR array was run both at Hot Zero Power (HZP) and Hot Full Power (HFP) condition, starting at a position where half of the control rod is inserted. This scenario was run using CTF/TORT-TD coupled code system with and without the new fuel thermal conductivity model. The purpose of this transient analysis was to show the impact of thermal conductivity degradation (TCD) on feedback effects, specifically Doppler Reactivity Coefficient (DRC) and, eventually, total core reactivity.

Results of Uranium Dioxide-Tungsten Irradiation Test and Post-Test Examination

NASA Technical Reports Server (NTRS)

Collins, J. F.; Debogdan, C. E.; Diianni, D. C.

1973-01-01

A uranium dioxide (UO2) fueled capsule was fabricated and irradiated in the NASA Plum Brook Reactor Facility. The capsule consisted of two bulk UO2 specimens clad with chemically vapor deposited tungsten (CVD W) 0.762 and 0.1016 cm (0.030-and 0.040-in.) thick, respectively. The second specimen with 0.1016-cm (0.040-in.) thick cladding was irradiated at temperature for 2607 hours, corresponding to an average burnup of 1.516 x 10 to the 20th power fissions/cu cm. Postirradiation examination showed distortion in the bottom end cap, failure of the weld joint, and fracture of the central vent tube. Diametral growth was 1.3 percent. No evidence of gross interaction between CVD tungsten or arc-cast tungsten cladding and the UO2 fuel was observed. Some of the fission gases passed from the fuel cavity to the gas surrounding the fuel specimen via the vent tube and possibly the end-cap weld failure. Whether the UO2 loss rates through the vent tube were within acceptable limits could not be determined in view of the end-cap weld failure.

K2xSn4–xS8–x (x = 0.65–1): a new metal sulfide for rapid and selective removal of Cs+, Sr2+ and UO22+ ions† †Electronic supplementary information (ESI) available: Raman spectra, thermogravimetric analysis, scanning electron microgram, X-ray crystallographic file (CIF) containing crystallographic refinement details, atomic coordinates with equivalent isotropic displacement parameters, anisotropic displacement parameters, and selected bond distances for KTS-3. See DOI: 10.1039/c5sc03040d

PubMed Central

Sarma, Debajit; Malliakas, Christos D.; Subrahmanyam, K. S.; Islam, Saiful M.

2016-01-01

The fission of uranium produces radionuclides, 137Cs and 90Sr, which are major constituents of spent nuclear fuel. The half-life of 137Cs and 90Sr is nearly 30 years and thus that makes them harmful to human life and the environment. The selective removal of these radionuclides in the presence of high salt concentrations from industrial nuclear waste is necessary for safe storage. Here we report the synthesis and crystal structure of K2xSn4–xS8–x (x = 0.65–1, KTS-3) a material which exhibits excellent Cs+, Sr2+ and UO22+ ion exchange properties in varying conditions. The compound adopts a layered structure which consists of exchangeable potassium ions sandwiched between infinite layers of octahedral and tetrahedral tin centers. K2xSn4–xS8–x (x = 0.65–1, KTS-3) crystallizes in the monoclinic space group P21/c with cell parameters a = 13.092(3) Å, b = 16.882(2) Å, c = 7.375(1) Å and β = 98.10(1)°. Refinement of the single crystal diffraction data revealed the presence of Sn vacancies in the tetrahedra that are long range ordered. The interlayer potassium ions of KTS-3 can be exchanged for Cs+, Sr2+ and UO22+. KTS-3 exhibits rapid and efficient ion exchange behavior in a broad pH range. The distribution coefficients (Kd) for KTS-3 are high for Cs+ (5.5 × 104), Sr2+ (3.9 × 105) and UO22+ (2.7 × 104) at neutral pH (7.4, 6.9, 5.7 ppm Cs+, Sr2+ and UO22+, respectively; V/m ∼ 1000 mL g–1). KTS-3 exhibits impressive Cs+, Sr2+ and UO22+ ion exchange properties in high salt concentration and over a broad pH range, which coupled with the low cost, environmentally friendly nature and facile synthesis underscores its potential in treating nuclear waste. PMID:29910868

Effect of reactor radiation on the thermal conductivity of TREAT fuel

NASA Astrophysics Data System (ADS)

Mo, Kun; Miao, Yinbin; Kontogeorgakos, Dimitrios C.; Connaway, Heather M.; Wright, Arthur E.; Yacout, Abdellatif M.

2017-04-01

The Transient Reactor Test Facility (TREAT) at the Idaho National Laboratory is resuming operations after more than 20 years in latency in order to produce high-neutron-flux transients for investigating transient-induced behavior of reactor fuels and their interactions with other materials and structures. A parallel program is ongoing to develop a replacement core in which the fuel, historically containing highly-enriched uranium (HEU), is replaced by low-enriched uranium (LEU). Both the HEU and prospective LEU fuels are in the form of UO2 particles dispersed in a graphite matrix, but the LEU fuel will contain a much higher volume of UO2 particles, which may create a larger area of interphase boundaries between the particles and the graphite. This may lead to a higher volume fraction of graphite exposed to the fission fragments escaping from the UO2 particles, and thus may induce a higher volume of fission-fragment damage on the fuel graphite. In this work, we analyzed the reactor-radiation induced thermal conductivity degradation of graphite-based dispersion fuel. A semi-empirical method to model the relative thermal conductivity with reactor radiation was proposed and validated based on the available experimental data. Prediction of thermal conductivity degradation of LEU TREAT fuel during a long-term operation was performed, with a focus on the effect of UO2 particle size on fission-fragment damage. The proposed method can be further adjusted to evaluate the degradation of other properties of graphite-based dispersion fuel.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marchetti, M.; University of Montpellier, IES, UMR 5214, F-34000, Montpellier; Laux, D.

During irradiation UO{sub 2} nuclear fuel experiences the development of a non-uniform distribution of porosity which contributes to establish varying mechanical properties along the radius of the pellet. Radial variations of the porosity and of elastic properties in high burnup UO{sub 2} pellet can be investigated via high frequency acoustic microscopy. Ultrasound waves are generated by a piezoelectric transducer and focused on the sample, after having travelled through a coupling liquid. The elastic properties of the material are related to the velocity of the generated Rayleigh surface wave (VR). A 67 MWd/kgU UO{sub 2} pellet was characterized using the acousticmore » microscope installed in the hot cells of the Institute of Transuranium Elements: 90 MHz frequency was applied, methanol was used as coupling liquid and VR was measured at different radial positions. By comparing the porosity values obtained via acoustic microscopy with those determined using ceramographic image analysis a good agreement was found, especially in the areas close to the centre. In addition Young's modulus was calculated and its radial profile was correlated to the corresponding burnup profile. (authors)« less

Piezomagnetism and magnetoelastic memory in uranium dioxide

DOE PAGES

Jaime, M.; Saul, A.; Salamon, M.; ...

2017-07-24

Uranium dioxide (UO 2) is a prime nuclear fuel and perhaps the most thoroughly studied actinide material to date. Its thermal and magnetic properties remain, however, a puzzle resulting from strong couplings between magnetism and lattice vibrations. The magnetic state of this cubic material is characterized by a non- collinear antiferromagnetic structure and multidomain Jahn-Teller distortions that could be behind novel thermal properties. Here we show that single crystals of UO 2, subjected to magnetic fields up to 95 T in the magnetic state, exhibit the abrupt appearance of positive linear magnetostriction leading to a trigonal distortion. Upon reversal ofmore » the field the linear term also reverses sign, a hallmark of piezomagnetism. The switching phenomenon occurs at ± 18 T and persists during subsequent field reversals, demonstrating robust magneto-elastic memory. This is the first example of piezomagnetism in an actinide spin system and the magneto-elastic memory loop here is nearly an order of magnitude wider in field than those previously observed, making UO 2 the hardest piezomagnet known. The possibility of an inverse phase with reduced magnetocrystalline anisotropy is considered to explain these effects.« less

Piezomagnetism and magnetoelastic memory in uranium dioxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaime, M.; Saul, A.; Salamon, M.

Uranium dioxide (UO 2) is a prime nuclear fuel and perhaps the most thoroughly studied actinide material to date. Its thermal and magnetic properties remain, however, a puzzle resulting from strong couplings between magnetism and lattice vibrations. The magnetic state of this cubic material is characterized by a non- collinear antiferromagnetic structure and multidomain Jahn-Teller distortions that could be behind novel thermal properties. Here we show that single crystals of UO 2, subjected to magnetic fields up to 95 T in the magnetic state, exhibit the abrupt appearance of positive linear magnetostriction leading to a trigonal distortion. Upon reversal ofmore » the field the linear term also reverses sign, a hallmark of piezomagnetism. The switching phenomenon occurs at ± 18 T and persists during subsequent field reversals, demonstrating robust magneto-elastic memory. This is the first example of piezomagnetism in an actinide spin system and the magneto-elastic memory loop here is nearly an order of magnitude wider in field than those previously observed, making UO 2 the hardest piezomagnet known. The possibility of an inverse phase with reduced magnetocrystalline anisotropy is considered to explain these effects.« less

Pyroprocessing of Light Water Reactor Spent Fuels Based on an Electrochemical Reduction Technology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ohta, Hirokazu; Inoue, Tadashi; Sakamura, Yoshiharu

A concept of pyroprocessing light water reactor (LWR) spent fuels based on an electrochemical reduction technology is proposed, and the material balance of the processing of mixed oxide (MOX) or high-burnup uranium oxide (UO{sub 2}) spent fuel is evaluated. Furthermore, a burnup analysis for metal fuel fast breeder reactors (FBRs) is conducted on low-decontamination materials recovered by pyroprocessing. In the case of processing MOX spent fuel (40 GWd/t), UO{sub 2} is separately collected for {approx}60 wt% of the spent fuel in advance of the electrochemical reduction step, and the product recovered through the rare earth (RE) removal step, which hasmore » the composition uranium:plutonium:minor actinides:fission products (FPs) = 76.4:18.4:1.7:3.5, can be applied as an ingredient of FBR metal fuel without a further decontamination process. On the other hand, the electroreduced alloy of high-burnup UO{sub 2} spent fuel (48 GWd/t) requires further decontamination of residual FPs by an additional process such as electrorefining even if RE FPs are removed from the alloy because the recovered plutonium (Pu) is accompanied by almost the same amount of FPs in addition to RE. However, the amount of treated materials in the electrorefining step is reduced to {approx}10 wt% of the total spent fuel owing to the prior UO{sub 2} recovery step. These results reveal that the application of electrochemical reduction technology to LWR spent oxide fuel is a promising concept for providing FBR metal fuel by a rationalized process.« less

MITEE: A Compact Ultralight Nuclear Thermal Propulsion Engine for Planetary Science Missions

NASA Astrophysics Data System (ADS)

Powell, J.; Maise, G.; Paniagua, J.

2001-01-01

A new approach for a near-term compact, ultralight nuclear thermal propulsion engine, termed MITEE (Miniature Reactor Engine) is described. MITEE enables a wide range of new and unique planetary science missions that are not possible with chemical rockets. With U-235 nuclear fuel and hydrogen propellant the baseline MITEE engine achieves a specific impulse of approximately 1000 seconds, a thrust of 28,000 newtons, and a total mass of only 140 kilograms, including reactor, controls, and turbo-pump. Using higher performance nuclear fuels like U-233, engine mass can be reduced to as little as 80 kg. Using MITEE, V additions of 20 km/s for missions to outer planets are possible compared to only 10 km/s for H2/O2 engines. The much greater V with MITEE enables much faster trips to the outer planets, e.g., two years to Jupiter, three years to Saturn, and five years to Pluto, without needing multiple planetary gravity assists. Moreover, MITEE can utilize in-situ resources to further extend mission V. One example of a very attractive, unique mission enabled by MITEE is the exploration of a possible subsurface ocean on Europa and the return of samples to Earth. Using MITEE, a spacecraft would land on Europa after a two-year trip from Earth orbit and deploy a small nuclear heated probe that would melt down through its ice sheet. The probe would then convert to a submersible and travel through the ocean collecting samples. After a few months, the probe would melt its way back up to the MITEE lander, which would have replenished its hydrogen propellant by melting and electrolyzing Europa surface ice. The spacecraft would then return to Earth. Total mission time is only five years, starting from departure from Earth orbit. Other unique missions include Neptune and Pluto orbiter, and even a Pluto sample return. MITEE uses the cermet Tungsten-UO2 fuel developed in the 1960's for the 710 reactor program. The W-UO2 fuel has demonstrated capability to operate in 3000 K hydrogen for many hours - a much longer period than the approximately one hour burn time for MITEE. Using this cermet fuel, and technology available from other nuclear propulsion programs, MITEE could be developed and ready for implementation in a relatively short time, i.e., approximately seven years. An overview description of the MITEE engine and its performance capabilities is provided.

Time-resolved infrared reflectance studies of the dehydration-induced transformation of uranyl nitrate hexahydrate to the trihydrate form

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, Timothy J.; Sweet, Lucas E.; Meier, David E.

2015-09-08

Uranyl nitrate is a key species in the nuclear fuel cycle. However, this species is known to exist in different states of hydration, including the hexahydrate ([UO 2(NO 3) 2(H 2O) 6] often called UNH), the trihydrate [UO 2(NO 3) 2(H 2O) 3 or UNT], and in very dry environments the dihydrate form [UO 2(NO 3) 2(H 2O) 2]. Their relative stabilities depend on both water vapor pressure and temperature. In the 1950s and 1960s, the different phases were studied by infrared transmission spectroscopy but were limited both by instrumental resolution and by the ability to prepare the samples formore » transmission. We have revisited this problem using time-resolved reflectance spectroscopy, which requires no sample preparation and allows dynamic analysis while the sample is exposed to a flow of N 2 gas. Samples of known hydration state were prepared and confirmed via X-ray diffraction patterns of known species. In reflectance mode the hexahydrate UO 2(NO 3) 2(H 2O) 6 has a distinct uranyl asymmetric stretch band at 949.0 cm –1 that shifts to shorter wavelengths and broadens as the sample desiccates and recrystallizes to the trihydrate, first as a shoulder growing in on the blue edge but ultimately results in a doublet band with reflectance peaks at 966 and 957 cm –1. The data are consistent with transformation from UNH to UNT as UNT has two inequivalent UO 2 2+ sites. The dehydration of UO 2(NO 3) 2(H 2O) 6 to UO 2(NO 3) 2(H 2O) 3 is both a structural and morphological change that has the lustrous lime green UO 2(NO 3) 2(H 2O) 6 crystals changing to the matte greenish yellow of the trihydrate solid. As a result, the phase transformation and crystal structures were confirmed by density functional theory calculations and optical microscopy methods, both of which showed a transformation with two distinct sites for the uranyl cation in the trihydrate, with only one in the hexahydrate.« less

Calorimetric determination of energetics of solid solutions of UO 2+ x with CaO and Y 2O 3

NASA Astrophysics Data System (ADS)

Mazeina, Lena; Navrotsky, Alexandra; Greenblatt, Martha

2008-02-01

Quantitative study of thermodynamic properties of solid solutions of UO 2+ x with divalent and trivalent oxides is important for predicting the behavior of oxide fuel. Although early literature work measured vapor pressure in some of these solid solutions, direct calorimetric measurements of enthalpies of formation have been hampered by the refractory nature of such oxides. First measurements of the enthalpies of formation in the systems UO 2+ x-CaO and UO 2+ x-YO 1.5, obtained by high-temperature oxide melt solution calorimetry, are reported. Both systems show significantly negative (exothermic) heats of formation from binary oxides (UO 2, plus O 2 and CaO or YO 1.5, as well as from UO 2 plus UO 3 and CaO or YO 1.5), consistent with reported free energy measurements in the urania-yttria system. The energetic contributions of oxygen content (oxidation of U 4+) and of charge balanced ionic substitution as well as defect clustering are discussed. Behavior of urania-yttria is compared to that of corresponding systems in which the tetravalent ion is Ce, Zr, or Hf. The substantial additional stability in the solid solutions compared to pure UO 2+ x may retard, in both thermodynamic and kinetic sense, the oxidation and leaching of spent fuel to form aqueous U 6+ and solid uranyl phases.

Time-Resolved Infrared Reflectance Studies of the Dehydration-Induced Transformation of Uranyl Nitrate Hexahydrate to the Trihydrate Form

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, Timothy J.; Sweet, Lucas E.; Meier, David E.

Uranyl nitrate is a key species in the nuclear fuel cycle. However, this species is known to exist in different states of hydration, including the hexahydrate ([UO2(NO3)2(H2O)6] often called UNH), the trihydrate [UO2(NO3)2(H2O)3 or UNT], and in very dry environments the dihydrate form [UO2(NO3)2(H2O)2]. Their relative stabilities depend on both water vapor pressure and temperature. In the 1950s and 1960s the different phases were studied by infrared transmission spectroscopy, but were limited both by instrumental resolution and by the ability to prepare the samples for transmission. We have revisited this problem using time-resolved reflectance spectroscopy, which requires no sample preparationmore » and allows dynamic analysis while the sample is exposed to a flow of N2 gas. Samples of known hydration state were prepared and confirmed via X-ray diffraction patterns of known species. In reflectance mode the hexahydrate UO2(NO3)2(H2O)6 has a distinct uranyl asymmetric stretch band at 949.0 cm-1 that shifts to shorter wavelengths and broadens as the sample desiccates and recrystallizes to the trihydrate, first as a shoulder growing in on the blue edge but ultimately results in a doublet band with reflectance peaks at 966 and 957 cm-1. The data are consistent with transformation from UNH to UNT as UNT has two inequivalent UO22+ sites. The dehydration of UO2(NO3)2(H2O)6 to UO2(NO3)2(H2O)3 is both a structural and morphological change that has the lustrous lime green UO2(NO3)2(H2O)6 crystals changing to the matte greenish yellow of the trihydrate solid. The phase transformation and crystal structures were confirmed by density functional theory calculations and optical microscopy methods, both of which showed a transformation with two distinct sites for the uranyl cation in the trihydrate, with but one in the hexahydrate.« less

Chlorine Diffusion in Uranium Dioxide: Thermal Effects versus Radiation Enhanced Effects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pipon, Yves; Moncoffre, Nathalie; Bererd, Nicolas

2007-07-01

Chlorine is present as an impurity in the UO{sub 2} nuclear fuel. {sup 35}Cl is activated into {sup 36}Cl by thermal neutron capture. In case of interim storage or deep geological disposal of the spent fuel, this isotope is known to be able to contribute significantly to the instant release fraction because of its mobile behavior and its long half life (around 300000 years). It is therefore important to understand its migration behavior within the fuel rod. During reactor operation, chlorine diffusion can be due to thermally activated processes or can be favoured by irradiation defects induced by fission fragmentsmore » or alpha decay. In order to decouple both phenomena, we performed two distinct experiments to study the effects of thermal annealing on the behaviour of chlorine on one hand and the effects of the irradiation with fission products on the other hand. During in reactor processes, part of the {sup 36}Cl may be displaced from its original position, due to recoil or to collisions with fission products. In order to study the behavior of the displaced chlorine, {sup 37}Cl has been implanted into sintered depleted UO{sub 2} pellets (mean grain size around 18 {mu}m). The spatial distribution of the implanted and pristine chlorine has been analyzed by SIMS before and after treatment. Thermal annealing of {sup 37}Cl implanted UO{sub 2} pellets (implantation fluence of 10{sup 13} ions.cm{sup -2}) show that it is mobile from temperatures as low as 1273 K (E{sub a}=4.3 eV). The irradiation with fission products (Iodine, E=63.5 MeV) performed at 300 and 510 K, shows that the diffusion of chlorine is enhanced and that a thermally activated contribution is preserved (E{sub a}=0.1 eV). The diffusion coefficients measured at 1473 K and under fission product irradiation at 510 K are similar (D = 3.10{sup -14} cm{sup 2}.s{sup -1}). Considering in first approximation that the diffusion length L can be expressed as a function of the diffusion coefficient D and time t by : L=(Dt)1/2, the diffusion distance after 3 years is L=17 {mu}m. It results that there is a great probability for the chlorine contained in the UO{sub 2} grains to have reached the grain boundaries after 3 years, in the core of the fuel rod as well as at its periphery. Moreover, diffusion and concentration of chlorine at grain boundaries has been evidenced using SIMS mapping. Our results indicate therefore, that, during reactor operation and after, the majority of {sup 36}Cl is likely to have moved to grain boundaries, rim and gap. This fraction might then significantly contribute to the rapid or instant release of chlorine. This could have important consequences for safety assessment. During reactor operation, chlorine ({sup 35}Cl), an impurity of the nuclear fuel, is activated into {sup 36}Cl, a long lived mobile isotope. Because of its long half life and its mobility, this isotope may contribute significantly to the instant release fraction under disposal conditions. Thermal annealing of Cl implanted UO{sub 2} sintered pellets show that it is mobile from temperatures as low as 1273 K (E{sub a} = 4.3 eV). Chlorine diffusion induced by irradiation with fission products preserves a thermally activated contribution. The radiation induced defects significantly enhance chlorine migration. (authors)« less

Heat pipe nuclear reactor for space power

NASA Technical Reports Server (NTRS)

Koening, D. R.

1976-01-01

A heat-pipe-cooled nuclear reactor has been designed to provide 3.2 MWth to an out-of-core thermionic conversion system. The reactor is a fast reactor designed to operate at a nominal heat-pipe temperature of 1675 K. Each reactor fuel element consists of a hexagonal molybdenum block which is bonded along its axis to one end of a molybdenum/lithium-vapor heat pipe. The block is perforated with an array of longitudinal holes which are loaded with UO2 pellets. The heat pipe transfers heat directly to a string of six thermionic converters which are bonded along the other end of the heat pipe. An assembly of 90 such fuel elements forms a hexagonal core. The core is surrounded by a thermal radiation shield, a thin thermal neutron absorber, and a BeO reflector containing boron-loaded control drums.

Study on the leaching behavior of actinides from nuclear fuel debris

NASA Astrophysics Data System (ADS)

Kirishima, Akira; Hirano, Masahiko; Akiyama, Daisuke; Sasaki, Takayuki; Sato, Nobuaki

2018-04-01

For the prediction of the leaching behavior of actinides contained in the nuclear fuel debris generated by the Fukushima Daiichi nuclear power plant accident in Japan, simulated fuel debris consisting of a UO2-ZrO2 solid solution doped with 137Cs, 237Np, 236Pu, and 241Am tracers was synthesized and investigated. The synthesis of the debris was carried out by heat treatment at 1200 °C at different oxygen partial pressures, and the samples were subsequently used for leaching tests with Milli-Q water and seawater. The results of the leaching tests indicate that the leaching of actinides depends on the redox conditions under which the debris was generated; for example, debris generated under oxidative conditions releases more actinide nuclides to water than that generated under reductive conditions. Furthermore, we found that, as Zr(IV) increasingly substituted U(IV) in the fluorite crystal structure of the debris, the actinide leaching from the debris decreased. In addition, we found that seawater leached more actinides from the debris than pure water, which seems to be caused by the complexation of actinides by carbonate ions in seawater.

Nuclear Thermal Rocket Simulation in NPSS

NASA Technical Reports Server (NTRS)

Belair, Michael L.; Sarmiento, Charles J.; Lavelle, Thomas M.

2013-01-01

Four nuclear thermal rocket (NTR) models have been created in the Numerical Propulsion System Simulation (NPSS) framework. The models are divided into two categories. One set is based upon the ZrC-graphite composite fuel element and tie tube-style reactor developed during the Nuclear Engine for Rocket Vehicle Application (NERVA) project in the late 1960s and early 1970s. The other reactor set is based upon a W-UO2 ceramic-metallic (CERMET) fuel element. Within each category, a small and a large thrust engine are modeled. The small engine models utilize RL-10 turbomachinery performance maps and have a thrust of approximately 33.4 kN (7,500 lbf ). The large engine models utilize scaled RL-60 turbomachinery performance maps and have a thrust of approximately 111.2 kN (25,000 lbf ). Power deposition profiles for each reactor were obtained from a detailed Monte Carlo N-Particle (MCNP5) model of the reactor cores. Performance factors such as thermodynamic state points, thrust, specific impulse, reactor power level, and maximum fuel temperature are analyzed for each engine design.

Nuclear Thermal Rocket Simulation in NPSS

NASA Technical Reports Server (NTRS)

Belair, Michael L.; Sarmiento, Charles J.; Lavelle, Thomas L.

2013-01-01

Four nuclear thermal rocket (NTR) models have been created in the Numerical Propulsion System Simulation (NPSS) framework. The models are divided into two categories. One set is based upon the ZrC-graphite composite fuel element and tie tube-style reactor developed during the Nuclear Engine for Rocket Vehicle Application (NERVA) project in the late 1960s and early 1970s. The other reactor set is based upon a W-UO2 ceramic- metallic (CERMET) fuel element. Within each category, a small and a large thrust engine are modeled. The small engine models utilize RL-10 turbomachinery performance maps and have a thrust of approximately 33.4 kN (7,500 lbf ). The large engine models utilize scaled RL-60 turbomachinery performance maps and have a thrust of approximately 111.2 kN (25,000 lbf ). Power deposition profiles for each reactor were obtained from a detailed Monte Carlo N-Particle (MCNP5) model of the reactor cores. Performance factors such as thermodynamic state points, thrust, specific impulse, reactor power level, and maximum fuel temperature are analyzed for each engine design.

EXPERIMENTAL STUDIES OF TRANSIENT EFFECTS IN FAST REACTOR FUELS. SERIES I. UO$sub 2$ IRRADIATIONS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Field, J.H.

1962-11-15

An experimental program to evaluate the performance of FCR and EFCR fuel during transient operation is outlined, and the initial series of tests are described in some detail. Test results from five experiments in the TREAT reactor, using 1-in. OD SS-clad UO/sub 2/ fuel specimens, are compared with regard to fuel temperatures, mechanical integrity, and post-irradiation appearance. Incipient fuel pin failure limits for transients are identified with maximum fuel temperatures in the range of 7000 deg F. Multiple transient damage to the cladding is likely for transients above the melting point of the fuel. (auth)

PRESSURIZED WATER REACTOR PROGRAM TECHNICAL PROGRESS REPORT FOR THE PERIOD MAY 5, 1955 TO JUNE 16, 1955

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

The current PWR plant and core parameters are listed. Resign requirements are briefly summarized for a radiation monitoring system, a fuel handling water system, a coolant purification system, an electrical power distribution system, and component shielding. Results of studies on thermal bowing and stressing of UO/sub 2/ are reported. A graph is presented of reactor power vs. reactor flow for various hot channel conditions. Development of U-- Mo and U-Nb alloys has been stopped because of the recent selection of UO/sub 2/ fuel material for the PWR core and blanket. The fabrication characteristics of UO/sub 2/ powders are being studied.more » Seamless Zircaloy-2 tubing has been tested to determine elastic limits, bursting pressures, and corrosion resistance. Fabrication techniques and tests for corrosion and defects in Zircaloy-clad U-Mo and UO/sub 2/ fuel rods are described. The preparation of UO/sub 2/ by various methods is being studied to determine which method produces a material most suitable for PWR fuel elements. The stability of UO/sub 2/ compacts in high temperature water and steam is being determined. Surface area and density measurements have been performed on samples of UO/sub 2/ powder prepared by various methods. Revelopment work on U-- Mo and U--Nb alloys has included studies of the effect on corrosion behavior of additions to the test water, additions to the alloys, homogenization of the alloys, annealing times, cladding, and fabrication techniques. Data are presented on relaxation in spring materials after exposure to a corrosive environment. Results are reported from loop and autoclave tests on fission product and crud deposition. Results of irradiation and corrosion testing of clad and unclad U--Mo and U-Nh alloys are described. The UO/sub 2/ irradiation program has included studies of dimensional changes, release of fission gases, and activity in the water surrounding the samples. A review of the methods of calculating reactor physics parameters has been completed, and the established procedures have been applied to determination of PWR reference design parameters. Critical experiments and primary loop shielding analyses are described. (D.E.B.)« less

High Power MPD Nuclear Electric Propulsion (NEP) for Artificial Gravity HOPE Missions to Callisto

NASA Technical Reports Server (NTRS)

McGuire, Melissa L.; Borowski, Stanley K.; Mason, Lee M.; Gilland, James

2003-01-01

This documents the results of a one-year multi-center NASA study on the prospect of sending humans to Jupiter's moon, Callisto, using an all Nuclear Electric Propulsion (NEP) space transportation system architecture with magnetoplasmadynamic (MPD) thrusters. The fission reactor system utilizes high temperature uranium dioxide (UO2) in tungsten (W) metal matrix cermet fuel and electricity is generated using advanced dynamic Brayton power conversion technology. The mission timeframe assumes on-going human Moon and Mars missions and existing space infrastructure to support launch of cargo and crewed spacecraft to Jupiter in 2041 and 2045, respectively.

Effect of reactor radiation on the thermal conductivity of TREAT fuel

DOE PAGES

Mo, Kun; Miao, Yinbin; Kontogeorgakos, Dimitrios C.; ...

2017-02-04

The Transient Reactor Test Facility (TREAT) at the Idaho National Laboratory is resuming operations after more than 20 years in latency in order to produce high-neutron-flux transients for investigating transient-induced behavior of reactor fuels and their interactions with other materials and structures. A parallel program is ongoing to develop a replacement core in which the fuel, historically containing highly-enriched uranium (HEU), is replaced by low-enriched uranium (LEU). Both the HEU and prospective LEU fuels are in the form of UO 2 particles dispersed in a graphite matrix, but the LEU fuel will contain a much higher volume of UO 2more » particles, which may create a larger area of interphase boundaries between the particles and the graphite. This may lead to a higher volume fraction of graphite exposed to the fission fragments escaping from the UO 2 particles, and thus may induce a higher volume of fission-fragment damage on the fuel graphite. In this work, we analyzed the reactor-radiation induced thermal conductivity degradation of graphite-based dispersion fuel. A semi-empirical method to model the relative thermal conductivity with reactor radiation was proposed and validated based on the available experimental data. Prediction of thermal conductivity degradation of LEU TREAT fuel during a long-term operation was performed, with a focus on the effect of UO 2 particle size on fission-fragment damage. Lastly, the proposed method can be further adjusted to evaluate the degradation of other properties of graphite-based dispersion fuel.« less

Effect of reactor radiation on the thermal conductivity of TREAT fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mo, Kun; Miao, Yinbin; Kontogeorgakos, Dimitrios C.

The Transient Reactor Test Facility (TREAT) at the Idaho National Laboratory is resuming operations after more than 20 years in latency in order to produce high-neutron-flux transients for investigating transient-induced behavior of reactor fuels and their interactions with other materials and structures. A parallel program is ongoing to develop a replacement core in which the fuel, historically containing highly-enriched uranium (HEU), is replaced by low-enriched uranium (LEU). Both the HEU and prospective LEU fuels are in the form of UO 2 particles dispersed in a graphite matrix, but the LEU fuel will contain a much higher volume of UO 2more » particles, which may create a larger area of interphase boundaries between the particles and the graphite. This may lead to a higher volume fraction of graphite exposed to the fission fragments escaping from the UO 2 particles, and thus may induce a higher volume of fission-fragment damage on the fuel graphite. In this work, we analyzed the reactor-radiation induced thermal conductivity degradation of graphite-based dispersion fuel. A semi-empirical method to model the relative thermal conductivity with reactor radiation was proposed and validated based on the available experimental data. Prediction of thermal conductivity degradation of LEU TREAT fuel during a long-term operation was performed, with a focus on the effect of UO 2 particle size on fission-fragment damage. Lastly, the proposed method can be further adjusted to evaluate the degradation of other properties of graphite-based dispersion fuel.« less

Development code for sensitivity and uncertainty analysis of input on the MCNPX for neutronic calculation in PWR core

NASA Astrophysics Data System (ADS)

Hartini, Entin; Andiwijayakusuma, Dinan

2014-09-01

This research was carried out on the development of code for uncertainty analysis is based on a statistical approach for assessing the uncertainty input parameters. In the butn-up calculation of fuel, uncertainty analysis performed for input parameters fuel density, coolant density and fuel temperature. This calculation is performed during irradiation using Monte Carlo N-Particle Transport. The Uncertainty method based on the probabilities density function. Development code is made in python script to do coupling with MCNPX for criticality and burn-up calculations. Simulation is done by modeling the geometry of PWR terrace, with MCNPX on the power 54 MW with fuel type UO2 pellets. The calculation is done by using the data library continuous energy cross-sections ENDF / B-VI. MCNPX requires nuclear data in ACE format. Development of interfaces for obtaining nuclear data in the form of ACE format of ENDF through special process NJOY calculation to temperature changes in a certain range.

FABRICATION DEVELOPMENT OF UO$sub 2$-STAINLESS STEEL COMPOSITE FUEL PLATES FOR CORE B OF THE ENRICO FERMI FAST BREEDER REACTOR

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cherubini, J.H.; Beaver, R.J.; Leitten, C.F. Jr.

1961-04-18

The development of an inexpensive composite fuel plate with a high burnup potential for application in a 500 deg C sodium environment as Core B of the Enrico Fermi Fast Breeder Reactor is described. The dispersion fuel product consists of 35 wt.% spheroidal UO/sub 2/ dispersed in type 347B stainless steel powder and clad with wrought type 347 stainless steel. Nominal over-all dimensions of Type II design fuel plates are 18.97 in. long x 2.406 in. wide x 0.112 in. thick with 0.005-in. cladding. Reliable processing methods for achieving a uniform distribution of spheroidal UO/sub 2/ in the matrix powdermore » and cladding the sintered powder compact by roll bonding are described. Examination of experimental plates reveals that the degree of UO/sub 2/ fragmentation and stringering encountered during processing is primarily a function of the degree of cold work employed in the finishing operation snd the starting quality of the UO/sub 2/ powder. Cladding studies indicate that a sound metallurgical bond can be achieved with an 87.5% reduction in thickness at 1200 deg C and that close processing control is required to meet the stringent tolerances specified. The developed process meets all criteria except possibly the surface finish requirement; occasionally, pitting occurs due to scale embedded during hot working. Detailed procedures covering composite plate manufacture are presented. (auth)« less

Analysis and fabrication of tungsten CERMET materials for ultra-high temperature reactor applications via pulsed electric current sintering

NASA Astrophysics Data System (ADS)

Webb, Jonathan A.

The optimized development path for the fabrication of ultra-high temperature W-UO2 CERMET fuel elements were explored within this dissertation. A robust literature search was conducted, which concluded that a W-UO 2 fuel element must contain a fine tungsten microstructure and spherical UO2 kernels throughout the entire consolidation process. Combined Monte Carlo and Computational Fluid Dynamics (CFD) analysis were used to determine the effects of rhenium and gadolinia additions on the performance of W-UO 2 fuel elements at refractory temperatures and in dry and water submerged environments. The computational analysis also led to the design of quasi-optimized fuel elements that can meet thermal-hydraulic and neutronic requirements A rigorous set of experiments were conducted to determine if Pulsed Electric Current Sintering (PECS) can fabricate tungsten and W-Ce02 specimens to the required geometries, densities and microstructures required for high temperature fuel elements as well as determine the mechanisms involved within the PECS consolidation process. The CeO2 acts as a surrogate for UO 2 fuel kernels in these experiments. The experiments seemed to confirm that PECS consolidation takes place via diffusional mass transfer methods; however, the densification process is rapidly accelerated due to the effects of current densities within the consolidating specimen. Fortunately the grain growth proceeds at a traditional rate and the PECS process can yield near fully dense W and W-Ce02 specimens with a finer microstructure than other sintering techniques. PECS consolidation techniques were also shown to be capable of producing W-UO2 segments at near-prototypic geometries; however, great care must be taken to coat the fuel particles with tungsten prior to sintering. Also, great care must be taken to ensure that the particles remain spherical in geometry under the influence of a uniaxial stress as applied during PECS, which involves mixing different fuel kernel sizes in order to reduce the porosity in the initial green compact. Particle mixing techniques were also shown to be capable of producing consolidated CERMETs, but with a less than desirable microstructure. The work presented herin will help in the development of very high temperature reactors for terrestrial and space missions in the future.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Silva, Chinthaka M.; Hunt, Rodney Dale; Snead, Lance Lewis

Uranium mononitride (UN) is important as a nuclear fuel. Fabrication of UN in its microspherical form also has its own merits since the advent of the concept of accident-tolerant fuel, where UN is being considered as a potential fuel in the form of TRISO particles. But, not many processes have been well established to synthesize kernels of UN. Therefore, a process for synthesis of microspherical UN with a minimum amount of carbon is discussed herein. First, a series of single-phased microspheres of uranium sesquinitride (U 2N 3) were synthesized by nitridation of UO 2+C microspheres at a few different temperatures.more » Resulting microspheres were of low-density U 2N 3 and decomposed into low-density UN. The variation of density of the synthesized sesquinitrides as a function of its chemical composition indicated the presence of extra (interstitial) nitrogen atoms corresponding to its hyperstoichiometry, which is normally indicated as α-U 2N 3. Average grain sizes of both U 2N 3 and UN varied in a range of 1–2.5 μm. In addition, these had a considerably large amount of pore spacing, indicating the potential sinterability of UN toward its use as a nuclear fuel.« less

Separation of uranium from technetium in recovery of spent nuclear fuel

DOEpatents

Friedman, H.A.

1984-06-13

A method for decontaminating uranium product from the Purex 5 process comprises addition of hydrazine to the product uranyl nitrate stream from the Purex process, which contains hexavalent (UO/sub 2//sup 2 +/) uranium and heptavalent technetium (TcO/sub 4/-). Technetium in the product stream is reduced and then complexed by the addition of oxalic acid (H/sub 2/C/sub 2/O/sub 4/), and the Tc-oxalate complex is readily separated from the 10 uranium by solvent extraction with 30 vol % tributyl phosphate in n-dodecane.

Separation of uranium from technetium in recovery of spent nuclear fuel

DOEpatents

Friedman, Horace A.

1985-01-01

A method for decontaminating uranium product from the Purex process comprises addition of hydrazine to the product uranyl nitrate stream from the Purex process, which contains hexavalent (UO.sub.2.sup.2+) uranium and heptavalent technetium (TcO.sub.4 -). Technetium in the product stream is reduced and then complexed by the addition of oxalic acid (H.sub.2 C.sub.2 O.sub.4), and the Tc-oxalate complex is readily separated from the uranium by solvent extraction with 30 vol. % tributyl phosphate in n-dodecane.

Bubble evolution in Kr-irradiated UO2 during annealing

NASA Astrophysics Data System (ADS)

He, L.; Bai, X. M.; Pakarinen, J.; Jaques, B. J.; Gan, J.; Nelson, A. T.; El-Azab, A.; Allen, T. R.

2017-12-01

Transmission electron microscopy observation of Kr bubble evolution in polycrystalline UO2 annealed at high temperature was conducted in order to understand the inert gas behavior in oxide nuclear fuel. The average diameter of intragranular bubbles increased gradually from 0.8 nm in as-irradiated sample at room temperature to 2.6 nm at 1600 °C and the bubble size distribution changed from a uniform distribution to a bimodal distribution above 1300 °C. The size of intergranular bubbles increased more rapidly than intragranular ones and bubble denuded zones near grain boundaries formed in all the annealed samples. It was found that high-angle grain boundaries held bigger bubbles than low-angle grain boundaries. Complementary atomistic modeling was conducted to interpret the effects of grain boundary character on the Kr segregation. The area density of strong segregation sites in the high-angle grain boundaries is much higher than that in the low angle grain boundaries.

The Key Role of U28 in the Aqueous Self-Assembly of Uranyl Peroxide Nanocages.

PubMed

Falaise, Clément; Nyman, May

2016-10-04

For 11 years now, the structural diversity and aesthetic beauty of uranyl-peroxide capsules have fascinated researchers from the diverse fields of mineralogy, polyoxometalate chemistry, and nuclear fuel technologies. There is still much to be learned about the mechanisms of the self-assembly process, and the role of solution parameters including pH, alkali template, temperature, time, and others. Here we have exploited the high solubility of the UO2 (2+) /H2 O2 /LiOH aqueous system to address the effect of the hydroxide concentration. Important techniques of this study are single-crystal X-ray diffraction, small-angle X-ray scattering, and Raman spectroscopy. Three key phases dominate the solution speciation as a function of time and the LiOH/UO2 (2+) ratio: the uranyl-triperoxide monomer [UO2 (O2 )3 ](4-) and the two capsules [(UO2 )(O2 )(OH)]24 (24-) (U24 ) and [(UO2 )(O2 )1.5 ]28 (28-) (U28 ). When the LiOH/U ratio is around three, U28 forms rapidly and this cluster can be isolated in high yield and purity. This result was most surprising and challenges the hypothesis that alkali templating is the most important determinant in the cluster geometry. Moreover, analogous experiments with KOH, NH4 OH, and TEAOH (TEA=tetraethylammonium) also rapidly yield U28 , which suggests that U28 is the kinetically favored species. Complete mapping of the pH-time phase space reveals only a narrow window of the U28 dominance, which is why it was previously overlooked as an important kinetic species in this chemical system, as well as others with different counterions. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A modified Embedded-Atom Method interatomic potential for uranium-silicide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beeler, Benjamin; Baskes, Michael; Andersson, David

Uranium-silicide (U-Si) fuels are being pursued as a possible accident tolerant fuel (ATF). This uranium alloy fuel bene ts from higher thermal conductivity and higher ssile density compared to uranium dioxide (UO 2). In order to perform engineering scale nuclear fuel performance simulations, the material properties of the fuel must be known. Currently, the experimental data available for U-Si fuels is rather limited. Thus, multiscale modeling e orts are underway to address this gap in knowledge. In this study, a semi-empirical modi ed Embedded-Atom Method (MEAM) potential is presented for the description of the U-Si system. The potential is ttedmore » to the formation energy, defect energies and structural properties of U 3Si 2. The primary phase of interest (U 3Si 2) is accurately described over a wide temperature range and displays good behavior under irradiation and with free surfaces. The potential can also describe a variety of U-Si phases across the composition spectrum.« less

A modified Embedded-Atom Method interatomic potential for uranium-silicide

DOE PAGES

Beeler, Benjamin; Baskes, Michael; Andersson, David; ...

2017-08-18

Uranium-silicide (U-Si) fuels are being pursued as a possible accident tolerant fuel (ATF). This uranium alloy fuel bene ts from higher thermal conductivity and higher ssile density compared to uranium dioxide (UO 2). In order to perform engineering scale nuclear fuel performance simulations, the material properties of the fuel must be known. Currently, the experimental data available for U-Si fuels is rather limited. Thus, multiscale modeling e orts are underway to address this gap in knowledge. In this study, a semi-empirical modi ed Embedded-Atom Method (MEAM) potential is presented for the description of the U-Si system. The potential is ttedmore » to the formation energy, defect energies and structural properties of U 3Si 2. The primary phase of interest (U 3Si 2) is accurately described over a wide temperature range and displays good behavior under irradiation and with free surfaces. The potential can also describe a variety of U-Si phases across the composition spectrum.« less

A modified Embedded-Atom Method interatomic potential for uranium-silicide

NASA Astrophysics Data System (ADS)

Beeler, Benjamin; Baskes, Michael; Andersson, David; Cooper, Michael W. D.; Zhang, Yongfeng

2017-11-01

Uranium-silicide (U-Si) fuels are being pursued as a possible accident tolerant fuel (ATF). This uranium alloy fuel benefits from higher thermal conductivity and higher fissile density compared to uranium dioxide (UO2). In order to perform engineering scale nuclear fuel performance simulations, the material properties of the fuel must be known. Currently, the experimental data available for U-Si fuels is rather limited. Thus, multiscale modeling efforts are underway to address this gap in knowledge. In this study, a semi-empirical modified Embedded-Atom Method (MEAM) potential is presented for the description of the U-Si system. The potential is fitted to the formation energy, defect energies and structural properties of U3Si2. The primary phase of interest (U3Si2) is accurately described over a wide temperature range and displays good behavior under irradiation and with free surfaces. The potential can also describe a variety of U-Si phases across the composition spectrum.

Nuclear Waste Disposal and Strategies for Predicting Long-Term Performance of Material

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wicks, G G

2001-03-28

Ceramics have been an important part of the nuclear community for many years. On December 2, 1942, an historic event occurred under the West Stands of Stagg Field, at the University of Chicago. Man initiated his first self-sustaining nuclear chain reaction and controlled it. The impact of this event on civilization is considered by many as monumental and compared by some to other significant events in history, such as the invention of the steam engine and the manufacturing of the first automobile. Making this event possible and the successful operation of this first man-made nuclear reactor, was the use ofmore » forty tons of UO2. The use of natural or enriched UO2 is still used today as a nuclear fuel in many nuclear power plants operating world-wide. Other ceramic materials, such as 238Pu, are used for other important purposes, such as ceramic fuels for space exploration to provide electrical power to operate instruments on board spacecrafts. Radioisotopic Thermoelectric Generators (RTGs) are used to supply electrical power and consist of a nuclear heat source and converter to transform heat energy from radioactive decay into electrical power, thus providing reliable and relatively uniform power over the very long lifetime of a mission. These sources have been used in the Galileo spacecraft orbiting Jupiter and for scientific investigations of Saturn with the Cassini spacecraft. Still another very important series of applications using the unique properties of ceramics in the nuclear field, are as immobilization matrices for management of some of the most hazardous wastes known to man. For example, in long-term management of radioactive and hazardous wastes, glass matrices are currently in production immobilizing high-level radioactive materials, and cementious forms have also been produced to incorporate low level wastes. Also, as part of nuclear disarmament activities, assemblages of crystalline phases are being developed for immobilizing weapons grade plutonium, to not only produce environmentally friendly products, but also forms that are proliferation resistant. All of these waste forms as well as others, are designed to take advantage of the unique properties of the ceramic systems.« less

Closed DTU fuel cycle with Np recycle and waste transmutation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beller, D.E.; Sailor, W.C.; Venneri, F.

1999-09-01

A nuclear energy scenario for the 21st century that included a denatured thorium-uranium-oxide (DTU) fuel cycle and new light water reactors (LWRs) supported by accelerator-driven transmutation of waste (ATW) systems was previously described. This coupled system with the closed DTU fuel cycle provides several improvements beyond conventional LWR (CLWR) (once-through, UO{sub 2} fuel) nuclear technology: increased proliferation resistance, reduced waste, and efficient use of natural resources. However, like CLWR fuel cycles, the spent fuel in the first one-third core discharged after startup contains higher-quality Pu than the equilibrium fuel cycle. To eliminate this high-grade Pu, Np is separated and recycledmore » with Th and U--rather than with higher actinides [(HA) including Pu]. The presence of Np in the LWR feed greatly increases the production of {sup 238}Pu so that a few kilograms of Pu generated enough alpha-decay heat that the separated Pu is highly resistant to proliferation. This alternate process also simplifies the pyrochemical separation of fuel elements (Th and U) from HAs. To examine the advantages of this concept, the authors modeled a US deployment scenario for nuclear energy that includes DTU-LWRs plus ATW`s to burn the actinides produced by these LWRs and to close the back-end of the DTU fuel cycle.« less

Optimization of burnable poison design for Pu incineration in fully fertile free PWR core

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fridman, E.; Shwageraus, E.; Galperin, A.

2006-07-01

The design challenges of the fertile-free based fuel (FFF) can be addressed by careful and elaborate use of burnable poisons (BP). Practical fully FFF core design for PWR reactor has been reported in the past [1]. However, the burnable poison option used in the design resulted in significant end of cycle reactivity penalty due to incomplete BP depletion. Consequently, excessive Pu loading were required to maintain the target fuel cycle length, which in turn decreased the Pu burning efficiency. A systematic evaluation of commercially available BP materials in all configurations currently used in PWRs is the main objective of thismore » work. The BP materials considered are Boron, Gd, Er, and Hf. The BP geometries were based on Wet Annular Burnable Absorber (WABA), Integral Fuel Burnable Absorber (IFBA), and Homogeneous poison/fuel mixtures. Several most promising combinations of BP designs were selected for the full core 3D simulation. All major core performance parameters for the analyzed cases are very close to those of a standard PWR with conventional UO{sub 2} fuel including possibility of reactivity control, power peaking factors, and cycle length. The MTC of all FFF cores was found at the full power conditions at all times and very close to that of the UO{sub 2} core. The Doppler coefficient of the FFF cores is also negative but somewhat lower in magnitude compared to UO{sub 2} core. The soluble boron worth of the FFF cores was calculated to be lower than that of the UO{sub 2} core by about a factor of two, which still allows the core reactivity control with acceptable soluble boron concentrations. The main conclusion of this work is that judicial application of burnable poisons for fertile free fuel has a potential to produce a core design with performance characteristics close to those of the reference PWR core with conventional UO{sub 2} fuel. (authors)« less

PRESSURIZED WATER REACTOR (PWR) PROJECT TECHNICAL PROGRESS REPORT FOR THE PERIOD DECEMBER 24, 1959 TO FEBRUARY 23, 1960

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

< 9 A < 2 6 < 7 4 8 9 6 2 6 equalizing vent valves on air locks 2, 4, and 5 was completed. An evaluation of the failed main coolant pump No. 1-80-F-737 was completed. The design for installing combination ball check and manual stop valves on the boiler water level sight glasses, to prevent the escape of steam should a defective sight glass develop, was completed. The main coolant pumps No. 80 and No. 79 were modified by increasing the radial clearance of the impeller wear ring and by removing the upper labyrinth ring. A designmore » for relocating the cooling water flow orifice 17-J4-17 was completed. Metallurgy: Preliminary data from the Bett 69-1 in-pile thermal conductivity capsules indicate that the thermal conductivity of as-sintered ZrO/sub 2/ 34 wt.% UO/sub 2/ appears to decrease from an initial value of about 1.6 Btu/hr-ft- deg F to about 0.7 Btu/hr-ft- deg F after 17 days irradiation in an estimated perturbed flux of 4 x 10/sup 13/. The thermal conductivities of UO/sub 2/ and BeO 51 wt.% UO/sub 2/ fuel remained unchanged during this time. Examination of the two failed X-3-1 fuel plates and the two failed CR-V-m fuel plates showed that a definite burnup limitation exists for bulk UO/sub 2/i of about 16 x 10/sup 20/ to 21.5 x 10/sup 20/ fissions/cc at which point the fuel increases in volume about 4- -5%. Irradiation of both fine and coarse dis-persions of 28 wt.% UO/sub 2/in BeO to exposures of about 11 x 10/sup 20/ fissions/cc shows this material has very poor dimensional stabllity and poor fission gas retention ability. The fine particles dispersion showed approximately 4.8 times the thickness increase as did the coarse particles. Interim examination of a bulk B/sub 4/ burnable poison plate irradiated in the HB-1 loop to about 60 at.% B/sup 10/ burnup showed a 17% increase in plate thickness. The technical feasibility of fabricating blanket receptacles with full length fuel channels and an integral cover plate by form rolling was established. Hack-pressure-bonding appears to be a suitable means of incorporating void volume in fuel compartments of oxide plates. High density (99% T.D.) and improved microstructure of B/sub 4/C-SiC burnable poisons are achieved when small (2 micron) B/sub 4/C particle size powder is used ia hot pressing compacts. Measurements of the self-diffusion coefficients of uranium in UO/sub 2/ by the method of surface activity decrease were completed. Experiments on the diffusion of Xe/sup 133/ in Core 2--type UO/sup 2/ fuel platelets were completed. Diffusion anaeals carried out at 1000 deg C on samples from the X-3-1 and the 14-28 irradiation tests show that the apparent diffusion coefficient for Kr/sup 85/ incresses considerably with burnup. An average activation energy for thoron emanation in UO/sub 2/ was estimated to be 44 kcal/mole. An initial experiment on the release of helium from slightly irradiated B/sub 4/C at 900 deg C resulted in a diffusion coefficient for helium of 3.5 x 10/sup -8/ Physics: Calculatad values for seed-blanket power sharing as a function of PWR-1 Seed 1 life were compared with measured data obtained from thermal instrumentation at Shippingport. Two-dimensional depletion studies in the PWR-2 "composite cell" geometry were completed for seed assembly configurations having different radial fuel zoning. An eighth core representation is being employed for a two- dimensional depletion calculation of PWR-2. An analysis of the effect on the axial power distribution of the nonuniform temperature distribution in an 8 ft PWR-2 core loaded with 295 kg of U/sup 235/ indicated that local variations in power density of as much as 15% may occur, relative to the distribution that would exist if the axial temperature distribution were uniform. A technique was developed which makes possible an approximately correct description of the neutron capture rate within small rectangular boron wafers in diffusion theory calculations. Seed peaking factors measured in a five-cluster slab of PWR-2 mock- up materials were measured and compared with calculated peaking factors obtained using the nuclear« less

Multiple Irradiation Capsule Experiment (MICE)-3B Irradiation Test of Space Fuel Specimens in the Advanced Test Reactor (ATR) - Close Out Documentation for Naval Reactors (NR) Information

DOE Office of Scientific and Technical Information (OSTI.GOV)

M. Chen; CM Regan; D. Noe

2006-01-09

Few data exist for UO{sub 2} or UN within the notional design space for the Prometheus-1 reactor (low fission rate, high temperature, long duration). As such, basic testing is required to validate predictions (and in some cases determine) performance aspects of these fuels. Therefore, the MICE-3B test of UO{sub 2} pellets was designed to provide data on gas release, unrestrained swelling, and restrained swelling at the upper range of fission rates expected for a space reactor. These data would be compared with model predictions and used to determine adequacy of a space reactor design basis relative to fission gas releasemore » and swelling of UO{sub 2} fuel and to assess potential pellet-clad interactions. A primary goal of an irradiation test for UN fuel was to assess performance issues currently associated with this fuel type such as gas release, swelling and transient performance. Information learned from this effort may have enabled use of UN fuel for future applications.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Verkerk, B.

In 1959 a fuel development program was undertaken based on UO/sub 2/ in which it was intended to study all variables that could influence the quality of fabricated UO/sub 2/-pellets. Later this program was extended to a study of electrolytic UO/sub 2/ with the fabrication of swaged or vibratory compacted fuel elements in mind, and recently the study of the UO/sub 2/-PuO/sub 2/ system was incorporated in it. In order to obtain a better knowledge of the UO/sub 2/- powders that can be used for sintering purposes, an extensive study was made of various preparation methods. A small plutonium laboratorymore » containing equipment for the preparation of UO/sub 2/-- PuO/sub 2/ pellets containing 1 to 10% PuO/sub 2/ was set up and preliminary experiments were performed. Work on a small scale was done on pressing and sintering of UO/sub 2/ made along various routes. The reduction process was also studied. For the regeneration of scrap, especially for the case of enriched material, a 5-kg batch dissolution and precipitation plant was built. This installation is also used for various precipitation studies on a larger scale. Within the scope of tue fuel development program the study of canning materials is also of great importance. For the ship-propulsion reactor Zircaloy-2 was chosen as canning material. Various welding experiments were done in an argon-arc welding chamber and it was found that under well selected conditions very satisfactory end-cap welds could be obtained. 1n the corrosion program it became clear that proper conditioning is of utmost importance. Means of pre-operation treatment are being studied. In the HFR a low-temperature, low-pressure loop for the irradiation of capsules is in regular operation. The pressurized loop now under construction was designed for testing of fuel rods and clusters as planned for the ship-propulsion reactor, under conditions close to those of the actual reactor. The facilities for the post- irradiation measurements consist of two lead cells. (auth)« less

Inductive Double-Contingency Analysis of UO2 Powder Bulk Blending Operations at a Commercial Fuel Plant (U)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Skiles, S. K.

1994-12-22

An inductive double-contingency analysis (DCA) method developed by the criticality safety function at the Savannah River Site, was applied in Criticality Safety Evaluations (CSEs) of five major plant process systems at the Westinghouse Electric Corporation`s Commercial Nuclear Fuel Manufacturing Plant in Columbia, South Carolina (WEC-Cola.). The method emphasizes a thorough evaluation of the controls intended to provide barriers against criticality for postulated initiating events, and has been demonstrated effective at identifying common mode failure potential and interdependence among multiple controls. A description of the method and an example of its application is provided.

Development of Macroscale Models of UO 2 Fuel Sintering and Densification using Multiscale Modeling and Simulation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Greenquist, Ian; Tonks, Michael

2016-10-01

Light water reactor fuel pellets are fabricated using sintering to final densities of 95% or greater. During reactor operation, the porosity remaining in the fuel after fabrication decreases further due to irradiation-assisted densification. While empirical models have been developed to describe this densification process, a mechanistic model is needed as part of the ongoing work by the NEAMS program to develop a more predictive fuel performance code. In this work we will develop a phase field model of sintering of UO 2 in the MARMOT code, and validate it by comparing to published sintering data. We will then add themore » capability to capture irradiation effects into the model, and use it to develop a mechanistic model of densification that will go into the BISON code and add another essential piece to the microstructure-based materials models. The final step will be to add the effects of applied fields, to model field-assisted sintering of UO 2. The results of the phase field model will be validated by comparing to data from field-assisted sintering. Tasks over three years: 1. Develop a sintering model for UO 2 in MARMOT 2. Expand model to account for irradiation effects 3. Develop a mechanistic macroscale model of densification for BISON« less

System analysis with improved thermo-mechanical fuel rod models for modeling current and advanced LWR materials in accident scenarios

NASA Astrophysics Data System (ADS)

Porter, Ian Edward

A nuclear reactor systems code has the ability to model the system response in an accident scenario based on known initial conditions at the onset of the transient. However, there has been a tendency for these codes to lack the detailed thermo-mechanical fuel rod response models needed for accurate prediction of fuel rod failure. This proposed work will couple today's most widely used steady-state (FRAPCON) and transient (FRAPTRAN) fuel rod models with a systems code TRACE for best-estimate modeling of system response in accident scenarios such as a loss of coolant accident (LOCA). In doing so, code modifications will be made to model gamma heating in LWRs during steady-state and accident conditions and to improve fuel rod thermal/mechanical analysis by allowing axial nodalization of burnup-dependent phenomena such as swelling, cladding creep and oxidation. With the ability to model both burnup-dependent parameters and transient fuel rod response, a fuel dispersal study will be conducted using a hypothetical accident scenario under both PWR and BWR conditions to determine the amount of fuel dispersed under varying conditions. Due to the fuel fragmentation size and internal rod pressure both being dependent on burnup, this analysis will be conducted at beginning, middle and end of cycle to examine the effects that cycle time can play on fuel rod failure and dispersal. Current fuel rod and system codes used by the Nuclear Regulatory Commission (NRC) are compilations of legacy codes with only commonly used light water reactor materials, Uranium Dioxide (UO2), Mixed Oxide (U/PuO 2) and zirconium alloys. However, the events at Fukushima Daiichi and Three Mile Island accident have shown the need for exploration into advanced materials possessing improved accident tolerance. This work looks to further modify the NRC codes to include silicon carbide (SiC), an advanced cladding material proposed by current DOE funded research on accident tolerant fuels (ATF). Several additional fuels will also be analyzed, including uranium nitride (UN), uranium carbide (UC) and uranium silicide (U3Si2). Focusing on the system response in an accident scenario, an emphasis is placed on the fracture mechanics of the ceramic cladding by design the fuel rods to eliminate pellet cladding mechanical interaction (PCMI). The time to failure and how much of the fuel in the reactor fails with an advanced fuel design will be analyzed and compared to the current UO2/Zircaloy design using a full scale reactor model.

Analysis of pellet cladding interaction and creep of U 3SIi2 fuel for use in light water reactors

NASA Astrophysics Data System (ADS)

Metzger, Kathryn E.

Following the accident at the Fukushima plant, enhancing the accident tolerance of the light water reactor (LWR) fleet became a topic of serious discussion. Under the direction of congress, the DOE office of Nuclear Energy added accident tolerant fuel development as a primary component to the existing Advanced Fuels Program. The DOE defines accident tolerant fuels as fuels that "in comparison with the standard UO2- Zircaloy system currently used by the nuclear industry, can tolerate loss of active cooling in the reactor core for a considerably longer time period (depending on the LWR system and accident scenario) while maintaining or improving the fuel performance during normal operations, operational transients, as well as design-basis and beyond design-basis events." To be economically viable, proposed accident tolerant fuels and claddings should be backward compatible with LWR designs, provide significant operating cost improvements such as power uprates, increased fuel burnup, or increased cycle length. In terms of safety, an alternative fuel pellet must have resistance to water corrosion comparable to UO2, thermal conductivity equal to or larger than that of UO2, and a melting temperature that allows the material to remain solid under power reactor conditions. Among the candidates, U3Si2 has a number of advantageous thermophysical properties, including; high density, high thermal conductivity at room temperature, and a high melting temperature. These properties support its use as an accident tolerant fuel while its high uranium density is capable of supporting uprates to the LWR fleet. This research characterizes U3Si2 pellets and analyzes U3Si2 under light water reactor conditions using the fuel performance code BISON. While some thermophysical properties for U3Si2 have been found in the literature, the irradiation behavior is sparse and limited to experience with dispersion fuels. Accordingly, the creep behavior for U3Si2 has been unknown, making it difficult to predict fuel-cladding mechanical behavior. This information is essential for designing accident tolerant fuel systems where ceramic claddings, like silicon carbide (SiC) are proposed. This research provides a model for both the thermal and irradiation creep behavior for U3Si2. This body of research is comprised of both experimental and modeling components. Characterization of the fuel microstructure includes; optical microscopy with pore and grain size analysis, helium pycnometry for density determination, mercury intrusion porosimetry, compositional analysis in the form of XRD, second phase identification using EDX, electrical resistance measurement via four point probe, determination of hardness and toughness through Vickers indentation testing, and determination of elastic properties using the impulse excitation method. Post-sintering grain size data allowed for the determination of grain boundary activation energy and diffusion coefficients, which were used to develop creep models. This was extended to lattice and irradiation enhanced diffusion in order to develop a U3Si2 creep model over thermal and irradiation creep regimes. In addition to the creep model, thermal and swelling behavior models for U3Si2 were implemented into the BISON fuel performance code. A series of simulations evaluated the performance and behavior of U3Si2 under typical light water reactor conditions with advanced SiC ceramic cladding. Simulation results show that fuel creep relieves stress in the ceramic cladding and postpones the. moment of fuel-clad contact. However, the stress reduction to the cladding is minimal because the fuel creep rate is low while the swelling rate is high. Future work should include the investigation of monolithic U3Si2 irradiation swelling since the current model relies upon the swelling data of U3Si2 particles in a metallic dispersion fuel. Additionally, planned thermal creep testing at the University of South Carolina can provide confirmation of the U3Si2 creep model contained herein.

Chlorination of UO 2, PuO 2 and rare earth oxides using ZrCl 4 in LiCl-KCl eutectic melt

NASA Astrophysics Data System (ADS)

Sakamura, Yoshiharu; Inoue, Tadashi; Iwai, Takashi; Moriyama, Hirotake

2005-04-01

A new chlorination method using ZrCl 4 in a molten salt bath has been investigated for the pyrometallurgical reprocessing of nuclear fuels. ZrCl 4 has a high reactivity with oxygen but is not corrosive to refractory metals such as steel. Rare earth oxides (La 2O 3, CeO 2, Nd 2O 3 and Y 2O 3) and actinide oxides (UO 2 and PuO 2) were allowed to react with ZrCl 4 in a LiCl-KCl eutectic salt at 773 K to give a metal chloride solution and a precipitate of ZrO 2. An addition of zirconium metal as a reductant was effective in chlorinating the dioxides. When the oxides were in powder form, the reaction was observed to progress rapidly. Cyclic voltammetry provided a convenient way of establishing when the reaction was completed. It was demonstrated that the ZrCl 4 chlorination method, free from corrosive gas, was very simple and useful.

Fabrication of micro-cell UO2-Mo pellet with enhanced thermal conductivity

NASA Astrophysics Data System (ADS)

Kim, Dong-Joo; Rhee, Young Woo; Kim, Jong Hun; Kim, Keon Sik; Oh, Jang Soo; Yang, Jae Ho; Koo, Yang-Hyun; Song, Kun-Woo

2015-07-01

As one of accident tolerant fuel pellets which should have features of good thermal conductivity and high fission product retention, a micro-cell UO2-Mo pellet has been studied in the aspect of fabrication and thermal property. It was intended to develop the compatible process with conventional UO2 pellet fabrication process. The effects of processing parameters such as the size and density of UO2 granule and the size of Mo powder have been studied to produce sound and dense pellet with completely connected uniform Mo cell-walls. The micro-cell UO2-Mo pellet consists of many Mo micro-cells and UO2 in them. The thermal conductivity of the micro-cell UO2-Mo pellet was measured and compared to those of the UO2 pellet and the UO2-Mo pellet with dispersed form of Mo particles. The thermal conductivity of the micro-cell UO2-Mo pellet was much enhanced and was found to be influenced by the Mo volumetric fraction and pellet integrity. A continuous Mo micro-cell works as a heat conducting channel in the pellet, greatly enhancing the thermal conductivity of the micro cell UO2-Mo pellet.

Complete reduction of high-density UO2 to metallic U in molten Li2O-LiCl

NASA Astrophysics Data System (ADS)

Choi, Eun-Young; Lee, Jeong

2017-10-01

The large size and high density of spent fuel pellets make it difficult to use the pellets directly in electrolytic reduction (also called as oxide reduction, OR) for pyroprocessing owing to the slow diffusion of molten Li2O-LiCl salt electrolyte into the pellets. In this study, we investigated complete OR of high-density UO2 to metallic U without any remaining UO2. Only partial reductions near the surface of high-density UO2 pellets were observed under operation conditions employing fast electrolysis rate that allowed previously complete reduction of low-density UO2 pellets. Complete reduction of high-density UO2 pellets was observed at fast electrolysis rate when the pellet size was reduced. The complete reduction of high-density UO2 pellets without size reduction was achieved at slow electrolysis rate, which allowed sufficient chemical reduction of UO2 with the lithium metal generated by the cathode reaction.

Investigation of molybdate melts as an alternative method of reprocessing used nuclear fuel

DOE PAGES

Hames, Amber L.; Tkac, Peter; Paulenova, Alena; ...

2017-01-17

Here, an investigation of molybdate melts containing sodium molybdate (Na 2MoO 4) and molybdenum trioxide (MoO 3) to achieve the separation of uranium from fission products by crystallization has been performed. The separation is based on the difference in solubility of the fission product metal oxides compared to the uranium oxide or molybdate in the molybdate melt. The molybdate melt dissolves uranium dioxide at high temperatures, and upon cooling, uranium precipitates as uranium dioxide or molybdate, whereas the fission product metals remain soluble in the melt. Small-scale experiments using gram quantities of uranium dioxide have been performed to investigate themore » feasibility of UO 2 purification from the fission products. The composition of the uranium precipitate as well as data for partitioning of several fission product surrogates between the uranium precipitate and molybdate melt for various melt compositions are presented and discussed. The fission products Cs, Sr, Ru and Rh all displayed very large distribution ratios. The fission products Zr, Pd, and the lanthanides also displayed good distribution ratios (D > 10). A melt consisting of 20 wt% MoO 3-50 wt% Na 2MoO 4-30 wt% UO 2 heated to 1313 K and cooled to 1123 K for the physical separation of the UO 2 product from the melt, and washed once with Na 2MoO 4 displays optimum conditions for separation of the UO 2 from the fission products.« less

Development of molecular dynamics potential for uranium silicide fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, Jianguo; Zhang, Yongfeng; Hales, Jason D.

2016-09-01

Use of uranium–silicide (U-Si) in place of uranium dioxide (UO2) is one of the promising concepts being proposed to increase the accident tolerance of nuclear fuels. This is due to a higher thermal conductivity than UO2 that results in lower centerline temperatures. U-Si also has a higher fissile density, which may enable some new cladding concepts that would otherwise require increased enrichment limits to compensate for their neutronic penalty. However, many critical material properties for U-Si have not been determined experimentally. For example, silicide compounds (U3Si2 and U3Si) are known to become amorphous under irradiation. There was clear independent experimentalmore » evidence to support a crystalline to amorphous transformation in those compounds. However, it is still not well understood how the amorphous transformation will affect on fuel behavior. It is anticipated that modeling and simulation may deliver guidance on the importance of various properties and help prioritize experimental work. In order to develop knowledge-based models for use at the engineering scale with a minimum of empirical parameters and increase the predictive capabilities of the developed model, inputs from atomistic simulations are essential. First-principles based density functional theory (DFT) calculations will provide the most reliable information. However, it is probably not possible to obtain kinetic information such as amorphization under irradiation directly from DFT simulations due to size and time limitations. Thus, a more feasible way may be to employ molecular dynamics (MD) simulation. Unfortunately, so far no MD potential is available for U-Si to discover the underlying mechanisms. Here, we will present our recent progress in developing a U-Si potential from ab initio data. This work is supported by the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program funded by the U.S. Department of Energy, Office of Nuclear Energy.« less

Development of molecular dynamics potential for uranium silicide fuels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, Jianguo; Zhang, Yongfeng; Hales, Jason D.

Use of uranium–silicide (U-Si) in place of uranium dioxide (UO2) is one of the promising concepts being proposed to increase the accident tolerance of nuclear fuels. This is due to a higher thermal conductivity than UO2 that results in lower centerline temperatures. U-Si also has a higher fissile density, which may enable some new cladding concepts that would otherwise require increased enrichment limits to compensate for their neutronic penalty. However, many critical material properties for U-Si have not been determined experimentally. For example, silicide compounds (U3Si2 and U3Si) are known to become amorphous under irradiation. There was clear independent experimentalmore » evidence to support a crystalline to amorphous transformation in those compounds. However, it is still not well understood how the amorphous transformation will affect on fuel behavior. It is anticipated that modeling and simulation may deliver guidance on the importance of various properties and help prioritize experimental work. In order to develop knowledge-based models for use at the engineering scale with a minimum of empirical parameters and increase the predictive capabilities of the developed model, inputs from atomistic simulations are essential. First-principles based density functional theory (DFT) calculations will provide the most reliable information. However, it is probably not possible to obtain kinetic information such as amorphization under irradiation directly from DFT simulations due to size and time limitations. Thus, a more feasible way may be to employ molecular dynamics (MD) simulation. Unfortunately, so far no MD potential is available for U-Si to discover the underlying mechanisms. Here, we will present our recent progress in developing a U-Si potential from ab initio data. This work is supported by the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program funded by the U.S. Department of Energy, Office of Nuclear Energy.« less

Computational study of the energetics and defect clustering tendencies for Y- and La-doped UO 2

DOE PAGES

Solomon, J. M.; Alexandrov, V.; Sadigh, B.; ...

2014-07-24

The energetics and defect-ordering tendencies in solid solutions of uoritestructured UO 2 with trivalent rare earth cations (M 3+=Y, La) are investigated computationally using a combination of ionic-pair-potential and densityfunctional- theory (DFT) based methods. Calculated enthalpies of formation with respect to constituent oxides show higher energetic stability for La solid solutions relative to Y, consistent with the di erences in experimentally measured solubility limits for the two systems. Additionally, calculations performed for di erent atomic con gurations show a preference for reduced (increased) oxygen vacancy coordination around La (Y) dopants. The current results are shown to be qualitatively consistent withmore » related calculations and calorimetry measurements in other trivalent-doped uorite-structured oxides, which show a tendency for increasing stability and increasing preference for higher oxygen coordination with increasing size of the trivalent impurity. The implications of these results are discussed in the context of the e ect of trivalent impurities on oxygen-ion mobilities in UO 2, which are relevant to the understanding of experimental observations concerning the e ect of trivalent ssion products on oxidative corrosion rates of spent nuclear fuel.« less

Grain growth and pore coarsening in dense nano-crystalline UO 2+x fuel pellets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yao, Tiankai; Mo, Kun; Yun, Di

Dense nano-sized UO 2+x pellets are synthesized by spark plasma sintering with controlled stoichiometries (UO 2.03 and UO 2.11) and grain sizes (~100 nm), and subsequently isothermally annealed to study their effects on grain growth kinetics and microstructure stability. The grain growth kinetics is determined and analyzed focusing on the interaction between grain boundary migration, pore growth and coalescence. Grains grow much bigger in nano-sized UO 2.11 than UO 2.03 upon thermal annealing, consistent with the fact that hyper-stoichiometric UO 2+x is beneficial for sintering due to enhanced U ion diffusion from excessive O ion interstitials. The activation energies ofmore » the grain growth for UO 2.03 and UO 2.11 are determined as ~1.0 and 1.3~2.0 eV, respectively. As compared with the micron-sized UO 2 in which volumetric diffusion dominates the grain coarsening with an activation energy of ~3.0 eV, the enhanced grain growth kinetics in nano-sized UO 2+x suggests that grain boundary diffusion controls grain growth. Lastly, the higher activation energy of more hyper-stoichiometric nano-sized UO 2.11 may be attributed to the excessive O interstitials pinning grain boundary migration.« less

Grain growth and pore coarsening in dense nano-crystalline UO 2+x fuel pellets

DOE PAGES

Yao, Tiankai; Mo, Kun; Yun, Di; ...

2017-03-25

Dense nano-sized UO 2+x pellets are synthesized by spark plasma sintering with controlled stoichiometries (UO 2.03 and UO 2.11) and grain sizes (~100 nm), and subsequently isothermally annealed to study their effects on grain growth kinetics and microstructure stability. The grain growth kinetics is determined and analyzed focusing on the interaction between grain boundary migration, pore growth and coalescence. Grains grow much bigger in nano-sized UO 2.11 than UO 2.03 upon thermal annealing, consistent with the fact that hyper-stoichiometric UO 2+x is beneficial for sintering due to enhanced U ion diffusion from excessive O ion interstitials. The activation energies ofmore » the grain growth for UO 2.03 and UO 2.11 are determined as ~1.0 and 1.3~2.0 eV, respectively. As compared with the micron-sized UO 2 in which volumetric diffusion dominates the grain coarsening with an activation energy of ~3.0 eV, the enhanced grain growth kinetics in nano-sized UO 2+x suggests that grain boundary diffusion controls grain growth. Lastly, the higher activation energy of more hyper-stoichiometric nano-sized UO 2.11 may be attributed to the excessive O interstitials pinning grain boundary migration.« less

How are the energy waves blocked on the way from hot to cold?

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bai, Xianming; He, Lingfeng; Khafizov, Marat

Representing the Center for Materials Science of Nuclear Fuel (CMSNF), this document is one of the entries in the Ten Hundred and One Word Challenge. As part of the challenge, the 46 Energy Frontier Research Centers were invited to represent their science in images, cartoons, photos, words and original paintings, but any descriptions or words could only use the 1000 most commonly used words in the English language, with the addition of one word important to each of the EFRCs and the mission of DOE energy. The mission of CMSNF to develop an experimentally validated multi-scale computational capability for themore » predictive understanding of the impact of microstructure on thermal transport in nuclear fuel under irradiation, with ultimate application to UO2 as a model system« less

A physical description of fission product behavior fuels for advanced power reactors.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaganas, G.; Rest, J.; Nuclear Engineering Division

2007-10-18

The Global Nuclear Energy Partnership (GNEP) is considering a list of reactors and nuclear fuels as part of its chartered initiative. Because many of the candidate materials have not been explored experimentally under the conditions of interest, and in order to economize on program costs, analytical support in the form of combined first principle and mechanistic modeling is highly desirable. The present work is a compilation of mechanistic models developed in order to describe the fission product behavior of irradiated nuclear fuel. The mechanistic nature of the model development allows for the possibility of describing a range of nuclear fuelsmore » under varying operating conditions. Key sources include the FASTGRASS code with an application to UO{sub 2} power reactor fuel and the Dispersion Analysis Research Tool (DART ) with an application to uranium-silicide and uranium-molybdenum research reactor fuel. Described behavior mechanisms are divided into subdivisions treating fundamental materials processes under normal operation as well as the effect of transient heating conditions on these processes. Model topics discussed include intra- and intergranular gas-atom and bubble diffusion, bubble nucleation and growth, gas-atom re-solution, fuel swelling and ?scion gas release. In addition, the effect of an evolving microstructure on these processes (e.g., irradiation-induced recrystallization) is considered. The uranium-alloy fuel, U-xPu-Zr, is investigated and behavior mechanisms are proposed for swelling in the {alpha}-, intermediate- and {gamma}-uranium zones of this fuel. The work reviews the FASTGRASS kinetic/mechanistic description of volatile ?scion products and, separately, the basis for the DART calculation of bubble behavior in amorphous fuels. Development areas and applications for physical nuclear fuel models are identified.« less

Uranium Dioxides and Debris Fragments Released to the Environment with Cesium-Rich Microparticles from the Fukushima Daiichi Nuclear Power Plant.

PubMed

Ochiai, Asumi; Imoto, Junpei; Suetake, Mizuki; Komiya, Tatsuki; Furuki, Genki; Ikehara, Ryohei; Yamasaki, Shinya; Law, Gareth T W; Ohnuki, Toshihiko; Grambow, Bernd; Ewing, Rodney C; Utsunomiya, Satoshi

2018-03-06

Trace U was released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) during the meltdowns, but the speciation of the released components of the nuclear fuel remains unknown. We report, for the first time, the atomic-scale characteristics of nanofragments of the nuclear fuels that were released from the FDNPP into the environment. Nanofragments of an intrinsic U-phase were discovered to be closely associated with radioactive cesium-rich microparticles (CsMPs) in paddy soils collected ∼4 km from the FDNPP. The nanoscale fuel fragments were either encapsulated by or attached to CsMPs and occurred in two different forms: (i) UO 2+X nanocrystals of ∼70 nm size, which are embedded into magnetite associated with Tc and Mo on the surface and (ii) Isometric (U,Zr)O 2+X nanocrystals of ∼200 nm size, with the U/(U+Zr) molar ratio ranging from 0.14 to 0.91, with intrinsic pores (∼6 nm), indicating the entrapment of vapors or fission-product gases during crystallization. These results document the heterogeneous physical and chemical properties of debris at the nanoscale, which is a mixture of melted fuel and reactor materials, reflecting the complex thermal processes within the FDNPP reactor during meltdown. Still CsMPs are an important medium for the transport of debris fragments into the environment in a respirable form.

Advanced fuels modeling: Evaluating the steady-state performance of carbide fuel in helium-cooled reactors using FRAPCON 3.4

NASA Astrophysics Data System (ADS)

Hallman, Luther, Jr.

Uranium carbide (UC) has long been considered a potential alternative to uranium dioxide (UO2) fuel, especially in the context of Gen IV gas-cooled reactors. It has shown promise because of its high uranium density, good irradiation stability, and especially high thermal conductivity. Despite its many benefits, UC is known to swell at a rate twice that of UO2. However, the swelling phenomenon is not well understood, and we are limited to a weak empirical understanding of the swelling mechanism. One suggested cladding for UC is silicon carbide (SiC), a ceramic that demonstrates a number of desirable properties. Among them are an increased corrosion resistance, high mechanical strength, and irradiation stability. However, with increased temperatures, SiC exhibits an extremely brittle nature. The brittle behavior of SiC is not fully understood and thus it is unknown how SiC would respond to the added stress of a swelling UC fuel. To better understand the interaction between these advanced materials, each has been implemented into FRAPCON, the preferred fuel performance code of the Nuclear Regulatory Commission (NRC); additionally, the material properties for a helium coolant have been incorporated. The implementation of UC within FRAPCON required the development of material models that described not only the thermophysical properties of UC, such as thermal conductivity and thermal expansion, but also models for the swelling, densification, and fission gas release associated with the fuel's irradiation behavior. This research is intended to supplement ongoing analysis of the performance and behavior of uranium carbide and silicon carbide in a helium-cooled reactor.

Oxygen diffusion model of the mixed (U,Pu)O2 ± x: Assessment and application

NASA Astrophysics Data System (ADS)

Moore, Emily; Guéneau, Christine; Crocombette, Jean-Paul

2017-03-01

The uranium-plutonium (U,Pu)O2 ± x mixed oxide (MOX) is used as a nuclear fuel in some light water reactors and considered for future reactor generations. To gain insight into fuel restructuring, which occurs during the fuel lifetime as well as possible accident scenarios understanding of the thermodynamic and kinetic behavior is crucial. A comprehensive evaluation of thermo-kinetic properties is incorporated in a computational CALPHAD type model. The present DICTRA based model describes oxygen diffusion across the whole range of plutonium, uranium and oxygen compositions and temperatures by incorporating vacancy and interstitial migration pathways for oxygen. The self and chemical diffusion coefficients are assessed for the binary UO2 ± x and PuO2 - x systems and the description is extended to the ternary mixed oxide (U,Pu)O2 ± x by extrapolation. A simulation to validate the applicability of this model is considered.

Status Report on the Fabrication of Fuel Cladding Chemical Interaction Test Articles for ATR Irradiations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Field, Kevin G.; Howard, Richard H.

FeCrAl alloys are a promising new class of alloys for light water reactor (LWR) applications due to their superior oxidation and corrosion resistance in high temperature environments. The current R&D efforts have focused on the alloy composition and processing routes to generate nuclear grade FeCrAl alloys with optimized properties for enhanced accident tolerance while maintaining properties needed for normal operation conditions. Therefore, the composition and processing routes must be optimized to maintain the high temperature steam oxidation (typically achieved by increasing the Cr and Al content) while still exhibiting properties conducive to normal operation in a LWR (such as radiationmore » tolerance where reducing Cr content is favorable). Within this balancing act is the addition of understanding the influence on composition and processing routes on the FeCrAl alloys for fuel-cladding chemical interactions (FCCI). Currently, limited knowledge exists on FCCI for the FeCrAl-UO 2 clad-fuel system. To overcome the knowledge gaps on the FCCI for the FeCrAl-UO2 clad-fuel system a series of fueled irradiation tests have been developed for irradiation in the Advanced Test Reactor (ATR) housed at the Idaho National Laboratory (INL). The first series of tests has already been reported. These tests used miniaturized 17x17 PWR fuel geometry rodlets of second-generation FeCrAl alloys fueled with industrial Westinghouse UO 2 fuel. These rodlets were encapsulated within a stainless steel housing.To provide high fidelity experiments and more robust testing, a new series of rodlets have been developed deemed the Accident Tolerant Fuel Experiment #1 Oak Ridge National Laboratory FCCI test (ATF-1 ORNL FCCI). The main driving factor, which is discussed in detail, was to provide a radiation environment where prototypical fuel-clad interface temperatures are met while still maintaining constant contact between industrial fuel and the candidate cladding alloys, hence promoting FCCI between the fuel-clad systems. The other factor was to develop a test bed where multiple candidate alloys could be evaluated within a single irradiation test train, thereby reducing overall costs and increasing efficiency in alloy screening efforts. A collaboration between ORNL and INL was developed to facilitate the completion of the test bed for FCCI testing. The report highlights the activities related to the development of the ATF-1 ORNL FCCI rodlets for irradiation in INL’s ATR as part of the on-going ATF-1 experiments.« less

High temperature investigation of the solid/liquid transition in the PuO2-UO2-ZrO2 system

NASA Astrophysics Data System (ADS)

Quaini, A.; Guéneau, C.; Gossé, S.; Sundman, B.; Manara, D.; Smith, A. L.; Bottomley, D.; Lajarge, P.; Ernstberger, M.; Hodaj, F.

2015-12-01

The solid/liquid transitions in the quaternary U-Pu-Zr-O system are of great interest for the analysis of core meltdown accidents in Pressurised Water Reactors (PWR) fuelled with uranium-dioxide and MOX. During a severe accident the Zr-based cladding can become completely oxidised due to the interaction with the oxide fuel and the water coolant. In this framework, the present analysis is focused on the pseudo-ternary system UO2-PuO2-ZrO2. The melting/solidification behaviour of five pseudo-ternary and one pseudo-binary ((PuO2)0.50(ZrO2)0.50) compositions have been investigated experimentally by a laser heating method under pre-set atmospheres. The effects of an oxidising or reducing atmosphere on the observed melting/freezing temperatures, as well as the amount of UO2 in the sample, have been clearly identified for the different compositions. The oxygen-to-metal ratio is a key parameter affecting the melting/freezing temperature because of incongruent vaporisation effects. In parallel, a detailed thermodynamic model for the UO2-PuO2-ZrO2 system has been developed using the CALPHAD method, and thermodynamic calculations have been performed to interpret the present laser heating results, as well as the high temperature behaviour of the cubic (Pu,U,Zr)O2±x-c mixed oxide phase. A good agreement was obtained between the calculated and experimental data points. This work enables an improved understanding of the major factors relevant to severe accident in nuclear reactors.

Synthesis of phase-pure U 2N 3 microspheres and its decomposition into UN

DOE PAGES

Silva, Chinthaka M.; Hunt, Rodney Dale; Snead, Lance Lewis; ...

2014-12-12

Uranium mononitride (UN) is important as a nuclear fuel. Fabrication of UN in its microspherical form also has its own merits since the advent of the concept of accident-tolerant fuel, where UN is being considered as a potential fuel in the form of TRISO particles. But, not many processes have been well established to synthesize kernels of UN. Therefore, a process for synthesis of microspherical UN with a minimum amount of carbon is discussed herein. First, a series of single-phased microspheres of uranium sesquinitride (U 2N 3) were synthesized by nitridation of UO 2+C microspheres at a few different temperatures.more » Resulting microspheres were of low-density U 2N 3 and decomposed into low-density UN. The variation of density of the synthesized sesquinitrides as a function of its chemical composition indicated the presence of extra (interstitial) nitrogen atoms corresponding to its hyperstoichiometry, which is normally indicated as α-U 2N 3. Average grain sizes of both U 2N 3 and UN varied in a range of 1–2.5 μm. In addition, these had a considerably large amount of pore spacing, indicating the potential sinterability of UN toward its use as a nuclear fuel.« less

Use of UO 2 films for electrochemical studies

NASA Astrophysics Data System (ADS)

Miserque, F.; Gouder, T.; Wegen, D. H.; Bottomley, P. D. W.

2001-10-01

UO 2 films have been prepared by dc reactive sputtering of a uranium metal target in an Ar/O 2 atmosphere. We have used the films deposited on gold substrates as working electrodes for electrochemical investigations as simulating the surfaces of fuel pellets. Film composition was determined by photoelectron spectroscopy (XPS and UPS) and X-ray diffraction (XRD). The oxide stoichiometry as a function of deposition conditions was determined and the appropriate conditions for UO 2.0 formation established. AC impedance and cyclic voltammetry measurements were performed. A double RC electrical equivalent circuit was used to fit the data from impedance measurements, similar to those used in unirradiated UO 2 or spent fuel pellets. However due to the porosity or adhesion defects on the thin films that permitted a direct contact between the solution and the gold substrate, we were obliged to add a contribution simulating the water-gold system. Cyclic voltammetry measurements show the influence of pH on the dissolution mechanism. Alkaline solutions permit the formation of an oxidised layer (UO 2.33) which is not present in the acidic solutions. In both pH=2 and pH=6 solutions, a U VI species layer is formed.

TOF-SIMS for Rapid Nuclear Forensics Evaluation of Uranium Oxide Particles

DTIC Science & Technology

2011-03-01

Fraction U-238 nU U metal CRM 112-A NBL Metal Assay and Isotopic .000052458 .0072017 --- .9927458 nUO2 UO2 --- NBL Commercial material...0 .992745 dU U metal CRM 115 NBL Uranium Assay .0000076 .0020291 .0000322 .9979311 dUO2 UO2 --- IBI Labs Commercial material --- .002- .0035...U500* U3O8 CRM U500 NBL Isotopic .005181 .49696 .000755 .49711 U900* U3O8 CRM U900 NBL Isotopic .007777 .90196 .003327 .08693 *Sample

Design and synthesis of target-responsive hydrogel for portable visual quantitative detection of uranium with a microfluidic distance-based readout device.

PubMed

Huang, Yishun; Fang, Luting; Zhu, Zhi; Ma, Yanli; Zhou, Leiji; Chen, Xi; Xu, Dunming; Yang, Chaoyong

2016-11-15

Due to uranium's increasing exploitation in nuclear energy and its toxicity to human health, it is of great significance to detect uranium contamination. In particular, development of a rapid, sensitive and portable method is important for personal health care for those who frequently come into contact with uranium ore mining or who investigate leaks at nuclear power plants. The most stable form of uranium in water is uranyl ion (UO2(2+)). In this work, a UO2(2+) responsive smart hydrogel was designed and synthesized for rapid, portable, sensitive detection of UO2(2+). A UO2(2+) dependent DNAzyme complex composed of substrate strand and enzyme strand was utilized to crosslink DNA-grafted polyacrylamide chains to form a DNA hydrogel. Colorimetric analysis was achieved by encapsulating gold nanoparticles (AuNPs) in the DNAzyme-crosslinked hydrogel to indicate the concentration of UO2(2+). Without UO2(2+), the enzyme strand is not active. The presence of UO2(2+) in the sample activates the enzyme strand and triggers the cleavage of the substrate strand from the enzyme strand, thereby decreasing the density of crosslinkers and destabilizing the hydrogel, which then releases the encapsulated AuNPs. As low as 100nM UO2(2+) was visually detected by the naked eye. The target-responsive hydrogel was also demonstrated to be applicable in natural water spiked with UO2(2+). Furthermore, to avoid the visual errors caused by naked eye observation, a previously developed volumetric bar-chart chip (V-Chip) was used to quantitatively detect UO2(2+) concentrations in water by encapsulating Au-Pt nanoparticles in the hydrogel. The UO2(2+) concentrations were visually quantified from the travelling distance of ink-bar on the V-Chip. The method can be used for portable and quantitative detection of uranium in field applications without skilled operators and sophisticated instruments. Copyright © 2016 Elsevier B.V. All rights reserved.

Development code for sensitivity and uncertainty analysis of input on the MCNPX for neutronic calculation in PWR core

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hartini, Entin, E-mail: entin@batan.go.id; Andiwijayakusuma, Dinan, E-mail: entin@batan.go.id

2014-09-30

This research was carried out on the development of code for uncertainty analysis is based on a statistical approach for assessing the uncertainty input parameters. In the butn-up calculation of fuel, uncertainty analysis performed for input parameters fuel density, coolant density and fuel temperature. This calculation is performed during irradiation using Monte Carlo N-Particle Transport. The Uncertainty method based on the probabilities density function. Development code is made in python script to do coupling with MCNPX for criticality and burn-up calculations. Simulation is done by modeling the geometry of PWR terrace, with MCNPX on the power 54 MW with fuelmore » type UO2 pellets. The calculation is done by using the data library continuous energy cross-sections ENDF / B-VI. MCNPX requires nuclear data in ACE format. Development of interfaces for obtaining nuclear data in the form of ACE format of ENDF through special process NJOY calculation to temperature changes in a certain range.« less

Nuclear Waste Package Mockups: A Study of In-situ Redox State

NASA Astrophysics Data System (ADS)

Helean, K.; Anderson, B.; Brady, P. V.

2006-05-01

The Yucca Mountain Repository (YMR), located in southern Nevada, is to be the first facility in the U.S. for the permanent disposal of high-level radioactive waste and spent nuclear fuels. Total system performance assessment(TSPA) has indicated that among the major radionuclides contributing to dose are Np, Tc, and I. These three radionuclides are mobile in most geochemical settings, and therefore sequestering them within the repository horizon is a priority for the Yucca Mountain Project (YMP). Corroding steel may offset radionuclide transport processes within the proposed waste packages at YMR by retaining radionuclides, creating locally reducing conditions, and reducing porosity. Ferrous iron has been shown to reduce UO22+ to UO2s, and some ferrous iron-bearing ion-exchange materials have been shown to adsorb radionuclides and heavy metals. Locally reducing conditions may lead to the reduction and subsequent immobilization of problematic dissolved species such as TcO4-, NpO2+, and UO22+ and can also inhibit corrosion of spent nuclear fuel. Water occluded during corrosion produces bulky corrosion products, and consequently less porosity is available for water and radionuclide transport. The focus of this study is on the nature of Yucca Mountain waste package corrosion products and their effects on local redox conditions, radionuclide transport, and porosity. In order to measure in-situ redox, six small-scale (1:40) waste package mockups were constructed using A516 and 316 stainless steel, the same materials as the proposed Yucca Mountain waste packages. The mockups are periodically injected with a simulated groundwater and the accumulated effluent and corrosion products are evaluated for their Fe(II)/Fe(III) content and mineralogy. Oxygen fugacities are then calculated and, thus, in-situ redox conditions are determined. Early results indicate that corrosion products are largely amorphous Fe-oxyhydroxides, goethite and magnetite. That information together with the measured Fe(II)/Fe(III) ratios in the mockup effluent constrain the oxygen fugacity to approximately 10-38 atm, many orders of magnitude below ambient. These results and their impact on radionuclide migration from YMR will be discussed.

Recent advances in the study of the UO2-PuO2 phase diagram at high temperatures

NASA Astrophysics Data System (ADS)

Böhler, R.; Welland, M. J.; Prieur, D.; Cakir, P.; Vitova, T.; Pruessmann, T.; Pidchenko, I.; Hennig, C.; Guéneau, C.; Konings, R. J. M.; Manara, D.

2014-05-01

Recently, novel container-less laser heating experimental data have been published on the melting behaviour of pure PuO2 and PuO2-rich compositions in the uranium dioxide-plutonium dioxide system. Such data showed that previous data obtained by more traditional furnace heating techniques were affected by extensive interaction between the sample and its containment. It is therefore paramount to check whether data so far used by nuclear engineers for the uranium-rich side of the pseudo-binary dioxide system can be confirmed or not. In the present work, new data are presented both in the UO2-rich part of the phase diagram, most interesting for the uranium-plutonium dioxide based nuclear fuel safety, and in the PuO2 side. The new results confirm earlier furnace heating data in the uranium-dioxide rich part of the phase diagram, and more recent laser-heating data in the plutonium-dioxide side of the system. As a consequence, it is also confirmed that a minimum melting point must exist in the UO2-PuO2 system, at a composition between x(PuO2) = 0.4 and x(PuO2) = 0.7 and 2900 K ⩽ T ⩽ 3000 K. Taking into account that, especially at high temperature, oxygen chemistry has an effect on the reported phase boundary uncertainties, the current results should be projected in the ternary U-Pu-O system. This aspect has been extensively studied here by X-ray diffraction and X-ray absorption spectroscopy. The current results suggest that uncertainty bands related to oxygen behaviour in the equilibria between condensed phases and gas should not significantly affect the qualitative trend of the current solid-liquid phase boundaries.

Initial results from safety testing of US AGR-2 irradiation test fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Morris, Robert Noel; Hunn, John D.; Baldwin, Charles A.

Two cylindrical compacts containing tristructural isotropic (TRISO)-coated particles with kernels that contained a mixture of uranium carbide and uranium oxide (UCO) and two compacts with UO 2-kernel TRISO particles have undergone 1600°C safety testing. These compacts were irradiated in the US Advanced Gas Reactor Fuel Development and Qualification Program's second irradiation test (AGR-2). The time-dependent releases of several radioisotopes ( 110mAg, 134Cs, 137Cs, 154Eu, 155Eu, 90Sr, and 85Kr) were monitored while heating the fuel specimens to 1600°C in flowing helium for 300 h. The UCO compacts behaved similarly to previously reported 1600°C-safety-tested UCO compacts from the AGR-1 irradiation. No failedmore » TRISO or failed SiC were detected (based on krypton and cesium release), and cesium release through intact SiC was very low. Release behavior of silver, europium, and strontium appeared to be dominated by inventory originally released through intact coating layers during irradiation but retained in the compact matrix until it was released during safety testing. Both UO 2 compacts exhibited cesium release from multiple particles whose SiC failed during the safety test. Europium and strontium release from these two UO 2 compacts appeared to be dominated by release from the particles with failed SiC. Silver release was characteristically like the release from the UCO compacts in that an initial release of the majority of silver trapped in the matrix occurred during ramping to 1600°C. However, additional silver release was observed later in the safety testing due to the UO 2 TRISO with failed SiC. Failure of the SiC layer in the UO 2 fuel appears to have been dominated by CO corrosion, as opposed to the palladium degradation observed in AGR-1 UCO fuel.« less

Initial results from safety testing of US AGR-2 irradiation test fuel

DOE PAGES

Morris, Robert Noel; Hunn, John D.; Baldwin, Charles A.; ...

2017-08-18

Two cylindrical compacts containing tristructural isotropic (TRISO)-coated particles with kernels that contained a mixture of uranium carbide and uranium oxide (UCO) and two compacts with UO 2-kernel TRISO particles have undergone 1600°C safety testing. These compacts were irradiated in the US Advanced Gas Reactor Fuel Development and Qualification Program's second irradiation test (AGR-2). The time-dependent releases of several radioisotopes ( 110mAg, 134Cs, 137Cs, 154Eu, 155Eu, 90Sr, and 85Kr) were monitored while heating the fuel specimens to 1600°C in flowing helium for 300 h. The UCO compacts behaved similarly to previously reported 1600°C-safety-tested UCO compacts from the AGR-1 irradiation. No failedmore » TRISO or failed SiC were detected (based on krypton and cesium release), and cesium release through intact SiC was very low. Release behavior of silver, europium, and strontium appeared to be dominated by inventory originally released through intact coating layers during irradiation but retained in the compact matrix until it was released during safety testing. Both UO 2 compacts exhibited cesium release from multiple particles whose SiC failed during the safety test. Europium and strontium release from these two UO 2 compacts appeared to be dominated by release from the particles with failed SiC. Silver release was characteristically like the release from the UCO compacts in that an initial release of the majority of silver trapped in the matrix occurred during ramping to 1600°C. However, additional silver release was observed later in the safety testing due to the UO 2 TRISO with failed SiC. Failure of the SiC layer in the UO 2 fuel appears to have been dominated by CO corrosion, as opposed to the palladium degradation observed in AGR-1 UCO fuel.« less

Uranium luminescence in La2 Zr2 O7 : effect of concentration and annealing temperature.

PubMed

Mohapatra, M; Rajeswari, B; Hon, N S; Kadam, R M

2016-12-01

The speciation of a particular element in any given matrix is a prerequisite to understanding its solubility and leaching properties. In this context, speciation of uranium in lanthanum zirconate pyrochlore (La 2 Zr 2 O 7  = LZO), prepared by a low-temperature combustion route, was carried out using a simple photoluminescence lifetime technique. The LZO matrix is considered to be a potential ceramic host for fixing nuclear and actinide waste products generated during the nuclear fuel cycle. Special emphasis has been given to understanding the dynamics of the uranium species in the host as a function of annealing temperature and concentration. It was found that, in the LZO host, uranium is stabilized as the commonly encountered uranyl species (UO 2 2+ ) up to a heat treatment of 500 °C at the surface. Above 500 °C, the uranyl ion is diffused into the matrix as the more symmetric octahedral uranate species (UO 6 6- ). The uranate ions thus formed replace the six-coordinated 'Zr' atoms at regular lattice positions. Further, it was observed that concentration quenching takes place beyond 5 mol% of uranium doping. The mechanism of the quenching was found to be a multipolar interaction. Copyright © 2016 John Wiley & Sons, Ltd. Copyright © 2016 John Wiley & Sons, Ltd.

Fabrication of high exposure nuclear fuel pellets

DOEpatents

Frederickson, James R.

1987-01-01

A method is disclosed for making a fuel pellet for a nuclear reactor. A mixture is prepared of PuO.sub.2 and UO.sub.2 powders, where the mixture contains at least about 30% PuO.sub.2, and where at least about 12% of the Pu is the Pu.sup.240 isotope. To this mixture is added about 0.3 to about 5% of a binder having a melting point of at least about 250.degree. F. The mixture is pressed to form a slug and the slug is granulated. Up to about 4.7% of a lubricant having a melting point of at least about 330.degree. F. is added to the granulated slug. Both the binder and the lubricant are selected from a group consisting of polyvinyl carboxylate, polyvinyl alcohol, naturally occurring high molecular weight cellulosic polymers, chemically modified high molecular weight cellulosic polymers, and mixtures thereof. The mixture is pressed to form a pellet and the pellet is sintered.

Status Report on Irradiation Capsules Designed to Evaluate FeCrAl-UO 2 Interactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Field, Kevin G.; Howard, Richard H.

This status report provides the background and current status of a series of irradiation capsules that were designed and are being built to test the interactions between candidate FeCrAl cladding for enhanced accident tolerant applications and prototypical enriched commercial UO 2 fuel in a neutron radiation environment. These capsules will test the degree, if any, of fuel cladding chemical interactions (FCCI) between FeCrAl and UO 2. The capsules are to be irradiated in the Advanced Test Reactor (ATR) at Idaho National Laboratory to burn-ups of 10, 30, and 50 GWd/MT with a nominal target temperature at the interfaces between themore » pellets and clad of 350°C.« less

Probing the oxygen environment in UO(2)(2+) by solid-state 17O nuclear magnetic resonance spectroscopy and relativistic density functional calculations.

PubMed

Cho, Herman; de Jong, Wibe A; Soderquist, Chuck Z

2010-02-28

A combined theoretical and solid-state (17)O nuclear magnetic resonance (NMR) study of the electronic structure of the uranyl ion UO(2)(2+) in (NH(4))(4)UO(2)(CO(3))(3) and rutherfordine (UO(2)CO(3)) is presented, the former representing a system with a hydrogen-bonding environment around the uranyl oxygens and the latter exemplifying a uranyl environment without hydrogens. Relativistic density functional calculations reveal unique features of the U-O covalent bond, including the finding of (17)O chemical shift anisotropies that are among the largest for oxygen ever reported (>1200 ppm). Computational results for the oxygen electric field gradient tensor are found to be consistently larger in magnitude than experimental solid-state (17)O NMR measurements in a 7.05 T magnetic field indicate. A modified version of the Solomon theory of the two-spin echo amplitude for a spin-5/2 nucleus is developed and applied to the analysis of the (17)O echo signal of U (17)O(2)(2+).

Oxidative Corrosion of the UO 2 (001) Surface by Nonclassical Diffusion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stubbs, Joanne E.; Biwer, Craig A.; Chaka, Anne M.

Uranium oxide is central to every stage of the nuclear fuel cycle, from mining through fuel fabrication and use, to waste disposal and environmental cleanup. Its chemical and mechanical stability are intricately linked to the concentration of interstitial O atoms within the structure and the oxidation state of U. We have previously shown that during corrosion of the UO2 (111) surface under either 1 atm O2 gas or oxygenated water at room temperature, oxygen interstitials diffuse into the substrate to form a superlattice with three-layer periodicity. In the current study, we present results from surface x-ray scattering that reveal themore » structure of the oxygen diffusion profile beneath the (001) surface. The first few layers below the surface oscillate strongly in their surface-normal lattice parameters, suggesting preferential interstitial occupation of every other layer below the surface, which is geometrically consistent with the interstitial network that forms below the oxidized (111) surface. Deeper layers are heavily contracted and indicate that the oxidation front penetrates ~52 Å below the (001) surface after 21 days of dry O2 gas exposure at ambient pressure and temperature. X-ray photoelectron spectroscopy indicates U is present as U(IV), U(V), and U(VI).« less

PUREX/UO{sub 3} deactivation project management plan

DOE Office of Scientific and Technical Information (OSTI.GOV)

Washenfelder, D.J.

1993-12-01

From 1955 through 1990, the Plutonium-Uranium Extraction Plant (PUREX) provided the United States Department of Energy Hanford Site with nuclear fuel reprocessing capability. It operated in sequence with the Uranium Trioxide (UO{sub 3}) Plant, which converted the PUREX liquid uranium nitrate product to solid UO{sub 3} powder. Final UO{sub 3} Plant operation ended in 1993. In December 1992, planning was initiated for the deactivation of PUREX and UO{sub 3} Plant. The objective of deactivation planning was to identify the activities needed to establish a passively safe, environmentally secure configuration at both plants, and ensure that the configuration could be retainedmore » during the post-deactivation period. The PUREX/UO{sub 3} Deactivation Project management plan represents completion of the planning efforts. It presents the deactivation approach to be used for the two plants, and the supporting technical, cost, and schedule baselines. Deactivation activities concentrate on removal, reduction, and stabilization of the radioactive and chemical materials remaining at the plants, and the shutdown of the utilities and effluents. When deactivation is completed, the two plants will be left unoccupied and locked, pending eventual decontamination and decommissioning. Deactivation is expected to cost $233.8 million, require 5 years to complete, and yield $36 million in annual surveillance and maintenance cost savings.« less

Neutronics Analysis of SMART Small Modular Reactor using SRAC 2006 Code

NASA Astrophysics Data System (ADS)

Ramdhani, Rahmi N.; Prastyo, Puguh A.; Waris, Abdul; Widayani; Kurniadi, Rizal

2017-07-01

Small modular reactors (SMRs) are part of a new generation of nuclear reactor being developed worldwide. One of the advantages of SMR is the flexibility to adopt the advanced design concepts and technology. SMART (System integrated Modular Advanced ReacTor) is a small sized integral type PWR with a thermal power of 330 MW that has been developed by KAERI (Korea Atomic Energy Research Institute). SMART core consists of 57 fuel assemblies which are based on the well proven 17×17 array that has been used in Korean commercial PWRs. SMART is soluble boron free, and the high initial reactivity is mainly controlled by burnable absorbers. The goal of this study is to perform neutronics evaluation of SMART core with UO2 as main fuel. Neutronics calculation was performed by using PIJ and CITATION modules of SRAC 2006 code with JENDL 3.3 as nuclear data library.

Investigating microstructural evolution during the electroreduction of UO2 to U in LiCl-KCl eutectic using focused ion beam tomography

NASA Astrophysics Data System (ADS)

Brown, L. D.; Abdulaziz, R.; Tjaden, B.; Inman, D.; Brett, D. J. L.; Shearing, P. R.

2016-11-01

Reprocessing of spent nuclear fuels using molten salt media is an attractive alternative to liquid-liquid extraction techniques. Pyroelectrochemical processing utilizes direct, selective, electrochemical reduction of uranium dioxide, followed by selective electroplating of a uranium metal. Thermodynamic prediction of the electrochemical reduction of UO2 to U in LiCl-KCl eutectic has shown to be a function of the oxide ion activity. The pO2- of the salt may be affected by the microstructure of the UO2 electrode. A uranium dioxide filled "micro-bucket" electrode has been partially electroreduced to uranium metal in molten lithium chloride-potassium chloride eutectic. This partial electroreduction resulted in two distinct microstructures: a dense UO2 and a porous U metal structure were characterised by energy dispersive X-ray spectroscopy. Focused ion beam tomography was performed on five regions of this electrode which revealed an overall porosity ranging from 17.36% at the outer edge to 3.91% towards the centre, commensurate with the expected extent of reaction in each location. The pore connectivity was also seen to reduce from 88.32% to 17.86% in the same regions and the tortuosity through the sample was modelled along the axis of propagation of the electroreduction, which was seen to increase from a value of 4.42 to a value of infinity (disconnected pores). These microstructural characteristics could impede the transport of O2- ions resulting in a change in the local pO2- which could result in the inability to perform the electroreduction.

Spent fuel radionuclide source-term model for assessing spent fuel performance in geological disposal. Part I: Assessment of the instant release fraction

NASA Astrophysics Data System (ADS)

Johnson, Lawrence; Ferry, Cécile; Poinssot, Christophe; Lovera, Patrick

2005-11-01

A source-term model for the short-term release of radionuclides from spent nuclear fuel (SNF) has been developed. It provides quantitative estimates of the fraction of various radionuclides that are expected to be released rapidly (the instant release fraction, or IRF) when water contacts the UO 2 or MOX fuel after container breaching in a geological repository. The estimates are based on correlation of leaching data for radionuclides with fuel burnup and fission gas release. Extrapolation of the data to higher fuel burnup values is based on examination of data on fuel restructuring, such as rim development, and on fission gas release data, which permits bounding IRF values to be estimated assuming that radionuclide releases will be less than fission gas release. The consideration of long-term solid-state changes influencing the IRF prior to canister breaching is addressed by evaluating alpha self-irradiation enhanced diffusion, which may gradually increase the accumulation of fission products at grain boundaries.

The effect of fission-energy Xe ion irradiation on the structural integrity and dissolution of the CeO2 matrix

NASA Astrophysics Data System (ADS)

Popel, A. J.; Le Solliec, S.; Lampronti, G. I.; Day, J.; Petrov, P. K.; Farnan, I.

2017-02-01

This work considers the effect of fission fragment damage on the structural integrity and dissolution of the CeO2 matrix in water, as a simulant for the UO2 matrix of spent nuclear fuel. For this purpose, thin films of CeO2 on Si substrates were produced and irradiated by 92 MeV 129Xe23+ ions to a fluence of 4.8 × 1015 ions/cm2 to simulate fission damage that occurs within nuclear fuels along with bulk CeO2 samples. The irradiated and unirradiated samples were characterised and a static batch dissolution experiment was conducted to study the effect of the induced irradiation damage on dissolution of the CeO2 matrix. Complex restructuring took place in the irradiated films and the irradiated samples showed an increase in the amount of dissolved cerium, as compared to the corresponding unirradiated samples. Secondary phases were also observed on the surface of the irradiated CeO2 films after the dissolution experiment.

Modelling explicit fracture of nuclear fuel pellets using peridynamics

NASA Astrophysics Data System (ADS)

Mella, R.; Wenman, M. R.

2015-12-01

Three dimensional models of explicit cracking of nuclear fuel pellets for a variety of power ratings have been explored with peridynamics, a non-local, mesh free, fracture mechanics method. These models were implemented in the explicitly integrated molecular dynamics code LAMMPS, which was modified to include thermal strains in solid bodies. The models of fuel fracture, during initial power transients, are shown to correlate with the mean number of cracks observed on the inner and outer edges of the pellet, by experimental post irradiation examination of fuel, for power ratings of 10 and 15 W g-1 UO2. The models of the pellet show the ability to predict expected features such as the mid-height pellet crack, the correct number of radial cracks and initiation and coalescence of radial cracks. This work presents a modelling alternative to empirical fracture data found in many fuel performance codes and requires just one parameter of fracture strain. Weibull distributions of crack numbers were fitted to both numerical and experimental data using maximum likelihood estimation so that statistical comparison could be made. The findings show P-values of less than 0.5% suggesting an excellent agreement between model and experimental distributions.

Assessing ligand selectivity for uranium over vanadium ions to aid in the discovery of superior adsorbents for extraction of UO 2 2+ from seawater

DOE PAGES

Ivanov, Alexander S.; Bryantsev, Vyacheslav S.

2016-06-06

Uranium is used as the basic fuel for nuclear power plants, which generate significant amounts of electricity and have life cycle carbon emissions that are as low as renewable energy sources. However, the extraction of this valuable energy commodity from the ground remains controversial, mainly because of environmental and health impacts. Alternatively, seawater offers an enormous uranium resource that may be tapped at minimal environmental cost. Nowadays, amidoxime polymers are the most widely utilized sorbent materials for large-scale extraction of uranium from seawater, but they are not perfectly selective for uranyl, UO 2 2+. In particular, the competition between UOmore » 2 2+ and VO 2+/VO2+ cations poses a significant challenge to the effi-cient mining of UO 2 2+. Thus, screening and rational design of more selective ligands must be accomplished. One of the key components in achieving this goal is the establishment of computational techniques capable of assessing ligand selec-tivity trends. Here, we report an approach based on quantum chemical calculations that achieves high accuracy in repro-ducing experimental aqueous stability constants for VO 2+/VO 2+ complexes with ten different oxygen donor lig-ands. The predictive power of the developed computational protocol was demonstrated for amidoxime-type ligands, providing greater insights into new design strategies for the development of the next generation of adsorbents with high selectivity toward UO 2 2+over VO 2+/VO 2+ ions. Furthermore, the results of calculations suggest that alkylation of amidox-ime moieties present in poly(acrylamidoxime) sorbents can be a potential route to better discrimination between the uranyl and competing vanadium ions within seawater.« less

On the nature of the phase transition in uranium dioxide

NASA Astrophysics Data System (ADS)

Gofryk, K.; Mast, D.; Antonio, D.; Shrestha, K.; Andersson, D.; Stanek, C.; Jaime, M.

Uranium dioxide (UO2) is by far the most studied actinide material as it is a primary fuel used in light water nuclear reactors. Its thermal and magnetic properties remain, however, a puzzle resulting from strong couplings between magnetism and lattice vibrations. UO2 crystalizes in the face-centered-cubic fluorite structure and is a Mott-Hubbard insulator with well-localized uranium 5 f-electrons. In addition, below 30 K, a long range antiferromagnetic ordering of the electric-quadrupole of the uranium moments is observed, forming complex non-collinear 3-k magnetic structure. This transition is accompanied by Jahn-Teller distortion of oxygen atoms. It is believed that the first order nature of the transition results from the competition between the exchange interaction and the Jahn-Teller distortion. Here we present results of our extensive thermodynamic investigations on well-characterized and oriented single crystals of UO2+x (x = 0, 0.033, 0.04, and 0.11). By focusing on the transition region under applied magnetic field we are able to study the interplay between different competing interactions (structural, magnetic, and electrical), its dynamics, and relationship to the oxygen content. We will discuss implications of these results. Work supported by the Department of Energy, Office of Basic Energy Sciences, Materials Sciences, and Engineering Division.

Fission products and nuclear fuel behaviour under severe accident conditions part 1: Main lessons learnt from the first VERDON test

NASA Astrophysics Data System (ADS)

Pontillon, Y.; Geiger, E.; Le Gall, C.; Bernard, S.; Gallais-During, A.; Malgouyres, P. P.; Hanus, E.; Ducros, G.

2017-11-01

This paper describes the first VERDON test performed at the end of September 2011 with special emphasis on the behaviour of fission products (FP) and actinides during the accidental sequence itself. Two other papers discuss in detail the post-test examination results (SEM, EPMA and SIMS) of the VERDON-1 sample. The first VERDON test was devoted to studying UO2 fuel behaviour and fission product releases under reducing conditions at very high temperature (∼2883 K), which was able to confirm the very good performance of the VERDON loop. The fuel sample did not lose its integrity during this test. According to the FP behaviour measured by the online gamma station (fuel sight), the general classification of the FP in relation to their released fraction is very accurate, and the burn-up effect on the release rate is clearly highlighted.

Performance of U3Si2 Fuel in a Reactivity Insertion Accident

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cheng, Lap Y.; Cuadra, Arantxa; Todosow, Michael

In this study we examined the performance of the U3Si2 fuel cladded with Zircaloy (Zr) in a reactivity insertion accident (RIA) in a PWR core. The power excursion as a result of a $1 reactivity insertion was calculated by a TRACE PWR plant model using point-kinetics, for alternative cores with UO2 and U3Si2 fuel assemblies. The point-kinetics parameters (feedback coefficients, prompt-neutron lifetime and group constants for six delayed-neutron groups) were obtained from beginning-of-cycle equilibrium full core calculations with PARCS. In the PARCS core calculations, the few-group parameters were developed utilizing the TRITON/NEWT tools in the SCALE package. In order tomore » assess the fuel response in finer detail (e.g. the maximum fuel temperature) the power shape and thermal boundary conditions from the TRACE/PARCS calculations were used to drive a BISON model of a fuel pin with U3Si2 and UO2 respectively. For a $1 reactivity transient both TRACE and BISON predicted a higher maximum fuel temperature for the UO2 fuel than the U3Si2 fuel. Furthermore, BISON is noted to calculate a narrower gap and a higher gap heat transfer coefficient than TRACE. This resulted in BISON predicting consistently lower fuel temperatures than TRACE. This study also provides a systematic comparison between TRACE and BISON using consistent transient boundary conditions. The TRACE analysis of the RIA only reflects the core-wide response in power. A refinement to the analysis would be to predict the local peaking in a three-dimensional core as a result of control rod ejection.« less

Small Reactor Designs Suitable for Direct Nuclear Thermal Propulsion: Interim Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bruce G. Schnitzler

Advancement of U.S. scientific, security, and economic interests requires high performance propulsion systems to support missions beyond low Earth orbit. A robust space exploration program will include robotic outer planet and crewed missions to a variety of destinations including the moon, near Earth objects, and eventually Mars. Past studies, in particular those in support of both the Strategic Defense Initiative (SDI) and the Space Exploration Initiative (SEI), have shown nuclear thermal propulsion systems provide superior performance for high mass high propulsive delta-V missions. In NASA's recent Mars Design Reference Architecture (DRA) 5.0 study, nuclear thermal propulsion (NTP) was again selectedmore » over chemical propulsion as the preferred in-space transportation system option for the human exploration of Mars because of its high thrust and high specific impulse ({approx}900 s) capability, increased tolerance to payload mass growth and architecture changes, and lower total initial mass in low Earth orbit. The recently announced national space policy2 supports the development and use of space nuclear power systems where such systems safely enable or significantly enhance space exploration or operational capabilities. An extensive nuclear thermal rocket technology development effort was conducted under the Rover/NERVA, GE-710 and ANL nuclear rocket programs (1955-1973). Both graphite and refractory metal alloy fuel types were pursued. The primary and significantly larger Rover/NERVA program focused on graphite type fuels. Research, development, and testing of high temperature graphite fuels was conducted. Reactors and engines employing these fuels were designed, built, and ground tested. The GE-710 and ANL programs focused on an alternative ceramic-metallic 'cermet' fuel type consisting of UO2 (or UN) fuel embedded in a refractory metal matrix such as tungsten. The General Electric program examined closed loop concepts for space or terrestrial applications as well as open loop systems for direct nuclear thermal propulsion. Although a number of fast spectrum reactor and engine designs suitable for direct nuclear thermal propulsion were proposed and designed, none were built. This report summarizes status results of evaluations of small nuclear reactor designs suitable for direct nuclear thermal propulsion.« less

PATHFINDER ATOMIC POWER PLANT TECHNICAL PROGRESS REPORT FOR JULY 1, 1959- SEPTEMBER 30, 1959

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

1960-10-31

ABS>Fuel Element Research and Development. Dynamic and static corrosion tests on 8001 Al were completed. Annealmmmg of 1100 cladding on 5083 and M400 cladding on X2219 were tested at 500 deg C, and investigation continued on producing X8101 Al alloy cladding in tube plates by extrusion. Boiler fuel element capsule irradiation tests and subassembly tests are described Heat transfer loop studies and fuel fabrication for the critical facility are reported. Boiler fuel element mechanical design and testing progress is desc ribed. and the superheater fuel element temperature evaluating routine is discussed. Low- enrichment superheater fuel element development included design studiesmore » and stainless steel powder and UO/sub 2/ powder fabrication studies Reactor Mechanical Studies. Research is reported on vessel and structure design, fabrication, and testing, recirculation system design, steam separator tests, and control rod studies. Nuclear Analysis. Reactor physics studies are reported on nuclear constants, baffle plate analysis, comparison of core representations, delayed neutron fraction. and shielding analysis of the reactor building. Reactor and system dynamics and critical experiments were also studied. Chemistry. Progress is reported on recombiner. radioactive gas removal and storage, ion exchanger and radiochemical processing. (For preceding period see ACNP-5915.) (T.R.H.)« less

Phase equilibria in the UO 2-PuO 2 system under a temperature gradient

NASA Astrophysics Data System (ADS)

Kleykamp, Heiko

2001-04-01

The phase behaviour of U 0.80Pu 0.20O 1.95 was investigated under a steady-state temperature gradient between the solidus and liquidus by a short-time power-to-melt irradiation experiment. The radial U, Pu, Am and O profiles in the fuel pin after redistribution were measured by X-ray microanalysis. During irradiation, an inner fuel melt forms which is separated from the outer solid only by one concentric liquid-solid-phase boundary. The UO 2 concentration increases to 85% and the PuO 2 concentration decreases to 15% on the solid side of the interface. Opposite gradients occur on the liquid side of the interface. The concentration discontinuity is a consequence of the necessary equality of the chemical potentials of UO 2 and PuO 2 on both sides of the phase boundary which corresponds to a 2750°C isotherm. The radial oxygen profile results in an O/(U + Pu) ratio of 2.00 at the fuel surface and 1.92 at the central void of the fuel. The redistribution is caused by the thermal diffusion of oxygen vacancies in the lattice along the temperature gradient. This process is quantified by the heat of transport Q*v which ranges between -10 kJ/mol at the central void and about -230 kJ/mol near the fuel surface.

TEM Characterization of High Burn-up Microstructure of U-7Mo Alloy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jian Gan; Brandon Miller; Dennis Keiser

2014-04-01

As an essential part of global nuclear non-proliferation effort, the RERTR program is developing low enriched U-Mo fuels (< 20% U-235) for use in research and test reactors that currently employ highly enriched uranium fuels. One type of fuel being developed is a dispersion fuel plate comprised of U-7Mo particles dispersed in Al alloy matrix. Recent TEM characterizations of the ATR irradiated U-7Mo dispersion fuel plates include the samples with a local fission densities of 4.5, 5.2, 5.6 and 6.3 E+21 fissions/cm3 and irradiation temperatures of 101-136?C. The development of the irradiated microstructure of the U-7Mo fuel particles consists ofmore » fission gas bubble superlattice, large gas bubbles, solid fission product precipitates and their association to the large gas bubbles, grain subdivision to tens or hundreds of nanometer size, collapse of bubble superlattice, and amorphisation. This presentation will describe the observed microstructures specifically focusing on the U-7Mo fuel particles. The impact of the observed microstructure on the fuel performance and the comparison of the relevant features with that of the high burn-up UO2 fuels will be discussed.« less

Cryochemical and CVD processing of shperical carbide fuels for propulsion reactors

NASA Astrophysics Data System (ADS)

Blair, H. Thomas; Carroll, David W.; Matthews, R. Bruce

1991-01-01

Many of the nuclear propulsion reactor concepts proposed for a manned mission to Mars use a coated spherical particle fuel form similar to that used in the Rover and NERVA propulsion reactors. The formation of uranium dicarbide microspheres using a cryochemical process and the coating of the UC2 spheres with zirconium carbide using chemical vapor deposition are being developed at Los Alamos National Laboratory. The cryochemical process is described with a discussion of the variables affecting the sphere formation and carbothermic reduction to produce UC2 spheres from UO2. Emphasis is placed on minimizing the wastes produced by the process. The ability to coat particles with ZrC was recaptured, and improvements in the process and equipment were developed. Volatile organometallic precursors were investigated as alternatives to the original ZrCl4 precursor.

Dynamic leaching studies of 48 MWd/kgU UO2 commercial spent nuclear fuel under oxic conditions

NASA Astrophysics Data System (ADS)

Serrano-Purroy, D.; Casas, I.; González-Robles, E.; Glatz, J. P.; Wegen, D. H.; Clarens, F.; Giménez, J.; de Pablo, J.; Martínez-Esparza, A.

2013-03-01

The leaching of a high-burn-up spent nuclear fuel (48 MWd/KgU) has been studied in a carbonate-containing solution and under oxic conditions using a Continuously Stirred Tank Flow-Through Reactor (CSTR). Two samples of the fuel, one prepared from the centre of the pellet (labelled CORE) and another one from the fuel pellet periphery, enriched with the so-called High Burn-Up Structure (HBS, labelled OUT) have been used.For uranium and actinides, the results showed that U, Np, Am and Cm gave very similar normalized dissolution rates, while Pu showed slower dissolution rates for both samples. In addition, dissolution rates were consistently two to four times lower for OUT sample compared to CORE sample.Considering the fission products release the main results are that Y, Tc, La and Nd dissolved very similar to uranium; while Cs, Sr, Mo and Rb have up to 10 times higher dissolution rates. Rh, Ru and Zr seemed to have lower dissolution rates than uranium. The lowest dissolution rates were found for OUT sample.Three different contributions were detected on uranium release, modelled and attributed to oxidation layer, fines and matrix release.

New measurement of the 242Pu(n,γ) cross section at n_TOF

NASA Astrophysics Data System (ADS)

Lerendegui-Marco, J.; Guerrero, C.; Cortés-Giraldo, M. A.; Quesada, J. M.; Mendoza, E.; Cano-Ott, D.; Eberhardt, K.; Junghans, A.

2016-03-01

The use of MOX fuel (mixed-oxide fuel made of UO2 and PuO2) in nuclear reactors allows substituting a large fraction of the enriched Uranium by Plutonium reprocessed from spent fuel. With the use of such new fuel composition rich in Pu, a better knowledge of the capture and fission cross sections of the Pu isotopes becomes very important. In particular, a new series of cross section evaluations have been recently carried out jointly by the European (JEFF) and United States (ENDF) nuclear data agencies. For the case of 242Pu, the two only neutron capture time-of-flight measurements available, from 1973 and 1976, are not consistent with each other, which calls for a new time-of flight capture cross section measurement. In order to contribute to a new evaluation, we have perfomed a neutron capture cross section measurement at the n_TOF-EAR1 facility at CERN using four C6D6 detectors, using a high purity target of 95 mg. The preliminary results assessing the quality and limitations (background, statistics and γ-flash effects) of this new experimental data are presented and discussed, taking into account that the aimed accuracy of the measurement ranges between 7% and 12% depending on the neutron energy region.

Monte Carlo Criticality Analysis of Simple Geometrics COntaining Tungsten Rhenium Alloys Engrained with Uranium Dioxide and Uranium Mononitride

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jonathan A. Webb; Indrajit Charit

2011-08-01

The critical mass and dimensions of simple geometries containing highly enriched uraniumdioxide (UO2) and uraniummononitride (UN) encapsulated in tungsten-rhenium alloys are determined using MCNP5 criticality calculations. Spheres as well as cylinders with length to radius ratios of 1.82 are computationally built to consist of 60 vol.% fuel and 40 vol.% metal matrix. Within the geometries the uranium is enriched to 93 wt.% uranium-235 and the rhenium content within the metal alloy was modeled over a range of 0 to 30 at.%. The spheres containing UO2 were determined to have a critical radius of 18.29 cm to 19.11 cm and amore » critical mass ranging from 366 kg to 424 kg. The cylinders containing UO2 were found to have a critical radius ranging from 17.07 cm to 17.844 cm with a corresponding critical mass of 406 kg to 471 kg. Spheres engrained with UN were determined to have a critical radius ranging from 14.82 cm to 15.19 cm and a critical mass between 222 kg and 242 kg. Cylinders which were engrained with UN were determined to have a critical radius ranging from 13.811 cm to 14.155 cm with a corresponding critical mass of 245 kg to 267 kg. The critical geometries were also computationally submerged in a neutronaically infinite medium of fresh water to determine the effects of rhenium addition on criticality accidents due to water submersion. The monte carlo analysis demonstrated that rhenium addition of up to 30 at.% can reduce the excess reactivity due to water submersion by up to $5.07 for UO2 fueled cylinders, $3.87 for UO2 fueled spheres and approximately $3.00 for UN fueled spheres and cylinders.« less

MicroRaman measurements for nuclear fuel reprocessing applications

DOE PAGES

Casella, Amanda; Lines, Amanda; Nelson, Gilbert; ...

2016-12-01

Treatment and reuse of used nuclear fuel is a key component in closing the nuclear fuel cycle. Solvent extraction reprocessing methods that have been developed contain various steps tailored to the separation of specific radionuclides, which are highly dependent upon solution properties. The instrumentation used to monitor these processes must be robust, require little or no maintenance, and be able to withstand harsh environments such as high radiation fields and aggressive chemical matrices. Our group has been investigating the use of optical spectroscopy for the on-line monitoring of actinides, lanthanides, and acid strength within fuel reprocessing streams. This paper willmore » focus on the development and application of a new MicroRaman probe for on-line real-time monitoring of the U(VI)/nitrate ion/nitric acid in solutions relevant to used nuclear fuel reprocessing. Previous research has successfully demonstrated the applicability on the macroscopic scale, using sample probes requiring larger solution volumes. In an effort to minimize waste and reduce dose to personnel, we have modified this technique to allow measurement at the microfluidic scale using a Raman microprobe. Under the current sampling environment, Raman samples typically require upwards of 10 mL and larger. Using the new sampling system, we can sample volumes at 10 μL or less, which is a scale reduction of over 1,000 fold in sample size. Finally, this paper will summarize our current work in this area including: comparisons between the macroscopic and microscopic probes for detection limits, optimized channel focusing, and application in a flow cell with varying levels of HNO 3, and UO 2(NO 3) 2.« less

Consistent criticality and radiation studies of Swiss spent nuclear fuel: The CS2M approach.

PubMed

Rochman, D; Vasiliev, A; Ferroukhi, H; Pecchia, M

2018-06-15

In this paper, a new method is proposed to systematically calculate at the same time canister loading curves and radiation sources, based on the inventory information from an in-core fuel management system. As a demonstration, the isotopic contents of the assemblies come from a Swiss PWR, considering more than 6000 cases from 34 reactor cycles. The CS 2 M approach consists in combining four codes: CASMO and SIMULATE to extract the assembly characteristics (based on validated models), the SNF code for source emission and MCNP for criticality calculations for specific canister loadings. The considered cases cover enrichments from 1.9 to 5.0% for the UO 2 assemblies and 4.8% for the MOX, with assembly burnup values from 7 to 74 MWd/kgU. Because such a study is based on the individual fuel assembly history, it opens the possibility to optimize canister loadings from the point-of-view of criticality, decay heat and emission sources. Copyright © 2018 Elsevier B.V. All rights reserved.

Analysis of gamma ray dose for dried up pond storing low enriched UO2 fuel

NASA Astrophysics Data System (ADS)

Nauchi, Yasushi; Suzuki, Motomu

2017-09-01

Gamma ray dose is calculated for loss of coolant accident in spent fuel pond (SFP) storing irradiated fuels used in light water reactors. Influence of modelling of fuel assemblies, source distributions, and loading fraction of fuel assemblies in the fuel rack on the dose are investigated.

Design of a Uranium Dioxide Spheroidization System

NASA Technical Reports Server (NTRS)

Cavender, Daniel P.; Mireles, Omar R.; Frendi, Abdelkader

2013-01-01

The plasma spheroidization system (PSS) is the first process in the development of tungsten-uranium dioxide (W-UO2) fuel cermets. The PSS process improves particle spherocity and surface morphology for coating by chemical vapor deposition (CVD) process. Angular fully dense particles melt in an argon-hydrogen plasma jet at between 32-36 kW, and become spherical due to surface tension. Surrogate CeO2 powder was used in place of UO2 for system and process parameter development. Particles range in size from 100 - 50 microns in diameter. Student s t-test and hypothesis testing of two proportions statistical methods were applied to characterize and compare the spherocity of pre and post process powders. Particle spherocity was determined by irregularity parameter. Processed powders show great than 800% increase in the number of spherical particles over the stock powder with the mean spherocity only mildly improved. It is recommended that powders be processed two-three times in order to reach the desired spherocity, and that process parameters be optimized for a more narrow particles size range. Keywords: spherocity, spheroidization, plasma, uranium-dioxide, cermet, nuclear, propulsion

METHOD FOR DECONTAMINATION OF REACTOR SOLUTIONS

DOEpatents

Maraman, W.J.; Baxman, H.R.; Baker, R.D.

1959-05-01

A process for U recovery from phosphate fuel solutions is described. To fuel solution drawn from the reactor is added Fe(NO/sub 3/)/sub 3/ which destroys the U complex and forms ferric phosphate complex. The UO/sub 2/(NO/sub 3/)/sub 2/ formed is extracted into TBP-kerosene in a countercurrent column. The TBP contalning UO/sub 2/(NO/sub 3/)/sub 2/ is further purified by an aqueous Al(NO/ sub 3/)/sub 3/ scrub solution. The pregnant solution then goes to an H/sub 3/PO/ sub 4/ stripping and kerosene washing column. The H/sub 3/PO/sub 4/--uranyl phosphate solution is separated at the bottom and boiled to remove HNO/sub 3/ then diluted to fuel solution make-up strength. (T.R.H.)

Quantification of process variables for carbothermic synthesis of UC 1-xN x fuel microspheres

DOE PAGES

Lindemer, Terrance B.; Silva, Chinthaka M.; Henry, Jr, John James; ...

2016-11-05

This report details the continued investigation of process variables involved in converting sol-gel-derived, urania-carbon microspheres to ~820-μm-dia. UC 1-xN x fuel kernels in flow-through, vertical Mo and W crucibles at temperatures up to 2123 K. Experiments included calcining of air-dried UO 3-H 2O-C microspheres in Ar and H 2-containing gases, conversion of the resulting UO 2-C kernels to dense UO2:2UC in the same gases and vacuum, and its conversion in N 2 to UC 1-xN x (x = ~0.85). The thermodynamics of the relevant reactions were applied extensively to interpret and control the process variables. Producing the precursor UO 2:2UCmore » kernel of ~96% theoretical density was required, but its subsequent conversion to UC 1-xN x at 2123 K was not accompanied by sintering and resulted in ~83-86% of theoretical density. Increasing the UC 1-xN x kernel nitride component to ~0.98 in flowing N 2-H 2 mixtures to evolve HCN was shown to be quantitatively consistent with present and past experiments and the only useful application of H 2 in the entire process.« less

Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres

NASA Astrophysics Data System (ADS)

Lindemer, T. B.; Silva, C. M.; Henry, J. J.; McMurray, J. W.; Voit, S. L.; Collins, J. L.; Hunt, R. D.

2017-01-01

This report details the continued investigation of process variables involved in converting sol-gel-derived, urania-carbon microspheres to ∼820-μm-dia. UC1-xNx fuel kernels in flow-through, vertical Mo and W crucibles at temperatures up to 2123 K. Experiments included calcining of air-dried UO3-H2O-C microspheres in Ar and H2-containing gases, conversion of the resulting UO2-C kernels to dense UO2:2UC in the same gases and vacuum, and its conversion in N2 to UC1-xNx (x = ∼0.85). The thermodynamics of the relevant reactions were applied extensively to interpret and control the process variables. Producing the precursor UO2:2UC kernel of ∼96% theoretical density was required, but its subsequent conversion to UC1-xNx at 2123 K was not accompanied by sintering and resulted in ∼83-86% of theoretical density. Increasing the UC1-xNx kernel nitride component to ∼0.98 in flowing N2-H2 mixtures to evolve HCN was shown to be quantitatively consistent with present and past experiments and the only useful application of H2 in the entire process.

Development of spent fuel reprocessing process based on selective sulfurization: Study on the Pu, Np and Am sulfurization

NASA Astrophysics Data System (ADS)

Kirishima, Akira; Amano, Yuuki; Nihei, Toshifumi; Mitsugashira, Toshiaki; Sato, Nobuaki

2010-03-01

For the recovery of fissile materials from spent nuclear fuel, we have proposed a novel reprocessing process based on selective sulfurization of fission products (FPs). The key concept of this process is utilization of unique chemical property of carbon disulfide (CS2), i.e., it works as a reductant for U3O8 but works as a sulfurizing agent for minor actinides and lanthanides. Sulfurized FPs and minor actinides (MA) are highly soluble to dilute nitric acid while UO2 and PuO2 are hardly soluble, therefore, FPs and MA can be removed from Uranium and Plutonium matrix by selective dissolution. As a feasibility study of this new concept, the sulfurization behaviours of U, Pu, Np, Am and Eu are investigated in this paper by the thermodynamical calculation, phase analysis of chemical analogue elements and tracer experiments.

Modelling of the Gadolinium Fuel Test IFA-681 using the BISON Code

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pastore, Giovanni; Hales, Jason Dean; Novascone, Stephen Rhead

2016-05-01

In this work, application of Idaho National Laboratory’s fuel performance code BISON to modelling of fuel rods from the Halden IFA-681 gadolinium fuel test is presented. First, an overview is given of BISON models, focusing on UO2/UO2-Gd2O3 fuel and Zircaloy cladding. Then, BISON analyses of selected fuel rods from the IFA-681 test are performed. For the first time in a BISON application to integral fuel rod simulations, the analysis is informed by detailed neutronics calculations in order to accurately capture the radial power profile throughout the fuel, which is strongly affected by the complex evolution of absorber Gd isotopes. Inmore » particular, radial power profiles calculated at IFE–Halden Reactor Project with the HELIOS code are used. The work has been carried out in the frame of the collaboration between Idaho National Laboratory and Halden Reactor Project. Some slide have been added as an Appendix to present the newly developed PolyPole-1 algorithm for modeling of intra-granular fission gas release.« less

Enhanced thermal conductivity of uranium dioxide-silicon carbide composite fuel pellets prepared by Spark Plasma Sintering (SPS)

NASA Astrophysics Data System (ADS)

Yeo, S.; Mckenna, E.; Baney, R.; Subhash, G.; Tulenko, J.

2013-02-01

Uranium dioxide (UO2)-10 vol% silicon carbide (SiC) composite fuel pellets were produced by oxidative sintering and Spark Plasma Sintering (SPS) at a range of temperatures from 1400 to 1600 °C. Both SiC whiskers and SiC powder particles were utilized. Oxidative sintering was employed over 4 h and the SPS sintering was employed only for 5 min at the highest hold temperature. It was noted that composite pellets sintered by SPS process revealed smaller grain size, reduced formation of chemical products, higher density, and enhanced interfacial contact compared to the pellets made by oxidative sintering. For given volume of SiC, the pellets with powder particles yielded a smaller grain size than pellets with SiC whiskers. Finally thermal conductivity measurements at 100 °C, 500 °C, and 900 °C revealed that SPS sintered UO2-SiC composites exhibited an increase of up to 62% in thermal conductivity compared to UO2 pellets, while the oxidative sintered composite pellets revealed significantly inferior thermal conductivity values. The current study points to the improved processing capabilities of SPS compared to oxidative sintering of UO2-SiC composites.

Towards the reanalysis of void coefficients measurements at proteus for high conversion light water reactor lattices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hursin, M.; Koeberl, O.; Perret, G.

2012-07-01

High Conversion Light Water Reactors (HCLWR) allows a better usage of fuel resources thanks to a higher breeding ratio than standard LWR. Their uses together with the current fleet of LWR constitute a fuel cycle thoroughly studied in Japan and the US today. However, one of the issues related to HCLWR is their void reactivity coefficient (VRC), which can be positive. Accurate predictions of void reactivity coefficient in HCLWR conditions and their comparisons with representative experiments are therefore required. In this paper an inter comparison of modern codes and cross-section libraries is performed for a former Benchmark on Void Reactivitymore » Effect in PWRs conducted by the OECD/NEA. It shows an overview of the k-inf values and their associated VRC obtained for infinite lattice calculations with UO{sub 2} and highly enriched MOX fuel cells. The codes MCNPX2.5, TRIPOLI4.4 and CASMO-5 in conjunction with the libraries ENDF/B-VI.8, -VII.0, JEF-2.2 and JEFF-3.1 are used. A non-negligible spread of results for voided conditions is found for the high content MOX fuel. The spread of eigenvalues for the moderated and voided UO{sub 2} fuel are about 200 pcm and 700 pcm, respectively. The standard deviation for the VRCs for the UO{sub 2} fuel is about 0.7% while the one for the MOX fuel is about 13%. This work shows that an appropriate treatment of the unresolved resonance energy range is an important issue for the accurate determination of the void reactivity effect for HCLWR. A comparison to experimental results is needed to resolve the presented discrepancies. (authors)« less

Influence of Background H2O on the Collision-Induced Dissociation Products Generated from [UO2NO3]+

NASA Astrophysics Data System (ADS)

Van Stipdonk, Michael J.; Iacovino, Anna; Tatosian, Irena

2018-04-01

Developing a comprehensive understanding of the reactivity of uranium-containing species remains an important goal in areas ranging from the development of nuclear fuel processing methods to studies of the migration and fate of the element in the environment. Electrospray ionization (ESI) is an effective way to generate gas-phase complexes containing uranium for subsequent studies of intrinsic structure and reactivity. Recent experiments by our group have demonstrated that the relatively low levels of residual H2O in a 2-D, linear ion trap (LIT) make it possible to examine fragmentation pathways and reactions not observed in earlier studies conducted with 3-D ion traps (Van Stipdonk et al. J. Am. Soc. Mass Spectrom. 14, 1205-1214, 2003). In the present study, we revisited the dissociation of complexes composed of uranyl nitrate cation [UVIO2(NO3)]+ coordinated by alcohol ligands (methanol and ethanol) using the 2-D LIT. With relatively low levels of background H2O, collision-induced dissociation (CID) of [UVIO2(NO3)]+ primarily creates [UO2(O2)]+ by the ejection of NO. However, CID (using He as collision gas) of [UVIO2(NO3)]+ creates [UO2(H2O)]+ and UO2 + when the 2-D LIT is used with higher levels of background H2O. Based on the results presented here, we propose that product ion spectrum in the previous experiments was the result of a two-step process: initial formation of [UVIO2(O2)]+ followed by rapid exchange of O2 for H2O by ion-molecule reaction. Our experiments illustrate the impact of residual H2O in ion trap instruments on the product ions generated by CID and provide a more accurate description of the intrinsic dissociation pathway for [UVIO2(NO3)]+. [Figure not available: see fulltext.

Phenomenology of BWR fuel assembly degradation

NASA Astrophysics Data System (ADS)

Kurata, Masaki; Barrachin, Marc; Haste, Tim; Steinbrueck, Martin

2018-03-01

Severe accidents occurred at the Fukushima-Daiichi Nuclear Power Station (FDNPS) which required an immediate re-examination of fuel degradation phenomenology. The present paper reviews the updated knowledge on the phenomenology of the fuel degradation, focusing mainly on the BWR fuel assembly degradation at the macroscopic scale and that of the individual interactions at the meso-scale. Oxidation of boron carbide (B4C) control rods potentially generates far larger amounts of heat and hydrogen under BWR accident conditions. All integral tests with B4C control rods or control blades have shown early failure, liquefaction, relocation and oxidation of B4C starting at temperatures around 1250 °C, well below the significant interaction temperatures of UO2-Zry. These interactions or reactions potentially influence the progress of fuel degradation in the early phase. The steam-starved conditions, which are being discussed as a likely scenario at the FDNPS accident, highly influence the individual interactions and potentially lead the fuel degradation in non-prototypical directions. The detailed phenomenology of individual interactions and their influence on the transient and on the late phase of the severe accidents are also discussed.

Functionalized Sugarcane Bagasse for U(VI) Adsorption from Acid and Alkaline Conditions.

PubMed

Su, Shouzheng; Liu, Qi; Liu, Jingyuan; Zhang, Hongsen; Li, Rumin; Jing, Xiaoyan; Wang, Jun

2018-01-15

The highly efficient removal of uranium from mine tailings effluent, radioactive wastewater and enrichment from seawater is of great significance for the development of nuclear industry. In this work, we prepared an efficient U(VI) adsorbent by EDTA modified sugarcane bagasse (MESB) with a simple process. The prepared adsorbent preserves high adsorptive capacity for UO 2 2+ (pH 3.0) and uranyl complexes, such as UO 2 (OH) + , (UO 2 ) 2 (OH) 2 2+ and (UO 2 ) 3 (OH) 5 + (pH 4.0 and pH 5.0) and good repeatability in acidic environment. The maximum adsorption capacity for U(VI) at pH 3.0, 4.0 and 5.0 is 578.0, 925.9 and 1394.1 mg/g and the adsorption capacity loss is only 7% after five cycles. With the pH from 3.0 to 5.0, the inhibitive effects of Na + and K + decreased but increased of Mg 2+ and Ca 2+ . MESB also exhibits good adsorption for [UO 2 (CO 3 ) 3 ] 4- at pH 8.3 from 10 mg/L to 3.3 μg/L. Moreover, MESB could effectively extract U(VI) from simulated seawater in the presence of other metals ions. This work provided a general and efficient uranyl enriched material for nuclear industry.

Alloy Selection for Accident Tolerant Fuel Cladding in Commercial Light Water Reactors

NASA Astrophysics Data System (ADS)

Rebak, Raul B.

2015-12-01

As a consequence of the March 2011 events at the Fukushima site, the U.S. congress asked the Department of Energy (DOE) to concentrate efforts on the development of nuclear fuels with enhanced accident tolerance. The new fuels had to maintain or improve the performance of current UO2-zirconium alloy rods during normal operation conditions and tolerate the loss of active cooling in the core for a considerably longer time period than the current system. DOE is funding cost-shared research to investigate the behavior of advanced steels both under normal operation conditions in high-temperature water [ e.g., 561 K (288 °C)] and under accident conditions for reaction with superheated steam. Current results show that, under accident conditions, the advanced ferritic steels (1) have orders of magnitude lower reactivity with steam, (2) would generate less hydrogen and heat than the current zirconium alloys, (3) are resistant to stress corrosion cracking under normal operation conditions, and (4) have low general corrosion in water at 561 K (288 °C).

Determining the minimum required uranium carbide content for HTGR UCO fuel kernels

DOE PAGES

McMurray, Jacob W.; Lindemer, Terrence B.; Brown, Nicholas R.; ...

2017-03-10

There are three important failure mechanisms that must be controlled in high-temperature gas-cooled reactor (HTGR) fuel for certain higher burnup applications are SiC layer rupture, SiC corrosion by CO, and coating compromise from kernel migration. All are related to high CO pressures stemming from free O generated when uranium present as UO 2 fissions and the O is not subsequently bound by other elements. Furthermore, in the HTGR UCO kernel design, CO buildup from excess O is controlled by the inclusion of additional uranium in the form of a carbide, UC x. An approach for determining the minimum UC xmore » content to ensure negligible CO formation was developed and demonstrated using CALPHAD models and the Serpent 2 reactor physics and depletion analysis tool. Our results are intended to be more accurate than previous estimates by including more nuclear and chemical factors, in particular the effect of transmutation products on the oxygen distribution as the fuel kernel composition evolves with burnup.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ivanov, Alexander S.; Bryantsev, Vyacheslav S.

Uranium is used as the basic fuel for nuclear power plants, which generate significant amounts of electricity and have life cycle carbon emissions that are as low as renewable energy sources. However, the extraction of this valuable energy commodity from the ground remains controversial, mainly because of environmental and health impacts. Alternatively, seawater offers an enormous uranium resource that may be tapped at minimal environmental cost. Nowadays, amidoxime polymers are the most widely utilized sorbent materials for large-scale extraction of uranium from seawater, but they are not perfectly selective for uranyl, UO 2 2+. In particular, the competition between UOmore » 2 2+ and VO 2+/VO2+ cations poses a significant challenge to the effi-cient mining of UO 2 2+. Thus, screening and rational design of more selective ligands must be accomplished. One of the key components in achieving this goal is the establishment of computational techniques capable of assessing ligand selec-tivity trends. Here, we report an approach based on quantum chemical calculations that achieves high accuracy in repro-ducing experimental aqueous stability constants for VO 2+/VO 2+ complexes with ten different oxygen donor lig-ands. The predictive power of the developed computational protocol was demonstrated for amidoxime-type ligands, providing greater insights into new design strategies for the development of the next generation of adsorbents with high selectivity toward UO 2 2+over VO 2+/VO 2+ ions. Furthermore, the results of calculations suggest that alkylation of amidox-ime moieties present in poly(acrylamidoxime) sorbents can be a potential route to better discrimination between the uranyl and competing vanadium ions within seawater.« less

Fabrication of simulated DUPIC fuel

NASA Astrophysics Data System (ADS)

Kang, Kweon Ho; Song, Ki Chan; Park, Hee Sung; Moon, Je Sun; Yang, Myung Seung

2000-12-01

Simulated DUPIC fuel provides a convenient way to investigate the DUPIC fuel properties and behavior such as thermal conductivity, thermal expansion, fission gas release, leaching, and so on without the complications of handling radioactive materials. Several pellets simulating the composition and microstructure of DUPIC fuel are fabricated by resintering the powder, which was treated through OREOX process of simulated spent PWR fuel pellets, which had been prepared from a mixture of UO2 and stable forms of constituent nuclides. The key issues for producing simulated pellets that replicate the phases and microstructure of irradiated fuel are to achieve a submicrometre dispersion during mixing and diffusional homogeneity during sintering. This study describes the powder treatment, OREOX, compaction and sintering to fabricate simulated DUPIC fuel using the simulated spent PWR fuel. The homogeneity of additives in the powder was observed after attrition milling. The microstructure of the simulated spent PWR fuel agrees well with the other studies. The leading structural features observed are as follows: rare earth and other oxides dissolved in the UO2 matrix, small metallic precipitates distributed throughout the matrix, and a perovskite phase finely dispersed on grain boundaries.

Multiscale modeling of thermal conductivity of high burnup structures in UO 2 fuels

DOE PAGES

Bai, Xian -Ming; Tonks, Michael R.; Zhang, Yongfeng; ...

2015-12-22

The high burnup structure forming at the rim region in UO 2 based nuclear fuel pellets has interesting physical properties such as improved thermal conductivity, even though it contains a high density of grain boundaries and micron-size gas bubbles. To understand this counterintuitive phenomenon, mesoscale heat conduction simulations with inputs from atomistic simulations and experiments were conducted to study the thermal conductivities of a small-grain high burnup microstructure and two large-grain unrestructured microstructures. We concluded that the phonon scattering effects caused by small point defects such as dispersed Xe atoms in the grain interior must be included in order tomore » correctly predict the thermal transport properties of these microstructures. In extreme cases, even a small concentration of dispersed Xe atoms such as 10 -5 can result in a lower thermal conductivity in the large-grain unrestructured microstructures than in the small-grain high burnup structure. The high-density grain boundaries in a high burnup structure act as defect sinks and can reduce the concentration of point defects in its grain interior and improve its thermal conductivity in comparison with its large-grain counterparts. Furthermore, an analytical model was developed to describe the thermal conductivity at different concentrations of dispersed Xe, bubble porosities, and grain sizes. Upon calibration, the model is robust and agrees well with independent heat conduction modeling over a wide range of microstructural parameters.« less

Selectivity in Ligand Binding to Uranyl Compounds: A Synthetic, Structural, Thermodynamic and Computational Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arnold, John

The uranyl cation (UO 2 2+) is the most abundant form of uranium on the planet. It is estimated that 4.5 billion tons of uranium in this form exist in sea water. The ability to bind and extract the uranyl cation from aqueous solution while separating it from other elements would provide a limitless source of nuclear fuel. A large body of research concerns the selective recognition and extraction of uranyl. A stable molecule, the cation has a linear O=U=O geometry. The short U-O bonds (1.78 Å) arise from the combination of uranium 5f/6d and oxygen 2p orbitals. Due tomore » the oxygen moieties being multiply bonded, these sites were not thought to be basic enough for Lewis acidic coordination to be a viable approach to sequestration. We believe that the goal of developing a practical system for uranium separation from seawater will not be attained without new insights into our existing fundamental knowledge of actinide chemistry. We posit that detailed studies of the kinetic and thermodynamic factors that influence interactions between f-elements and ligands with a range of donor atoms is essential to any major advance in this important area. The goal of this research is thus to broaden the coordination chemistry of the uranyl ion by studying new ligand systems via synthetic, structural, thermodynamic and computational methods. We anticipate that this fundamental science will find use beyond actinide separation technologies in areas such as nuclear waste remediation and nuclear materials.« less

Evaluation of B&W UO2/ThO2 VIII experimental core: criticality and thermal disadvantage factor analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carlo Parisi; Emanuele Negrenti

2017-02-01

In the framework of the OECD/NEA International Reactor Physics Experiment (IRPHE) Project, an evaluation of core VIII of the Babcock & Wilcox (B&W) Spectral Shift Control Reactor (SSCR) critical experiment program was performed. The SSCR concept, moderated and cooled by a variable mixture of heavy and light water, envisaged changing of the thermal neutron spectrum during the operation to encourage breeding and to sustain the core criticality. Core VIII contained 2188 fuel rods with 93% enriched UO2-ThO2 fuel in a moderator mixture of heavy and light water. The criticality experiment and measurements of the thermal disadvantage factor were evaluated.

Identification and Quantification of Carbon Phases in Conversion Fuel for the Transient Reactor Test Facility

DOE Office of Scientific and Technical Information (OSTI.GOV)

Steele, Robert; Mata, Angelica; Dunzik-Gougar, Mary Lou

2016-06-01

As part of an overall effort to convert US research reactors to low-enriched uranium (LEU) fuel use, a LEU conversion fuel is being designed for the Transient Reactor Test Facility (TREAT) at the Idaho National Laboratory. TREAT fuel compacts are comprised of UO2 fuel particles in a graphitic matrix material. In order to refine heat transfer modeling, as well as determine other physical and nuclear characteristics of the fuel, the amount and type of graphite and non-graphite phases within the fuel matrix must be known. In this study, we performed a series of complementary analyses, designed to allow detailed characterizationmore » of the graphite and phenolic resin based fuel matrix. Methods included Scanning Electron and Transmission Electron Microscopies, Raman spectroscopy, X-ray Diffraction, and Dual-Beam Focused Ion Beam Tomography. Our results indicate that no single characterization technique will yield all of the desired information; however, through the use of statistical and empirical data analysis, such as curve fitting, partial least squares regression, volume extrapolation and spectra peak ratios, a degree of certainty for the quantity of each phase can be obtained.« less

Assessment of empirical potential for MOX nuclear fuels and thermomechanical properties

NASA Astrophysics Data System (ADS)

Balboa, Hector; Van Brutzel, Laurent; Chartier, Alain; Le Bouar, Yann

2017-11-01

We assess five empirical interatomic potentials in the approximation of rigid ions and pair interactions for the (U1-y,Puy)O solid solution. The assessment compares available experimental data and Fink's recommendation with simulations on: the structural, thermodynamics, and mechanical properties over the full range of plutonium composition, from pure UO2 to pure PuO2 and for temperatures ranging from 300 K to the melting point. The best results are obtained by potentials referred as Cooper and Potashnikov potentials. The first one reproduces more accurately recommendations for the thermodynamics and mechanical properties exhibiting ductile-like behaviour during crack propagation, while the second one gives brittle behaviour at low temperature.

Advanced sample environments for in situ neutron diffraction studies of nuclear materials

NASA Astrophysics Data System (ADS)

Reiche, Helmut Matthias

Generation IV nuclear reactor concepts, such as the supercritical-water-cooled nuclear reactor (SCWR), are actively researched internationally. Operating conditions above the critical point of water (374°C, 22.1 MPa) and fuel core temperature that potentially exceed 1850°C put a high demand on the surrounding materials. For their safe application, it is essential to characterize and understand the material properties on an atomic scale such as crystal structure and grain orientation (texture) changes as a function of temperature and stress. This permits the refinement of models predicting the macroscopic behavior of the material. Neutron diffraction is a powerful tool in characterizing such crystallographic properties due to their deep penetration depth into condensed matter. This leads to the ability to study bulk material properties, as opposed to surface effects, and allows for complex sample environments to study e.g. the individual contributions of thermo-mechanical processing steps during manufacturing, operating or accident scenarios. I present three sample environments for in situ neutron diffraction studies that provide such crystallographic information and have been successfully commissioned and integrated into the user program of the High Pressure -- Preferred Orientation (HIPPO) diffractometer at the Los Alamos Neutron Science Center (LANSCE) user facility. I adapted a sample changer for reliable and fast automated texture measurements of multiple specimens. I built a creep furnace combining a 2700 N load frame with a resistive vanadium furnace, capable of temperatures up to 1000°C, and manipulated by a pair of synchronized rotation stages. This combination allows following deformation and temperature dependent texture and strain evolutions in situ. Utilizing the presented sample changer and creep furnace we studied pressure tubes made of Zr-2.5wt%Nb currently employed in CANDURTM nuclear reactors and proposed for future SCWRs, acting as the primary containment vessel of high temperature heavy water (D2O) inside the reactor core. The measured sample texture shows that upon traversing the phase transition, which proceeded according to the Burger orientation relationship, variant selection occurred during heating and cooling of the zirconium alloy. Experimental results of lattice strains depending on the crystallographic orientation can be used to calculate strain pole figures which grant insight into the three-dimensional mechanical response of a polycrystalline aggregate and represent an extremely powerful material model validation tool. Lastly, I developed a resistive graphite high-temperature furnace with sample motion for in situ crystal structure and texture measurements of nuclear materials at steady-state temperatures up to at least 2200°C. This permits in situ observation of e.g. phase transitions and coefficients of thermal expansion, as well as phase formation and texture development during solidification. Utilizing this apparatus, I investigated the carbothermic reduction of UO2 nanopowder forming uranium carbide, a promising Generation IV reactor fuel. The onset of the UO2 + 2C → UC + CO2 reaction was observed at 1440°C with the bulk portion being complete at 1500°C. I describe the novel synthesis for this nanoparticle UO2 powder, which closely imitates observed nano grains in partially burnt reactor fuels. Of the three opposing structure models reported for the non-quenchable cubic UC2 phase, stable between 1769°C and 2560°C, the NaCl-type structure according to Bowman is found to be correct. This is deemed major progress as the CaF2-type structure was used for recent thermal modeling of safety critical factors in nuclear reactors. A temperature dependent increase in density due to carbon diffusion has been observed and quantified. I provide first experimental data of an unspecified, reversible order-disorder transition in this delta-phase with its onset at ˜1800°C which is likely due to rotating C2 molecules in the sublattice.

Accident-tolerant oxide fuel and cladding

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mariani, Robert D.

Systems and methods for accident tolerant oxide fuel. One or more disks can be placed between fuel pellets comprising UO.sub.2, wherein such disks possess a higher thermal conductivity material than that of the UO.sub.2 to provide enhanced heat rejection thereof. Additionally, a cladding coating comprising zircaloy coated with a material that provides stability and high melting capability can be provided. The pellets can be configured as annular pellets having an annulus filled with the higher thermal conductivity material. The material coating the zircaloy can be, for example, Zr.sub.5Si.sub.4 or another silicide such as, for example, a Zr-Silicide that limits corrosion.more » The aforementioned higher thermal conductivity material can be, for example, Si, Zr.sub.xSi.sub.y, Zr, or Al.sub.2O.sub.3.« less

Initial Microstructure Evaluation of a U3Si2 + W Fuel Pin Fabricated Via Arc Melt Gravity Drop Casting

NASA Astrophysics Data System (ADS)

Hoggan, Rita E.; Harp, Jason M.

2018-02-01

Injection casting has historically been used to fabricate metallic nuclear fuel on a large scale. Casting of intermetallic fuel forms, such as U3Si2, may be an alternative pathway for fabrication of fuel pins to powder metallurgy. To investigate casting on a small scale, arc melt gravity drop casting was employed to cast a one-off pin of U3Si2 for evaluation as a fabrication method for U3Si2 as a light water reactor fuel. The pin was sectioned and examined via optical microscopy and scanning electron microscopy equipped with energy dispersive x-ray spectroscopy (EDS). Image analysis was used to estimate the volume fraction of phase impurities as well as porosity. The primary phase determined by EDS was U3Si2 with U-O and U-Si-W phase impurities. Unusually high levels of tungsten were observed because of accidental tungsten introduction during arc melting. No significant changes in microstructure were observed after annealing a section of the pin at 800°C for 72 h. The average density of the sectioned specimens was 12.4 g/cm3 measured via Archimedes principle immersion density and He gas displacement.

Thermodynamics of fission products in UO(2 ± x).

PubMed

Nerikar, P V; Liu, X-Y; Uberuaga, B P; Stanek, C R; Phillpot, S R; Sinnott, S B

2009-10-28

The stabilities of selected fission products-Xe, Cs, and Sr-are investigated as a function of non-stoichiometry x in UO(2 ± x). In particular, density functional theory (DFT) is used to calculate the incorporation and solution energies of these fission products at the anion and cation vacancy sites, at the divacancy, and at the bound Schottky defect. In order to reproduce the correct insulating state of UO(2), the DFT calculations are performed using spin polarization and with the Hubbard U term. In general, higher charge defects are more soluble in the fuel matrix and the solubility of fission products increases as the hyperstoichiometry increases. The solubility of fission product oxides is also explored. Cs(2)O is observed as a second stable phase and SrO is found to be soluble in the UO(2) matrix for all stoichiometries. These observations mirror experimentally observed phenomena.

Chemical compatibility between UO2 fuel and SiC cladding for LWRs. Application to ATF (Accident-Tolerant Fuels)

NASA Astrophysics Data System (ADS)

Braun, James; Guéneau, Christine; Alpettaz, Thierry; Sauder, Cédric; Brackx, Emmanuelle; Domenger, Renaud; Gossé, Stéphane; Balbaud-Célérier, Fanny

2017-04-01

Silicon carbide-silicon carbide (SiC/SiC) composites are considered to replace the current zirconium-based cladding materials thanks to their good behavior under irradiation and their resistance under oxidative environments at high temperature. In the present work, a thermodynamic analysis of the UO2±x/SiC system is performed. Moreover, using two different experimental methods, the chemical compatibility of SiC towards uranium dioxide, with various oxygen contents (UO2±x) is investigated in the 1500-1970 K temperature range. The reaction leads to the formation of mainly uranium silicides and carbides phases along with CO and SiO gas release. Knudsen Cell Mass Spectrometry is used to measure the gas release occurring during the reaction between UO2+x and SiC powders as function of time and temperature. These experimental conditions are representative of an open system. Diffusion couple experiments with pellets are also performed to study the reaction kinetics in closed system conditions. In both cases, a limited chemical reaction is observed below 1700 K, whereas the reaction is enhanced at higher temperature due to the decomposition of SiC leading to Si vaporization. The temperature of formation of the liquid phase is found to lie between 1850 < T < 1950 K.

Calculation and comparison of xenon and samarium reactivities of the HEU, LEU core in the low power research reactor.

PubMed

Dawahra, S; Khattab, K; Saba, G

2015-07-01

Comparative studies for the conversion of the fuel from HEU to LEU in the Miniature Neutron Source Reactor (MNSR) have been performed using the MCNP4C and GETERA codes. The precise calculations of (135)Xe and (149)Sm concentrations and reactivities were carried out and compared during the MNSR operation time and after shutdown for the existing HEU fuel (UAl4-Al, 90% enriched) and the potential LEU fuels (U3Si2-Al, U3Si-Al, U9Mo-Al, 19.75% enriched and UO2, 12.6% enriched) in this paper using the MCNP4C and GETERA codes. It was found that the (135)Xe and (149)Sm reactivities did not reach their equilibrium reactivities during the daily operating time of the reactor. The (149)Sm reactivities could be neglected compared to (135)Xe reactivities during the reactor operating time and after shutdown. The calculations for the UAl4-Al produced the highest (135)Xe reactivity in all the studied fuel group during the reactor operation (0.39 mk) and after the reactor shutdown (0.735 mk), It followed by U3Si-Al (0.34 mk, 0.653 mk), U3Si2-Al (0.33 mk, 0.634 mk), U9Mo-Al (0.3 mk, 0.568 mk) and UO2 (0.24 mk, 0.448 mk) fuels, respectively. Finally, the results showed that the UO2 was the best candidate for fuel conversion to LEU in the MNSR since it gave the lowest (135)Xe reactivity during the reactor operation and after shutdown. Copyright © 2015 Elsevier Ltd. All rights reserved.

Neutronics Studies of Uranium-bearing Fully Ceramic Micro-encapsulated Fuel for PWRs

DOE PAGES

George, Nathan M.; Maldonado, G. Ivan; Terrani, Kurt A.; ...

2014-12-01

Our study evaluated the neutronics and some of the fuel cycle characteristics of using uranium-based fully ceramic microencapsulated (FCM) fuel in a pressurized water reactor (PWR). Specific PWR lattice designs with FCM fuel have been developed that are expected to achieve higher specific burnup levels in the fuel while also increasing the tolerance to reactor accidents. The SCALE software system was the primary analysis tool used to model the lattice designs. A parametric study was performed by varying tristructural isotropic particle design features (e.g., kernel diameter, coating layer thicknesses, and packing fraction) to understand the impact on reactivity and resultingmore » operating cycle length. Moreover, to match the lifetime of an 18-month PWR cycle, the FCM particle fuel design required roughly 10% additional fissile material at beginning of life compared with that of a standard uranium dioxide (UO 2) rod. Uranium mononitride proved to be a favorable fuel for the fuel kernel due to its higher heavy metal loading density compared with UO 2. The FCM fuel designs evaluated maintain acceptable neutronics design features for fuel lifetime, lattice peaking factors, and nonproliferation figure of merit.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Snepvangers, J.J.M.

Equipment and results are described connected with irradiation studies of UO/sub 2/ fuels, fuel element testing in pressurized water loops, graphite irradiation, and steel irradiations with and without temperature control. The apparatus described is associated with a 20-Mw pool-type research reactor. (T.F.H.)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jackson, Timothy D; Hollenbach, Daniel F; Shedlock, Daniel

Radiography by Selective Detection (RSD), was investigated for its ability to determine the presence and types of defects in a UO{sub 2} fuel rod surrounded by zirconium cladding. Images created using a Monte Carlo model compared favorably with actual X-ray backscatter images from mock fuel rods. A fuel rod was modeled as a rectangular parallelepiped with zirconium cladding, and pencil beam X-ray sources of 160 kVp (79 keV avg) and 480 kVp (218 keV avg) were generated using the Monte Carlo N-Particle Transport Code to attempt to image void and palladium (Pd) defects in the interior and on the surfacemore » of the fuel pellet. It was found that the 160 kVp spectrum was unable to detect the presence of interior defects, whereas the 480 kVp spectrum detected them with both the standard and the RSD backscatter methods, though the RSD method was very inefficient. It was also found that both energy spectra were able to detect void and Pd defects on the surface using both imaging methods. Additionally, two mock fuel rods were imaged using a backscatter X-ray imaging system, one consisting of hafnium pellets in a Zircaloy-4 cladding and the other consisting of steel pellets in a Zircalloy-4 cladding which was then encased in a steel cladding (a double encapsulation configuration employed in irradiation and experiments). It was found that the system was capable of detecting individual HfO{sub 2} pellets in a Zircaloy-4 cladding and may be capable of detecting individual steel pellets in the double-encapsulated sample. It is expected that the system would also be capable of detecting individual UO{sub 2} pellets in a Zircaloy-4 cladding, though no UO{sub 2} fuel rod was available for imaging.« less

Assessment of solid/liquid equilibria in the (U, Zr)O2+y system

NASA Astrophysics Data System (ADS)

Mastromarino, S.; Seibert, A.; Hashem, E.; Ciccioli, A.; Prieur, D.; Scheinost, A.; Stohr, S.; Lajarge, P.; Boshoven, J.; Robba, D.; Ernstberger, M.; Bottomley, D.; Manara, D.

2017-10-01

Solid/liquid equilibria in the system UO2sbnd ZrO2 are revisited in this work by laser heating coupled with fast optical thermometry. Phase transition points newly measured under inert gas are in fair agreement with the early measurements performed by Wisnyi et al., in 1957, the only study available in the literature on the whole pseudo-binary system. In addition, a minimum melting point is identified here for compositions near (U0.6Zr0.4)O2+y, around 2800 K. The solidus line is rather flat on a broad range of compositions around the minimum. It increases for compositions closer to the pure end members, up to the melting point of pure UO2 (3130 K) on one side and pure ZrO2 (2970 K) on the other. Solid state phase transitions (cubic-tetragonal-monoclinic) have also been observed in the ZrO2-rich compositions X-ray diffraction. Investigations under 0.3 MPa air (0.063 MPa O2) revealed a significant decrease in the melting points down to 2500 K-2600 K for increasing uranium content (x(UO2)> 0.2). This was found to be related to further oxidation of uranium dioxide, confirmed by X-ray absorption spectroscopy. For example, a typical oxidised corium composition U0.6Zr0.4O2.13 was observed to solidify at a temperature as low as 2493 K. The current results are important for assessing the thermal stability of the system fuel - cladding in an oxide based nuclear reactor, and for simulating the system behaviour during a hypothetical severe accident.

The crystal structure of ianthinite, [U 24+(UO 2) 4O 6(OH) 4(H 2O) 4](H 2O) 5: a possible phase for Pu 4+ incorporation during the oxidation of spent nuclear fuel

NASA Astrophysics Data System (ADS)

Burns, Peter C.; Finch, Robert J.; Hawthorne, Frank C.; Miller, Mark L.; Ewing, Rodney C.

1997-10-01

Ianthinite, [U 24+(UO 2) 4O 6(OH) 4(H 2O) 4](H 2O) 5, is the only known uranyl oxide hydrate mineral that contains U 4+, and it has been proposed that ianthinite may be an important Pu 4+-bearing phase during the oxidative dissolution of spent nuclear fuel. The crystal structure of ianthinite, orthorhombic, a = 0.7178(2), b = 1.1473(2), c = 3.039(1) nm, V = 2.5027 nm 3Z = 4, space group P2 1cn, has been solved by direct methods and refined by least-squares methods to an R index of 9.7% and a wR index of 12.6% using 888 unique observed [| F| ≥ 5 σ | F|] reflections. The structure contains both U 4+. The U 6+ cations are present as roughly linear (U 6+O 2) 2+ uranyl ion (Ur) that are in turn coordinated by five O 2- and OH - located at the equatorial positions of pentagonal bipyramids. The U 4+ cations are coordinated by O 2-, OH - and H 2O in a distorted octahedral arrangement. The Ur φ5and U 4+| 6 (φ: O 2-, OH -, H 2O) polyhedra l sharing edges to for two symmetrically distinct sheets at z ≈ 0.0 and z ≈ 0.25 that are parallel to (001). The sheets have the β-U 3O 8 sheet anion-topology. There are five symmetrically distinct H 2O groips located at z ≈ 0.125 between the sheets of U φn polyhedra, and the sheets of U φn polyhedra are linked together only by hydrogen bonding to the intersheet H 2O groups. The crystal-chemical requirements of U 4+ and Pu 4+ are very similar, suggesting that extensive Pu 4+ ↔ U 4+ substitution may occur within the sheets of U φn polyhedra in trh structure of ianthinine.

Preliminary Modeling of Accident Tolerant Fuel Concepts under Accident Conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gamble, Kyle A.; Hales, Jason D.

2016-12-01

The catastrophic events that occurred at the Fukushima-Daiichi nuclear power plant in 2011 have led to widespread interest in research of alternative fuels and claddings that are proposed to be accident tolerant. Thus, the United States Department of Energy through its NEAMS (Nuclear Energy Advanced Modeling and Simulation) program has funded an Accident Tolerant Fuel (ATF) High Impact Problem (HIP). The ATF HIP is funded for a three-year period. The purpose of the HIP is to perform research into two potential accident tolerant concepts and provide an in-depth report to the Advanced Fuels Campaign (AFC) describing the behavior of themore » concepts, both of which are being considered for inclusion in a lead test assembly scheduled for placement into a commercial reactor in 2022. The initial focus of the HIP is on uranium silicide fuel and iron-chromium-aluminum (FeCrAl) alloy cladding. Utilizing the expertise of three national laboratory participants (INL, LANL, and ANL) a comprehensive mulitscale approach to modeling is being used including atomistic modeling, molecular dynamics, rate theory, phase-field, and fuel performance simulations. In this paper, we present simulations of two proposed accident tolerant fuel systems: U3Si2 fuel with Zircaloy-4 cladding, and UO2 fuel with FeCrAl cladding. The simulations investigate the fuel performance response of the proposed ATF systems under Loss of Coolant and Station Blackout conditions using the BISON code. Sensitivity analyses are completed using Sandia National Laboratories’ DAKOTA software to determine which input parameters (e.g., fuel specific heat) have the greatest influence on the output metrics of interest (e.g., fuel centerline temperature). Early results indicate that each concept has significant advantages as well as areas of concern. Further work is required prior to formulating the proposition report for the Advanced Fuels Campaign.« less

Modelling Accident Tolerant Fuel Concepts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hales, Jason Dean; Gamble, Kyle Allan Lawrence

2016-05-01

The catastrophic events that occurred at the Fukushima-Daiichi nuclear power plant in 2011 have led to widespread interest in research of alternative fuels and claddings that are proposed to be accident tolerant. The United States Department of Energy (DOE) through its Nuclear Energy Advanced Modeling and Simulation (NEAMS) program has funded an Accident Tolerant Fuel (ATF) High Impact Problem (HIP). The ATF HIP is a three-year project to perform research on two accident tolerant concepts. The final outcome of the ATF HIP will be an in-depth report to the DOE Advanced Fuels Campaign (AFC) giving a recommendation on whether eithermore » of the two concepts should be included in their lead test assembly scheduled for placement into a commercial reactor in 2022. The two ATF concepts under investigation in the HIP are uranium silicide fuel and iron-chromium-aluminum (FeCrAl) alloy cladding. Utilizing the expertise of three national laboratory participants (Idaho National Laboratory, Los Alamos National Laboratory, and Argonne National Laboratory), a comprehensive multiscale approach to modeling is being used that includes atomistic modeling, molecular dynamics, rate theory, phase-field, and fuel performance simulations. Model development and fuel performance analysis are critical since a full suite of experimental studies will not be complete before AFC must prioritize concepts for focused development. In this paper, we present simulations of the two proposed accident tolerance fuel systems: U3Si2 fuel with Zircaloy-4 cladding, and UO2 fuel with FeCrAl cladding. Sensitivity analyses are completed using Sandia National Laboratories’ Dakota software to determine which input parameters (e.g., fuel specific heat) have the greatest influence on the output metrics of interest (e.g., fuel centerline temperature). We also outline the multiscale modelling approach being employed. Considerable additional work is required prior to preparing the recommendation report for the Advanced Fuels Campaign.« less

Performance of Transuranic-Loaded Fully Ceramic Micro-Encapsulated Fuel in LWRs Final Report, Including Void Reactivity Evaluation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Michael A. Pope; R. Sonat Sen; Brian Boer

2011-09-01

The current focus of the Deep Burn Project is on once-through burning of transuranics (TRU) in light-water reactors (LWRs). The fuel form is called Fully-Ceramic Micro-encapsulated (FCM) fuel, a concept that borrows the tri-isotropic (TRISO) fuel particle design from high-temperature reactor technology. In the Deep Burn LWR (DB-LWR) concept, these fuel particles are pressed into compacts using SiC matrix material and loaded into fuel pins for use in conventional LWRs. The TRU loading comes from the spent fuel of a conventional LWR after 5 years of cooling. Unit cell and assembly calculations have been performed using the DRAGON-4 code tomore » assess the physics attributes of TRU-only FCM fuel in an LWR lattice. Depletion calculations assuming an infinite lattice condition were performed with calculations of various reactivity coefficients performed at each step. Unit cells and assemblies containing typical UO2 and mixed oxide (MOX) fuel were analyzed in the same way to provide a baseline against which to compare the TRU-only FCM fuel. Then, assembly calculations were performed evaluating the performance of heterogeneous arrangements of TRU-only FCM fuel pins along with UO2 pins.« less

Thermodynamic Simulation of Equilibrium Composition of Reaction Products at Dehydration of a Technological Channel in a Uranium-Graphite Reactor

NASA Astrophysics Data System (ADS)

Pavliuk, A. O.; Zagumennov, V. S.; Kotlyarevskiy, S. G.; Bespala, E. V.

2018-01-01

The problems of accumulation of nuclear fuel spills in the graphite stack in the course of operation of uranium-graphite nuclear reactors are considered. The results of thermodynamic analysis of the processes in the graphite stack at dehydration of a technological channel, fuel element shell unsealing and migration of fission products, and activation of stable nuclides in structural elements of the reactor and actinides inside the graphite moderator are given. The main chemical reactions and compounds that are produced in these modes in the reactor channel during its operation and that may be hazardous after its shutdown and decommissioning are presented. Thermodynamic simulation of the equilibrium composition is performed using the specialized code TERRA. The results of thermodynamic simulation of the equilibrium composition in different cases of technological channel dehydration in the course of the reactor operation show that, if the temperature inside the active core of the nuclear reactor increases to the melting temperature of the fuel element, oxides and carbides of nuclear fuel are produced. The mathematical model of the nonstationary heat transfer in a graphite stack of a uranium-graphite reactor in the case of the technological channel dehydration is presented. The results of calculated temperature evolution at the center of the fuel element, the replaceable graphite element, the air gap, and in the surface layer of the block graphite are given. The numerical results show that, in the case of dehydration of the technological channel in the uranium-graphite reactor with metallic uranium, the main reaction product is uranium dioxide UO2 in the condensed phase. Low probability of production of pyrophoric uranium compounds (UH3) in the graphite stack is proven, which allows one to disassemble the graphite stack without the risk of spontaneous graphite ignition in the course of decommissioning of the uranium-graphite nuclear reactor.

Fission Product Inventory and Burnup Evaluation of the AGR-2 Irradiation by Gamma Spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harp, Jason Michael; Stempien, John Dennis; Demkowicz, Paul Andrew

Gamma spectrometry has been used to evaluate the burnup and fission product inventory of different components from the US Advanced Gas Reactor Fuel Development and Qualification Program's second TRISO-coated particle fuel irradiation test (AGR-2). TRISO fuel in this irradiation included both uranium carbide / uranium oxide (UCO) kernels and uranium oxide (UO 2) kernels. Four of the 6 capsules contained fuel from the US Advanced Gas Reactor program, and only those capsules will be discussed in this work. The inventories of gamma-emitting fission products from the fuel compacts, graphite compact holders, graphite spacers and test capsule shell were evaluated. Thesemore » data were used to measure the fractional release of fission products such as Cs-137, Cs-134, Eu-154, Ce-144, and Ag-110m from the compacts. The fraction of Ag-110m retained in the compacts ranged from 1.8% to full retention. Additionally, the activities of the radioactive cesium isotopes (Cs-134 and Cs-137) have been used to evaluate the burnup of all US TRISO fuel compacts in the irradiation. The experimental burnup evaluations compare favorably with burnups predicted from physics simulations. Predicted burnups for UCO compacts range from 7.26 to 13.15 % fission per initial metal atom (FIMA) and 9.01 to 10.69 % FIMA for UO 2 compacts. Measured burnup ranged from 7.3 to 13.1 % FIMA for UCO compacts and 8.5 to 10.6 % FIMA for UO 2 compacts. Results from gamma emission computed tomography performed on compacts and graphite holders that reveal the distribution of different fission products in a component will also be discussed. Gamma tomography of graphite holders was also used to locate the position of TRISO fuel particles suspected of having silicon carbide layer failures that lead to in-pile cesium release.« less

Fission Product Inventory and Burnup Evaluation of the AGR-2 Irradiation by Gamma Spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harp, Jason M.; Demkowicz, Paul A.; Stempien, John D.

Gamma spectrometry has been used to evaluate the burnup and fission product inventory of different components from the US Advanced Gas Reactor Fuel Development and Qualification Program's second TRISO-coated particle fuel irradiation test (AGR-2). TRISO fuel in this irradiation included both uranium carbide / uranium oxide (UCO) kernels and uranium oxide (UO2) kernels. Four of the 6 capsules contained fuel from the US Advanced Gas Reactor program, and only those capsules will be discussed in this work. The inventories of gamma-emitting fission products from the fuel compacts, graphite compact holders, graphite spacers and test capsule shell were evaluated. These datamore » were used to measure the fractional release of fission products such as Cs-137, Cs-134, Eu-154, Ce-144, and Ag-110m from the compacts. The fraction of Ag-110m retained in the compacts ranged from 1.8% to full retention. Additionally, the activities of the radioactive cesium isotopes (Cs-134 and Cs-137) have been used to evaluate the burnup of all US TRISO fuel compacts in the irradiation. The experimental burnup evaluations compare favorably with burnups predicted from physics simulations. Predicted burnups for UCO compacts range from 7.26 to 13.15 % fission per initial metal atom (FIMA) and 9.01 to 10.69 % FIMA for UO2 compacts. Measured burnup ranged from 7.3 to 13.1 % FIMA for UCO compacts and 8.5 to 10.6 % FIMA for UO2 compacts. Results from gamma emission computed tomography performed on compacts and graphite holders that reveal the distribution of different fission products in a component will also be discussed. Gamma tomography of graphite holders was also used to locate the position of TRISO fuel particles suspected of having silicon carbide layer failures that lead to in-pile cesium release.« less

Report on simulation of fission gas and fission product diffusion in UO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andersson, Anders David; Perriot, Romain Thibault; Pastore, Giovanni

2016-07-22

In UO 2 nuclear fuel, the retention and release of fission gas atoms such as xenon (Xe) are important for nuclear fuel performance by, for example, reducing the fuel thermal conductivity, causing fuel swelling that leads to mechanical interaction with the clad, increasing the plenum pressure and reducing the fuel–clad gap thermal conductivity. We use multi-­scale simulations to determine fission gas diffusion mechanisms as well as the corresponding rates in UO 2 under both intrinsic and irradiation conditions. In addition to Xe and Kr, the fission products Zr, Ru, Ce, Y, La, Sr and Ba have been investigated. Density functionalmore » theory (DFT) calculations are used to study formation, binding and migration energies of small clusters of Xe atoms and vacancies. Empirical potential calculations enable us to determine the corresponding entropies and attempt frequencies for migration as well as investigate the properties of large clusters or small fission gas bubbles. A continuum reaction-­diffusion model is developed for Xe and point defects based on the mechanisms and rates obtained from atomistic simulations. Effective fission gas diffusivities are then obtained by solving this set of equations for different chemical and irradiation conditions using the MARMOT phase field code. The predictions are compared to available experimental data. The importance of the large Xe U3O cluster (a Xe atom in a uranium + oxygen vacancy trap site with two bound uranium vacancies) is emphasized, which is a consequence of its high mobility and high binding energy. We find that the Xe U3O cluster gives Xe diffusion coefficients that are higher for intrinsic conditions than under irradiation over a wide range of temperatures. Under irradiation the fast-­moving Xe U3O cluster recombines quickly with irradiation-induced interstitial U ions, while this mechanism is less important for intrinsic conditions. The net result is higher concentration of the Xe U3O cluster for intrinsic conditions than under irradiation. We speculate that differences in the irradiation conditions and their impact on the Xe U3O cluster can explain the wide range of diffusivities reported in experimental studies. However, all vacancy-­mediated mechanisms underestimate the Xe diffusivity compared to the empirical radiation-­enhanced rate used in most fission gas release models. We investigate the possibility that diffusion of small fission gas bubbles or extended Xe-­vacancy clusters may give rise to the observed radiation-­enhanced diffusion coefficient. These studies highlight the importance of U divacancies and an octahedron coordination of uranium vacancies encompassing a Xe fission gas atom. The latter cluster can migrate via a multistep mechanism with a rather low effective barrier, which together with irradiation-induced clusters of uranium vacancies, gives rise to the irradiation-enhanced diffusion coefficient observed in experiments.« less

Comparison of silver release predictions using PARFUME with results from the AGR-2 irradiation experiment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Collin, Blaise P.; Demkowicz, Paul A.; Baldwin, Charles A.

2016-11-01

The PARFUME (PARticle FUel ModEl) code was used to predict silver release from tristructural isotropic (TRISO) coated fuel particles and compacts during the second irradiation experiment (AGR-2) of the Advanced Gas Reactor Fuel Development and Qualification program. The PARFUME model for the AGR-2 experiment used the fuel compact volume average temperature for each of the 559 days of irradiation to calculate the release of fission product silver from a representative particle for a select number of AGR-2 compacts and individual fuel particles containing either mixed uranium carbide/oxide (UCO) or 100% uranium dioxide (UO2) kernels. Post-irradiation examination (PIE) measurements were performedmore » to provide data on release of silver from these compacts and individual fuel particles. The available experimental fractional releases of silver were compared to their corresponding PARFUME predictions. Preliminary comparisons show that PARFUME under-predicts the PIE results in UCO compacts and is in reasonable agreement with experimental data for UO2 compacts. The accuracy of PARFUME predictions is impacted by the code limitations in the modeling of the temporal and spatial distributions of the temperature across the compacts. Nevertheless, the comparisons on silver release lie within the same order of magnitude.« less

Compaction of AWBA fuel pellets without binders (AWBA Development Program)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, R.G.R.

1982-08-01

Highly active oxide fuel powders, composed of UO/sub 2/, UO/sub 2/-ThO/sub 2/, or ThO/sub 2/, were compacted into ultra-high density pellets without the use of binders. The objective of the study was to select the optimum die lubricant for compacting these powders into pellets in preparation for sintering to densities in excess of 97% Theoretical Density. The results showed that sintered density was a function of both the lubricant bulk density and concentration with the lowest bulk density lubricant giving the highest sintered densities with a lubricant concentration of 0.1 weight percent. Five calcium and zinc stearates were evaluated withmore » a calcium stearate with a 15 lb/ft/sup 3/ bulk density being the best lubricant.« less

Richland five-year O2 R and D Program. Integrated site operation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1966-07-11

The technical feasibility of using an electrolytic reduction process to reduce metal scrap and oxide to usable uranium metal is being studied. The incentives for using electrolytic reduction at Richland may be summarized as follows: (1) reduce the unit and total costs of producing plutonium; (2) increase the flexibility of the Richland reactors for producing isotopes, particularly U-236; and (3) simplify the present fuel cycle complex. The scope of the mission is limited to the evaluation of hollow extruded I and E cores, the evaluation of electro-reduced uranium, an investigation of the solution rate of UO{sub 2} in the electrolyte,more » and small-scale irradiations of UO{sub 2} fuels in the N and K Reactors. Progress during FY 1966 is summarized.« less

High density, uniformly distributed W/UO2 for use in Nuclear Thermal Propulsion

NASA Astrophysics Data System (ADS)

Tucker, Dennis S.; Barnes, Marvin W.; Hone, Lance; Cook, Steven

2017-04-01

An inexpensive, quick method has been developed to obtain uniform distributions of UO2 particles in a tungsten matrix utilizing 0.5 wt percent low density polyethylene. Powders were sintered in a Spark Plasma Sintering (SPS) furnace at 1600 °C, 1700 °C, 1750 °C, 1800 °C and 1850 °C using a modified sintering profile. This resulted in a uniform distribution of UO2 particles in a tungsten matrix with high densities, reaching 99.46% of theoretical for the sample sintered at 1850 °C. The powder process is described and the results of this study are given below.

Results from the DOE Advanced Gas Reactor Fuel Development and Qualification Program

DOE Office of Scientific and Technical Information (OSTI.GOV)

David Petti

2014-06-01

Modular HTGR designs were developed to provide natural safety, which prevents core damage under all design basis accidents and presently envisioned severe accidents. The principle that guides their design concepts is to passively maintain core temperatures below fission product release thresholds under all accident scenarios. This level of fuel performance and fission product retention reduces the radioactive source term by many orders of magnitude and allows potential elimination of the need for evacuation and sheltering beyond a small exclusion area. This level, however, is predicated on exceptionally high fuel fabrication quality and performance under normal operation and accident conditions. Germanymore » produced and demonstrated high quality fuel for their pebble bed HTGRs in the 1980s, but no U.S. manufactured fuel had exhibited equivalent performance prior to the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program. The design goal of the modular HTGRs is to allow elimination of an exclusion zone and an emergency planning zone outside the plant boundary fence, typically interpreted as being about 400 meters from the reactor. To achieve this, the reactor design concepts require a level of fuel integrity that is better than that claimed for all prior US manufactured TRISO fuel, by a few orders of magnitude. The improved performance level is about a factor of three better than qualified for German TRISO fuel in the 1980’s. At the start of the AGR program, without a reactor design concept selected, the AGR fuel program selected to qualify fuel to an operating envelope that would bound both pebble bed and prismatic options. This resulted in needing a fuel form that could survive at peak fuel temperatures of 1250°C on a time-averaged basis and high burnups in the range of 150 to 200 GWd/MTHM (metric tons of heavy metal) or 16.4 to 21.8% fissions per initial metal atom (FIMA). Although Germany has demonstrated excellent performance of TRISO-coated UO2 particle fuel up to about 10% FIMA and 1150°C, UO2 fuel is known to have limitations because of CO formation and kernel migration at the high burnups, power densities, temperatures, and temperature gradients that may be encountered in the prismatic modular HTGRs. With uranium oxycarbide (UCO) fuel, the kernel composition is engineered to prevent CO formation and kernel migration, which are key threats to fuel integrity at higher burnups, temperatures, and temperature gradients. Furthermore, the recent poor fuel performance of UO2 TRISO fuel pebbles measured in Chinese irradiation testing in Russia and in German pebbles irradiated at 1250°C, and historic data on poorer fuel performance in safety testing of German pebbles that experienced burnups in excess of 10% FIMA [1] have each raised concern about the use of UO2 TRISO above 10% FIMA and 1150°C and the degree of margin available in the fuel system. This continues to be an active area of study internationally.« less

Estimating the time for dissolution of spent fuel exposed to unlimited water

DOE Office of Scientific and Technical Information (OSTI.GOV)

Leider, H.R.; Nguyen, S.N.; Stout, R.B.

1991-12-01

The release of radionuclides from spent fuel cannot be precisely predicted at this point because a satisfactory dissolution model based on specific chemical processes is not yet available. However, preliminary results on the dissolution rate of UO{sub 2} and spent fuel as a function of temperature and water composition have recently been reported. This information, together with data on fragment size distribution of spent fuel, are used to estimate the dissolution response of spent fuel in excess flowing water within the framework of a simple model. In this model, the reaction/dissolution front advances linearly with time and geometry is preserved.more » This also estimates the dissolution rate of the bulk of the fission products and higher actinides, which are uniformly distributed in the UO{sub 2} matrix and are presumed to dissolve congruently. We have used a fuel fragment distribution actually observed to calculate the time for total dissolution of spent fuel. A worst-case estimate was also made using the initial (maximum) rate of dissolution to predict the total dissolution time. The time for total dissolution of centimeter size particles is estimated to be 5.5 {times} 10{sup 4} years at 25{degrees}C.« less

The Manufacture of W-UO2 Fuel Elements for NTP Using the Hot Isostatic Pressing Consolidation Process

NASA Technical Reports Server (NTRS)

Broadway, Jeramie; Hickman, Robert; Mireles, Omar

2012-01-01

NTP is attractive for space exploration because: (1) Higher Isp than traditional chemical rockets (2)Shorter trip times (3) Reduced propellant mass (4) Increased payload. Lack of qualified fuel material is a key risk (cost, schedule, and performance). Development of stable fuel form is a critical path, long lead activity. Goals of this project are: Mature CERMET and Graphite based fuel materials and Develop and demonstrate critical technologies and capabilities.

DOE Office of Scientific and Technical Information (OSTI.GOV)

McMurray, Jacob W.; Lindemer, Terrence B.; Brown, Nicholas R.

There are three important failure mechanisms that must be controlled in high-temperature gas-cooled reactor (HTGR) fuel for certain higher burnup applications are SiC layer rupture, SiC corrosion by CO, and coating compromise from kernel migration. All are related to high CO pressures stemming from free O generated when uranium present as UO 2 fissions and the O is not subsequently bound by other elements. Furthermore, in the HTGR UCO kernel design, CO buildup from excess O is controlled by the inclusion of additional uranium in the form of a carbide, UC x. An approach for determining the minimum UC xmore » content to ensure negligible CO formation was developed and demonstrated using CALPHAD models and the Serpent 2 reactor physics and depletion analysis tool. Our results are intended to be more accurate than previous estimates by including more nuclear and chemical factors, in particular the effect of transmutation products on the oxygen distribution as the fuel kernel composition evolves with burnup.« less

γ-radiation induced corrosion of copper in bentonite-water systems under anaerobic conditions

NASA Astrophysics Data System (ADS)

Karin Norrfors, K.; Björkbacka, Åsa; Kessler, Amanda; Wold, Susanna; Jonsson, Mats

2018-03-01

In this work we have experimentally studied the impact of bentonite clay on the process of radiation-induced copper corrosion in anoxic water. The motivation for this is to further develop our understanding of radiation-driven processes occurring in deep geological repositories for spent nuclear fuel where copper canisters containing the spent nuclear fuel will be embedded in compacted bentonite. Experiments on radiation-induced corrosion in the presence and absence of bentonite were performed along with experiments elucidating the impact irradiation on the Cu2+ adsorption capacity of bentonite. The experiments presented in this work show that the presence of bentonite clay has no or very little effect on the magnitude of radiation-induced corrosion of copper in anoxic aqueous systems. The absence of a protective effect similar to that observed for radiation-induced dissolution of UO2 is attributed to differences in the corrosion mechanism. This provides further support for the previously proposed mechanism where the hydroxyl radical is the key radiolytic oxidant responsible for the corrosion of copper. The radiation effect on the bentonite sorption capacity of Cu2+ (reduced capacity) is in line with what has previously been reported for other cations. The reduced cation sorption capacity is partly attributed to a loss of Al-OH sites upon irradiation.

Raising Nuclear Thermal Propulsion (NTP) Technology Readiness Above 3

NASA Technical Reports Server (NTRS)

Gerrish, Harold P., Jr.

2014-01-01

NTP development is currently supported by the NASA program office "Advanced Exploration Systems". The concept is a main propulsion option being considered for human missions to Mars in the 2030's. Major NTP development took place in the 1960's and 1970's under the Rover/NERVA program. The technology had matured to TRL 6 and was preparing to go to TRL 7 with a prototype flight engine before the program was cancelled. Over the last 40 years, a variety of continuations started, but only lasted a few years each. The Rover/NERVA infrastructure is almost all gone. The only remains are a few pieces of hardware, final reports and a few who worked the Rover/NERVA. Two types of nuclear fuel are being investigated to meet the current engine design specific impulse of 900 seconds compared to approximately 850 seconds demonstrated during Rover/NERVA. One is a continuation of composite fuel with new coatings to better control mid-band corrosion. The other type is a CERMET fuel made of Tungsten and UO2. Both fuels are being made from Rover/NERVA lessons learned, but with slightly different recipes to increase fuel endurance at higher operating temperatures. The technology readiness level (TRL) of these current modified reactor fuels is approximately TRL 3. To keep the development cost low and help mature the TRL level past 4 quickly, a few special non-nuclear test facilities have been made to test surrogate fuel, with depleted uranium, as coupons and full length elements. Both facilities utilize inductive heating and are licensed to handle depleted uranium. TRL 5 requires exposing the fuel to a nuclear environment and TRL 6 requires a prototype ground or flight engine system test. Currently, three different NTP ground test facility options are being investigated: exhaust scrubber, bore hole, and total exhaust containment. In parallel, a prototype flight demonstration test is also being studied. The first human mission to Mars in the 2030's is currently 2033. For an advanced propulsion concept to be seriously considered for use, the engine development plans need to show it is feasible and affordable to reach TRL 8 by 2027 and can be qualified for human mission use.

Oxidizing dissolution mechanism of an irradiated MOX fuel in underwater aerated conditions at slightly acidic pH

NASA Astrophysics Data System (ADS)

Magnin, M.; Jégou, C.; Caraballo, R.; Broudic, V.; Tribet, M.; Peuget, S.; Talip, Z.

2015-07-01

The (U,Pu)O2 matrix behavior of an irradiated MIMAS-type (MIcronized MASter blend) MOX fuel, under radiolytic oxidation in aerated pure water at pH 5-5.5 was studied by combining chemical and radiochemical analyses of the alteration solution with Raman spectroscopy characterizations of the surface state. Two leaching experiments were performed on segments of irradiated fuel under different conditions: with or without an external γ irradiation field, over long periods (222 and 604 days, respectively). The gamma irradiation field was intended to be representative of the irradiation conditions for a fuel assembly in an underwater interim storage situation. The data acquired enabled an alteration mechanism to be established, characterized by uranium (UO22+) release mainly controlled by solubility of studtite over the long-term. The massive precipitation of this phase was observed for the two experiments based on high uranium oversaturation indexes of the solution and the kinetics involved depended on the irradiation conditions. External gamma irradiation accelerated the precipitation kinetics and the uranium concentrations (2.9 × 10-7 mol/l) were lower than for the non-irradiated reference experiment (1.4 × 10-5 mol/l), as the quantity of hydrogen peroxide was higher. Under slightly acidic pH conditions, the formation of an oxidized UO2+x phase was not observed on the surface and did not occur in the radiolysis dissolution mechanism of the fuel matrix. The Raman spectroscopy performed on the heterogeneous MOX fuel matrix surface, showed that the fluorite structure of the mainly UO2 phase surrounding the Pu-enriched aggregates had not been particularly impacted by any major structural change compared to the data obtained prior to leaching. For the plutonium, its behavior in solution involved a continuous release up to concentrations of approximately 3 × 10-6 mol L-1 with negligible colloid formation. This data appears to support a predominance of the +V oxidation state for plutonium in solution under highly oxidizing conditions. Furthermore, the Raman spectroscopy monitoring of the sample surface oxidation states did not point to any significant effect from the high Pu content of the aggregates (10-15%) and therefore did not indicate a better aggregate stability under radiolysis compared to the mainly UO2 matrix. This is because acidic pH conditions do not favor the development of oxidized layers on a fuel surface, with the exception of secondary phases.

Inclusions and Substructures in Uranium of Nuclear Purity. Report No. 51; INCLUSIONES Y SUBESTRUCTURAS EN URANIO DE PUREZA NUCLEAR. INFORME NO. 51

DOE Office of Scientific and Technical Information (OSTI.GOV)

Biloni, H.; Lindenvald, N.; Sabato, J.A.

1961-01-01

The inclusions in uranium of nuclear purity (UC, UH/sub 3/, UO/sub 2/, UO, UN, and the complexes which include the intersolubility of U with C and N or with C, N, and O) were . analyzed metallographically, and the results reported by other authors were discussed critically. The existence of the fine precipitate reticular substructure, sensitive to thermal treatments, which generally appears in uraniunn was analyzed. Its origins were discussed in accordance with bibliographic data. Complementary data for its comprehension are given from the metallographic analysis of U--Al and U-- Fe alloys with low Al and Fe concentrations. (tr-auth)

Comparing results of X-ray diffraction, µ-Raman spectroscopy and neutron diffraction when identifying chemical phases in seized nuclear material, during a comparative nuclear forensics exercise.

PubMed

Rondahl, Stina Holmgren; Pointurier, Fabien; Ahlinder, Linnea; Ramebäck, Henrik; Marie, Olivier; Ravat, Brice; Delaunay, François; Young, Emma; Blagojevic, Ned; Hester, James R; Thorogood, Gordon; Nelwamondo, Aubrey N; Ntsoane, Tshepo P; Roberts, Sarah K; Holliday, Kiel S

2018-01-01

This work presents the results for identification of chemical phases obtained by several laboratories as a part of an international nuclear forensic round-robin exercise. In this work powder X-ray diffraction (p-XRD) is regarded as the reference technique. Neutron diffraction produced a superior high-angle diffraction pattern relative to p-XRD. Requiring only small amounts of sample, µ-Raman spectroscopy was used for the first time in this context as a potentially complementary technique to p-XRD. The chemical phases were identified as pure UO 2 in two materials, and as a mixture of UO 2 , U 3 O 8 and an intermediate species U 3 O 7 in the third material.

Carbon monoxide formation in UO2 kerneled HTR fuel particles containing oxygen getters

NASA Astrophysics Data System (ADS)

Proksch, E.; Strigl, A.; Nabielek, H.

1986-01-01

Mass spectrometric measurements of CO in irradiated UO2 fuel particles containing oxygen getters are summarized. Uranium carbide addition in the 3% to 15% range reduces the CO release by factors between 25 and 80, up to burn-up levels as high as 70% FIMA. Unintentional gettering by SiC in TRISO coated particles with failed inner pyrocarbon layers results in CO reduction factors between 15 and 110. For ZrC, ambiguous results are obtained; ZrC probably results in CO reduction by a factor of 40; Ce2O3 and La2O3 seem less effective than the carbides; for Ce2O3, reduction factors between 3 and 15 are found. However, the results are possibly incorrect due to premature oxidation of the getter already during fabrication. Addition of SiO2 + Al2O3 has no influence on CO release.

Structural evolution of a uranyl peroxide nano-cage fullerene: U60, at elevated pressures

NASA Astrophysics Data System (ADS)

Turner, K. M.; Lin, Y.; Zhang, F.; McGrail, B.; Burns, P. C.; Mao, W. L.; Ewing, R. C.

2015-12-01

U60 is a uranyl peroxide nano-cage that adopts a highly symmetric fullerene topology; it is topologically identical to C60. Several studies on the aqueous-phase of U60 clusters, [UO2(O2)(OH)]6060-, have shown its persistence in complex solutions and over lengthy time scales. Peroxide enhances corrosion of nuclear fuel in a reactor accident-uranyl peroxides often form near contaminated sites. U60 (Fm-3) crystallizes with approximate formula: Li68K12(OH)20[UO2(O2)(OH)]60(H2O)310. Here, we have used the diamond anvil cell (DAC) to examine U60 to understand the stability of this cluster at high pressures. We used a symmetric DAC with 300 μm culet diamonds and two different pressure-transmitting media: a mixture of methanol+ethanol and silicone oil. Using a combination of in situ Raman spectroscopy and synchrotron XRD, and electrospray ionization mass spectroscopy (ESI-MS) ex situ, we have determined the pressure-induced evolution of U60. Crystalline U60 undergoes an irreversible phase transition to a tetragonal structure at 4.1 GPa, and irreversibly amorphizes at 13 GPa. The amorphous phase likely consists of clusters of U60. Above 15 GPa, the U60 cluster is irreversibly destroyed. ESI-MS shows that this phase consists of species that likely have between 10-20 uranium atoms. Raman spectroscopy complements the diffraction measurements. U60 shows two dominant vibrational modes: a symmetric stretch of the uranyl U-O triple bond (810 cm-1), and a symmetric stretch of the U-O2-U peroxide bond (820 cm-1). As pressure is increased, these modes shift to higher wavenumbers, and overlap at 4 GPa. At 15 GPa, their intensity decreases below detection. These experiments reveal several novel behaviors including a new phase of U60. Notably, the amorphization of U60 occurs before the collapse of its cluster topology. This is different from the behavior of solvated C60 at high pressure, which maintains a hcp structure up to 30 GPa, while the clusters disorder. These results suggest that uranyl peroxide nano-cage clusters are persistent once formed, regardless of the state of the cluster: crystalline, amorphous, or in solution. These results add to the body of evidence suggesting that uranyl peroxides are important compounds to consider when dealing with environmental impacts of nuclear waste contamination.

Characterization of the Kinetics of NF3-Fluorination of NpO2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Casella, Andrew M.; Scheele, Randall D.; McNamara, Bruce K.

2015-12-23

The exploitation of selected actinide and fission product fluoride volatilities has long been considered as a potentially attractive compact method for recycling used nuclear fuels to avoid generating the large volumes of radioactive waste arising from aqueous reprocessing [1-7]. The most developed process uses the aggressive and hazardous fluorinating agents hydrogen fluoride (HF) and/or molecular fluorine (F2) at high temperatures to volatilize the greatest fraction of the used nuclear fuel into a single gas stream. The volatilized fluorides are subsequently separated using a series of fractionation and condensation columns to recover the valuable fuel constituents and fission products. In pursuitmore » of a safer and less complicated approach, we investigated an alternative fluoride volatility-based process using the less hazardous fluorinating agent nitrogen trifluoride (NF3) and leveraging its less aggressive nature to selectively evolve fission product and actinide fluorides from the solid phase based on their reaction temperatures into a single recycle stream [8-15]. In this approach, successive isothermal treatments using NF3 will first evolve the more thermally susceptible used nuclear fuel constituents leaving the other constituents in the residual solids until subsequent isothermal temperature treatments cause these others to volatilize. During investigation of this process, individual neat used fuel components were treated with isothermal NF3 in an attempt to characterize the kinetics of each fluorination reaction to provide input into the design of a new volatile fluoride separations approach. In these directed investigations, complex behavior was observed between NF3 and certain solid reactants such as the actinide oxides of uranium, plutonium, and neptunium. Given the similar thermal reaction susceptibilities of neptunium oxide (NpO2) and uranium dioxide (UO2) and the importance of Np and U, we initially focused our efforts on determining the reaction kinetic parameters for NpO2. Characterizing the NF3 fluorination of NpO2 using established models for gas-solid reactions [16] proved unsuccessful so we developed a series of successive fundamental reaction mechanisms to characterize the observed successive fluorination reactions leading to production of the volatile neptunium hexafluoride (NpF6).« less

Report on in-situ studies of flash sintering of uranium dioxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Raftery, Alicia Marie

Flash sintering is a novel type of field assisted sintering that uses an electric field and current to provide densification of materials on very short time scales. The potential for field assisted sintering techniques to be used in producing nuclear fuel is gaining recognition due to the potential economic benefits and improvements in material properties. The flash sintering behavior has so far been linked to applied and material parameters, but the underlying mechanisms active during flash sintering have yet to be identified. This report summarizes the efforts to investigate flash sintering of uranium dioxide using dilatometer studies at Los Alamosmore » National Laboratory and two separate sets of in-situ studies at Brookhaven National Laboratory’s NSLS-II XPD-1 beamline. The purpose of the dilatometer studies was to understand individual parameter (applied and material) effects on the flash behavior and the purpose of the in-situ studies was to better understand the mechanisms active during flash sintering. As far as applied parameters, it was found that stoichiometry, or oxygen-to-metal ratio, has a significant effect on the flash behavior (time to flash and speed of flash). Composite systems were found to have degraded sintering behavior relative to pure UO 2. The critical field studies are complete for UO 2.00 and will be analyzed against an existing model for comparison. The in-situ studies showed that the strength of the field and current are directly related to the sample temperature, with temperature-driven phase changes occurring at high values. The existence of an ‘incubation time’ has been questioned, due to a continuous change in lattice parameter values from the moment that the field is applied. Some results from the in-situ experiments, which should provide evidence regarding ion migration, are still being analyzed. Some preliminary conclusions can be made from these results with regard to using field assisted sintering to fabricate nuclear fuel. First, the pure UO 2-based system shows promising behavior with flash sintering, but composite systems are likely to show better sintering behavior with spark plasma sintering. Efforts to develop these methods should therefore be tailored towards the likelihood of success. Additionally, modeling is a rapidly developing aspect of current flash sintering research and should be used in parallel with experiments. Ultimately, ongoing flash sintering studies on various materials, like those summarized in this report, are rapidly contributing to the feasibility of controlling this method for use in the future.« less

Criteria for the selection of materials for water-cooled reactors., with comments on D 2O reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lewis, W.B.

1962-07-06

When intense radiation, high temperatures, and high mechanical stresses act in combination on different materials in contact, the familiar classification of materials into solids, liquids, and gases is a handicap rather than a help. Water becomes a source of H 2 that will pass into a metal and change its resistance to stress. Hydrogen diffuses rapidly through metals even at water temperatures. At the higher temperatures in nuclear fuel, O 2 and C diffuse rapidly. In some ceramic fuels the operating temperatures are so high that even heavy atoms will dwell less than a msec in any given lattice position.more » With so high a rate of the breaking of bonds, diffusion and interaction, the contribution of all substances present to the general ecology needs consideration. The stabilization of the mechanical properties of metals when bombarded by fast neutrons and exposed to wandering atoms, especially H, has to be studied. The behavior of Zr alloys and UO/sub 2/ in such environments has been extensively studied, and useful design criteria have been set and explored. (auth)« less

The U(VI) speciation influenced by a novel Paenibacillus isolate from Mont Terri Opalinus clay.

PubMed

Lütke, Laura; Moll, Henry; Bachvarova, Velina; Selenska-Pobell, Sonja; Bernhard, Gert

2013-05-21

Bacterial cell walls have a high density of ionizable functional groups available for U(VI) binding, hence have a great potential to affect the speciation of this contaminant in the environment. The studied strain of the genus Paenibacillus is a novel isolate originating from the Mont Terri Opalinus clay formations (Switzerland) which are currently investigated as a potential host rock for future nuclear waste storage. U(VI) binding to the cell surface functional groups was studied by potentiometry combined with time-resolved laser-induced fluorescence spectroscopy (TRLFS). Four bacterial U(VI) surface complexes were identified: R-COO-UO2(+), R-O-PO3-UO2, R-O-PO3H-UO2(+), and (R-O-PO3)2-UO2(2-). The corresponding complex stability constants were calculated to be 5.33 ± 0.08, 8.89 ± 0.04, 12.92 ± 0.05, and 13.62 ± 0.08, respectively. Hence UO2(2+) displays a moderate to strong interaction with the bacterial surface functional groups. In the acidic pH range (pH 3) UO2(2+) binding onto the cell envelope is governed by coordination to hydrogen phosphoryl sites. Upon increasing the pH an increasing coordination of UO2(2+) to carboxylic and deprotonated phosphoryl sites was found. At a pH greater than 7 uranyl hydroxides dominate the speciation. Additionally the bacteria-mediated release of inorganic phosphate in dependence on [U(VI)] at different pH values was studied to assess the influence of phosphate release on U(VI) mobilization.

Processing of uranium oxide and silicon carbide based fuel using polymer infiltration and pyrolysis

NASA Astrophysics Data System (ADS)

Singh, Abhishek K.; Zunjarrao, Suraj C.; Singh, Raman P.

2008-09-01

Ceramic composite pellets consisting of uranium oxide, UO 2, contained within a silicon carbide matrix, were fabricated using a novel processing technique based on polymer infiltration and pyrolysis (PIP). In this process, particles of depleted uranium oxide, in the form of U 3O 8, were dispersed in liquid allylhydridopolycarbosilane (AHPCS), and subjected to pyrolysis up to 900 °C under a continuous flow of ultra high purity argon. The pyrolysis of AHPCS, at these temperatures, produced near-stoichiometric amorphous silicon carbide ( a-SiC). Multiple polymer infiltration and pyrolysis (PIP) cycles were performed to minimize open porosity and densify the silicon carbide matrix. Analytical characterization was conducted to investigate chemical interaction between U 3O 8 and SiC. It was observed that U 3O 8 reacted with AHPCS during the very first pyrolysis cycle, and was converted to UO 2. As a result, final composition of the material consisted of UO 2 particles contained in an a-SiC matrix. The physical and mechanical properties were also quantified. It is shown that this processing scheme promotes uniform distribution of uranium fuel source along with a high ceramic yield of the parent matrix.

Predicting equilibrium uranium isotope fractionation in crystals and solution

NASA Astrophysics Data System (ADS)

Schauble, E. A.

2015-12-01

Despite the rapidly growing interest in using 238U/235U measurements as a proxy for changes in oxygen abundance in surface and near-surface environments, the present theoretical understanding of uranium isotope fractionation is limited to a few simple gas-phase molecules and analogues of dissolved species (e.g., 1,2,3). Understanding uranium isotope fractionation behavior in more complicated species, such as crystals and adsorption complexes, will help in the design and interpretation of experiments and field studies, and may suggest other uses for 38U/235U measurements. In this study, a recently developed first-principles method for estimating the nuclear volume component of field shift fractionation in crystals and complex molecular species (4) is combined with mass-dependent fractionation theory to predict equilibrium 38U/235U fractionations in aqueous and crystalline uranium compounds, including uraninite (UO2). The nuclear field shift effect, caused by the interaction of electrons with the finite volume of the positive charge distribution in uranium nuclei, is estimated using Density Functional Theory and the Projector Augmented Wave method (DFT-PAW). Tests against relativistic electronic structure calculations and Mössbauer isomer shift data indicate that the DFT-PAW method is reasonably accurate, while being much better suited to models of complex and crystalline species. Initial results confirm previous predictions that the nuclear volume effect overwhelms mass depdendent fractionation in U(VI)-U(IV) exchange reactions, leading to higher 238U/235U in U(IV) species (i.e., for UO2 xtal vs. UO22+aq, ln αNV ≈ +1.8‰ , ln αMD ≈ -0.8‰, ln αTotal ≈ +1.0‰ at 25ºC). UO2 and U(H2O)94+, are within ~0.4‰ of each other, while U(VI) species appear to be more variable. This suggests that speciation is likely to significantly affect natural uranium isotope fractionations, in addition to oxidation state. Tentatively, it appears that uranyl-type (UO22+-bearing) structures will tend to have higher 238U/235U than uranate-type structures that lack strong U=O bonds. References: 1. Bigeleisen (1996) JACS 118:3676; 2. Schauble (2006) Eos 87:V21B-0570; 3. Abe et al. (2008) J Chem Phys 128:144309, 129:164309, & Abe et al. (2010) J Chem Phys 133:044309; 4. Schauble (2013) PNAS 110:17714.

Assessment of Possible Cycle Lengths for Fully-Ceramic Micro-Encapsulated Fuel-Based Light Water Reactor Concepts

DOE Office of Scientific and Technical Information (OSTI.GOV)

R. Sonat Sen; Michael A. Pope; Abderrafi M. Ougouag

2012-04-01

The tri-isotropic (TRISO) fuel developed for High Temperature reactors is known for its extraordinary fission product retention capabilities [1]. Recently, the possibility of extending the use of TRISO particle fuel to Light Water Reactor (LWR) technology, and perhaps other reactor concepts, has received significant attention [2]. The Deep Burn project [3] currently focuses on once-through burning of transuranic fissile and fissionable isotopes (TRU) in LWRs. The fuel form for this purpose is called Fully-Ceramic Micro-encapsulated (FCM) fuel, a concept that borrows the TRISO fuel particle design from high temperature reactor technology, but uses SiC as a matrix material rather thanmore » graphite. In addition, FCM fuel may also use a cladding made of a variety of possible material, again including SiC as an admissible choice. The FCM fuel used in the Deep Burn (DB) project showed promising results in terms of fission product retention at high burnup values and during high-temperature transients. In the case of DB applications, the fuel loading within a TRISO particle is constituted entirely of fissile or fissionable isotopes. Consequently, the fuel was shown to be capable of achieving reasonable burnup levels and cycle lengths, especially in the case of mixed cores (with coexisting DB and regular LWR UO2 fuels). In contrast, as shown below, the use of UO2-only FCM fuel in a LWR results in considerably shorter cycle length when compared to current-generation ordinary LWR designs. Indeed, the constraint of limited space availability for heavy metal loading within the TRISO particles of FCM fuel and the constraint of low (i.e., below 20 w/0) 235U enrichment combine to result in shorter cycle lengths compared to ordinary LWRs if typical LWR power densities are also assumed and if typical TRISO particle dimensions and UO2 kernels are specified. The primary focus of this summary is on using TRISO particles with up to 20 w/0 enriched uranium kernels loaded in Pressurized Water Reactor (PWR) assemblies. In addition to consideration of this 'naive' use of TRISO fuel in LWRs, several refined options are briefly examined and others are identified for further consideration including the use of advanced, high density fuel forms and larger kernel diameters and TRISO packing fractions. The combination of 800 {micro}m diameter kernels of 20% enriched UN and 50% TRISO packing fraction yielded reactivity sufficient to achieve comparable burnup to present-day PWR fuel.« less

Influence of the interpellet space to the Instant Release Fraction determination of a commercial UO2 Boiling Water Reactor Spent Nuclear Fuel

NASA Astrophysics Data System (ADS)

Martínez-Torrents, A.; Serrano-Purroy, D.; Casas, I.; De Pablo, J.

2018-02-01

The contact of the coolant with the fuel pin during irradiation produces a gradient of temperature in the fuel pellet that segregates the radionuclides (RN) depending on its volatility and reactivity. This segregation determines the Instant Release Fraction (IRF), an important source of radiological risk in the performance assessment (PA) of a Deep Geologic Repository (DGR). RN segregation was studied radially in previous papers. In the present work, it was studied axially, taking into special consideration the cutting position of the solid sample to be studied. Iodine and caesium were the RN with the highest release, while the contribution of rubidium, strontium, molybdenum and technetium to the IRF depended on their chemical state. The interpellet presence (known also as dishing) effect was clearly observed for caesium, increasing its release by one order of magnitude. According to these results, one of the major contributions to the IRF comes from the RN trapped in the dishing and has to be considered in the sampling and data interpretation that will be performed for the PA of the DGR.

A Historical Review of Cermet Fuel Development and the Engine Performance Implications

NASA Technical Reports Server (NTRS)

Stewart, Mark E.

2015-01-01

To better understand Cermet engine performance, examined historical material development reports two issues: High vaporization rate of UO2, High temperature chemical stability of UO2. Cladding and chemical stabilizers each result in large, order of magnitude improvements in high temperature performance. Few samples were tested above 2770 K. Results above 2770 K are ambiguous. Contemporary testing may clarify performance. Cermet sample testing during the NERVA Rover era. Important properties, melting temperature, vaporization rate, strength, Brittle-to-Ductile Transition, cermet sample test results, engine performance, location, peak temperature.

Enhancing BWR proliferation resistance fuel with minor actinides

NASA Astrophysics Data System (ADS)

Chang, Gray S.

2009-03-01

To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides ( 237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO 2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm 3) to the top (0.35 g/cm 3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides ( 237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms for peace and the intermediate-term of nuclear energy reconnaissance.

Diffusion Couple Alloying of Refractory Metals in Austenitic and Ferritic/Martensitic Steels

DTIC Science & Technology

2012-03-01

applications of austenitic stainless steel and ferritic/martensitic steel can vary from structural and support components in the reactor core to reactor fuel ... fuel . It serves as a boundary to prevent both fission products from escaping to the core coolant, and segregates the fuel from the coolant to...uranium oxide (UO2) fuel in the core . It resists corrosion by the fuel matrix on the inner surface of the cladding and the liquid sodium coolant on

Comparing results of X-ray diffraction, µ-Raman spectroscopy and neutron diffraction when identifying chemical phases in seized nuclear material, during a comparative nuclear forensics exercise

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rondahl, Stina Holmgren; Pointurier, Fabien; Ahlinder, Linnea

This work presents the results for identification of chemical phases obtained by several laboratories as a part of an international nuclear forensic round-robin exercise. In this work powder X-ray diffraction (p-XRD) is regarded as the reference technique. Neutron diffraction produced a superior high-angle diffraction pattern relative to p-XRD. Requiring only small amounts of sample, µ-Raman spectroscopy was used for the first time in this context as a potentially complementary technique to p-XRD. The chemical phases were identified as pure UO 2 in two materials, and as a mixture of UO 2, U 3O 8 and an intermediate species U 3Omore » 7 in the third material.« less

Comparing results of X-ray diffraction, µ-Raman spectroscopy and neutron diffraction when identifying chemical phases in seized nuclear material, during a comparative nuclear forensics exercise

DOE PAGES

Rondahl, Stina Holmgren; Pointurier, Fabien; Ahlinder, Linnea; ...

2018-01-24

This work presents the results for identification of chemical phases obtained by several laboratories as a part of an international nuclear forensic round-robin exercise. In this work powder X-ray diffraction (p-XRD) is regarded as the reference technique. Neutron diffraction produced a superior high-angle diffraction pattern relative to p-XRD. Requiring only small amounts of sample, µ-Raman spectroscopy was used for the first time in this context as a potentially complementary technique to p-XRD. The chemical phases were identified as pure UO 2 in two materials, and as a mixture of UO 2, U 3O 8 and an intermediate species U 3Omore » 7 in the third material.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Valderrama, Billy; He, Lingfeng; Henderson, Hunter B.

Fission products, such as krypton (Kr), are known to be insoluble within UO 2, segregating towards grain boundaries, eventually leading to a lowering of the thermal conductivity and fuel swelling. Recent computational studies have identified that differences in grain boundary structure have a significant effect on the segregation behavior of fission products. However, experimental work supporting these simulations is lacking. Atom probe tomography was used to measure the Kr distribution across grain boundaries in UO 2. Polycrystalline depleted-UO 2 samples was irradiated with 0.7 and 1.8 MeV Kr-ions and annealed to 1000ºC, 1300ºC, and 1600°C for 1 hour to producemore » a Kr-bubble dominated microstructure. The results of this work indicate a strong dependence of Kr concentration as a function of grain boundary structure. Temperature also influences grain boundary chemistry with greater Kr concentration evident at higher temperatures, resulting in a reduced Kr concentration in the bulk. While Kr migration is active at elevated temperatures, no changes in grain size or texture were observed in the irradiated UO 2 samples.« less

Average structure and local configuration of excess oxygen in UO(2+x).

PubMed

Wang, Jianwei; Ewing, Rodney C; Becker, Udo

2014-03-19

Determination of the local configuration of interacting defects in a crystalline, periodic solid is problematic because defects typically do not have a long-range periodicity. Uranium dioxide, the primary fuel for fission reactors, exists in hyperstoichiometric form, UO(2+x). Those excess oxygen atoms occur as interstitial defects, and these defects are not random but rather partially ordered. The widely-accepted model to date, the Willis cluster based on neutron diffraction, cannot be reconciled with the first-principles molecular dynamics simulations present here. We demonstrate that the Willis cluster is a fair representation of the numerical ratio of different interstitial O atoms; however, the model does not represent the actual local configuration. The simulations show that the average structure of UO(2+x) involves a combination of defect structures including split di-interstitial, di-interstitial, mono-interstitial, and the Willis cluster, and the latter is a transition state that provides for the fast diffusion of the defect cluster. The results provide new insights in differentiating the average structure from the local configuration of defects in a solid and the transport properties of UO(2+x).

Measurement of UO2 surface oxidation using grazing-incidence x-ray diffraction: Implications for nuclear forensics

NASA Astrophysics Data System (ADS)

Tracy, Cameron L.; Chen, Chien-Hung; Park, Sulgiye; Davisson, M. Lee; Ewing, Rodney C.

2018-04-01

Nuclear forensics involves determination of the origin and history of interdicted nuclear materials based on the detection of signatures associated with their production and trafficking. The surface oxidation undergone by UO2 when exposed to air is a potential signature of its atmospheric exposure during handling and transport. To assess the sensitivity of this oxidation to atmospheric parameters, surface sensitive grazing-incidence x-ray diffraction (GIXRD) measurements were performed on UO2 samples exposed to air of varying relative humidity (34%, 56%, and 95% RH) and temperature (room temperature, 50 °C, and 100 °C). Near-surface unit cell contraction was observed following exposure, indicating oxidation of the surface and accompanying reduction of the uranium cation ionic radii. The extent of unit cell contraction provides a measure of the extent of oxidation, allowing for comparison of the effects of various exposure conditions. No clear influence of relative humidity on the extent of oxidation was observed, with samples exhibiting similar degrees of unit cell contraction at all relative humidities investigated. In contrast, the thickness of the oxidized layers increased substantially with increasing temperature, such that differences on the order of 10 °C yielded readily observable crystallographic signatures of the exposure conditions.

Laser-induced breakdown spectroscopy of light water reactor simulated used nuclear fuel: Main oxide phase

DOE PAGES

Campbell, Keri R.; Judge, Elizabeth J.; Barefield, James E.; ...

2017-04-22

We show the analysis of light water reactor simulated used nuclear fuel using laser-induced breakdown spectroscopy (LIBS) is explored using a simplified version of the main oxide phase. The main oxide phase consists of the actinides, lanthanides, and zirconium. The purpose of this study is to develop a rapid, quantitative technique for measuring zirconium in a uranium dioxide matrix without the need to dissolve the material. A second set of materials including cerium oxide is also analyzed to determine precision and limit of detection (LOD) using LIBS in a complex matrix. Two types of samples are used in this study:more » binary and ternary oxide pellets. The ternary oxide, (U,Zr,Ce)O 2 pellets used in this study are a simplified version the main oxide phase of used nuclear fuel. The binary oxides, (U,Ce)O 2 and (U,Zr)O 2 are also examined to determine spectral emission lines for Ce and Zr, potential spectral interferences with uranium and baseline LOD values for Ce and Zr in a UO 2 matrix. In the spectral range of 200 to 800 nm, 33 cerium lines and 25 zirconium lines were identified and shown to have linear correlation values (R 2) > 0.97 for both the binary and ternary oxides. The cerium LOD in the (U,Ce)O 2 matrix ranged from 0.34 to 1.08 wt% and 0.94 to 1.22 wt% in (U,Ce,Zr)O 2 for 33 of Ce emission lines. The zirconium limit of detection in the (U,Zr)O 2 matrix ranged from 0.84 to 1.15 wt% and 0.99 to 1.10 wt% in (U,Ce,Zr)O 2 for 25 Zr lines. Finally, the effect of multiple elements in the plasma and the impact on the LOD is discussed.« less

Carbothermic Synthesis of ~820- m UN Kernels. Investigation of Process Variables

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lindemer, Terrence; Silva, Chinthaka M; Henry, Jr, John James

2015-06-01

This report details the continued investigation of process variables involved in converting sol-gel-derived, urainia-carbon microspheres to ~820-μm-dia. UN fuel kernels in flow-through, vertical refractory-metal crucibles at temperatures up to 2123 K. Experiments included calcining of air-dried UO 3-H 2O-C microspheres in Ar and H 2-containing gases, conversion of the resulting UO 2-C kernels to dense UO 2:2UC in the same gases and vacuum, and its conversion in N 2 to in UC 1-xN x. The thermodynamics of the relevant reactions were applied extensively to interpret and control the process variables. Producing the precursor UO 2:2UC kernel of ~96% theoretical densitymore » was required, but its subsequent conversion to UC 1-xN x at 2123 K was not accompanied by sintering and resulted in ~83-86% of theoretical density. Decreasing the UC 1-xN x kernel carbide component via HCN evolution was shown to be quantitatively consistent with present and past experiments and the only useful application of H2 in the entire process.« less

Roadmap to an Engineering-Scale Nuclear Fuel Performance & Safety Code

DOE Office of Scientific and Technical Information (OSTI.GOV)

Turner, John A; Clarno, Kevin T; Hansen, Glen A

2009-09-01

Developing new fuels and qualifying them for large-scale deployment in power reactors is a lengthy and expensive process, typically spanning a period of two decades from concept to licensing. Nuclear fuel designers serve an indispensable role in the process, at the initial exploratory phase as well as in analysis of the testing results. In recent years fuel performance capabilities based on first principles have been playing more of a role in what has traditionally been an empirically dominated process. Nonetheless, nuclear fuel behavior is based on the interaction of multiple complex phenomena, and recent evolutionary approaches are being applied moremore » on a phenomenon-by-phenomenon basis, targeting localized problems, as opposed to a systematic approach based on a fundamental understanding of all interacting parameters. Advanced nuclear fuels are generally more complex, and less understood, than the traditional fuels used in existing reactors (ceramic UO{sub 2} with burnable poisons and other minor additives). The added challenges are primarily caused by a less complete empirical database and, in the case of recycled fuel, the inherent variability in fuel compositions. It is clear that using the traditional approach to develop and qualify fuels over the entire range of variables pertinent to the U.S. Department of Energy (DOE) Office of Nuclear Energy on a timely basis with available funds would be very challenging, if not impossible. As a result the DOE Office of Nuclear Energy has launched the Nuclear Energy Advanced Modeling and Simulation (NEAMS) approach to revolutionize fuel development. This new approach is predicated upon transferring the recent advances in computational sciences and computer technologies into the fuel development program. The effort will couple computational science with recent advances in the fundamental understanding of physical phenomena through ab initio modeling and targeted phenomenological testing to leapfrog many fuel-development activities. Realizing the full benefits of this approach will likely take some time. However, it is important that the developmental activities for modeling and simulation be tightly coupled with the experimental activities to maximize feedback effects and accelerate both the experimental and analytical elements of the program toward a common objective. The close integration of modeling and simulation and experimental activities is key to developing a useful fuel performance simulation capability, providing a validated design and analysis tool, and understanding the uncertainties within the models and design process. The efforts of this project are integrally connected to the Transmutation Fuels Campaign (TFC), which maintains as a primary objective to formulate, fabricate, and qualify a transuranic-based fuel with added minor actinides for use in future fast reactors. Additional details of the TFC scope can be found in the Transmutation Fuels Campaign Execution Plan. This project is an integral component of the TFC modeling and simulation effort, and this multiyear plan borrowed liberally from the Transmutation Fuels Campaign Modeling and Simulation Roadmap. This document provides the multiyear staged development plan to develop a continuum-level Integrated Performance and Safety Code (IPSC) to predict the behavior of the fuel and cladding during normal reactor operations and anticipated transients up to the point of clad breach.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carmack, Jon; Hayes, Steven; Walters, L. C.

This document explores startup fuel options for a proposed test/demonstration fast reactor. The fuel options considered are the metallic fuels U-Zr and U-Pu-Zr and the ceramic fuels UO 2 and UO 2-PuO 2 (MOX). Attributes of the candidate fuel choices considered were feedstock availability, fabrication feasibility, rough order of magnitude cost and schedule, and the existing irradiation performance database. The reactor-grade plutonium bearing fuels (U-Pu-Zr and MOX) were eliminated from consideration as the initial startup fuels because the availability and isotopics of domestic plutonium feedstock is uncertain. There are international sources of reactor grade plutonium feedstock but isotopics and availabilitymore » are also uncertain. Weapons grade plutonium is the only possible source of Pu feedstock in sufficient quantities needed to fuel a startup core. Currently, the available U.S. source of (excess) weapons-grade plutonium is designated for irradiation in commercial light water reactors (LWR) to a level that would preclude diversion. Weapons-grade plutonium also contains a significant concentration of gallium. Gallium presents a potential issue for both the fabrication of MOX fuel as well as possible performance issues for metallic fuel. Also, the construction of a fuel fabrication line for plutonium fuels, with or without a line to remove gallium, is expected to be considerably more expensive than for uranium fuels. In the case of U-Pu-Zr, a relatively small number of fuel pins have been irradiated to high burnup, and in no case has a full assembly been irradiated to high burnup without disassembly and re-constitution. For MOX fuel, the irradiation database from the Fast Flux Test Facility (FFTF) is extensive. If a significant source of either weapons-grade or reactor-grade Pu became available (i.e., from an international source), a startup core based on Pu could be reconsidered.« less

Probing the Oxygen Environment in UO22+ by Solid-State O-17 Nuclear Magnetic Resonance Spectroscopy and Relativistic Density Functional Calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cho, Herman M.; De Jong, Wibe A.; Soderquist, Chuck Z.

A combined theoretical and solid-state O-17 NMR study of the electronic structure of the uranyl ion UO22+ in (NH4)4UO2(CO3)3 and rutherfordine UO2CO3 is presented, the former representing a system with a hydrogen-bonding environment around the uranyl oxygens, and the latter exemplifying a uranyl environment without hydrogens. A fully relativistic ab initio treatment reveals unique features of the U-O covalent bond, including the finding of O-17 chemical shift anisotropies that are among the largest ever reported (>1200 ppm). Computational results for the oxygen electric field gradient tensor are found to be consistently larger in magnitude than experimental solid-state O-17 NMR measurementsmore » in a 7.05 T magnetic field indicate. A modified version of the Solomon theory of the two-spin echo amplitude for a spin-5/2 nucleus is developed and applied to the analysis of the O-17 echo signal of UO22+. The William R. Wiley environmental Molecular Sciences Laboratory is a US Department of Energy national scientific user facility located at Pacific Northwest National Laboratory (PNNL) in Richland, Washington. PNNL is operated by Battelle for the US Department of Energy.« less

3D Microstructural Characterization of Uranium Oxide as a Surrogate Nuclear Fuel: Effect of Oxygen Stoichiometry on Grain Boundary Distributions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudman, K.; Dickerson, P.; Byler, Darrin David

The initial microstructure of an oxide fuel can play a key role in its performance. At low burn-ups, the diffusion of fission products can depend strongly on grain size and grain boundary (GB) characteristics, which in turn depend on processing conditions and oxygen stoichiometry. Serial sectioning techniques using Focused Ion Beam were developed to obtain Electron Backscatter Diffraction (EBSD) data for depleted UO2 pellets that were processed to obtain 3 different oxygen stoichiometries. The EBSD data were used to create 3D microstructure reconstructions and to gather statistical information on the grain and GB crystallography, with emphasis on identifying the charactermore » (twist, tilt, mixed) for GBs that meet the Coincident Site Lattice (CSL) criterion as well as GBs with the most common misorientation angles. Data on dihedral angles at triple points were also collected. The results were compared across different samples to understand effects of oxygen content on microstructure evolution.« less

Static electric dipole polarizabilities of An(5+/6+) and AnO2 (+/2+) (An = U, Np, and Pu) ions.

PubMed

Parmar, Payal; Peterson, Kirk A; Clark, Aurora E

2014-12-21

The parallel components of static electric dipole polarizabilities have been calculated for the lowest lying spin-orbit states of the penta- and hexavalent oxidation states of the actinides (An) U, Np, and Pu, in both their atomic and molecular diyl ion forms (An(5+/6+) and AnO2 (+/2+)) using the numerical finite-field technique within a four-component relativistic framework. The four-component Dirac-Hartree-Fock method formed the reference for MP2 and CCSD(T) calculations, while multireference Fock space coupled-cluster (FSCC), intermediate Hamiltonian Fock space coupled-cluster (IH-FSCC) and Kramers restricted configuration interaction (KRCI) methods were used to incorporate additional electron correlation. It is observed that electron correlation has significant (∼5 a.u.(3)) impact upon the parallel component of the polarizabilities of the diyls. To the best of our knowledge, these quantities have not been previously reported and they can serve as reference values in the determination of various electronic and response properties (for example intermolecular forces, optical properties, etc.) relevant to the nuclear fuel cycle and material science applications. The highest quality numbers for the parallel components (αzz) of the polarizability for the lowest Ω levels corresponding to the ground electronic states are (in a.u.(3)) 44.15 and 41.17 for UO2 (+) and UO2 (2+), respectively, 45.64 and 41.42 for NpO2 (+) and NpO2 (2+), respectively, and 47.15 for the PuO2 (+) ion.

Carbon monoxide formation in UO 2 kerneled HTR fuel particles containing oxygen getters

NASA Astrophysics Data System (ADS)

Proksch, E.; Strigl, A.; Nabielek, H.

1986-06-01

Mass spectrometric measurements of CO in irradiated UO 2 kerneled HTR fuel particles containing various oxygen getters are summarized and evaluated. Uranium carbide addition in the 3 to 15% range reduces the CO release by factors between 25 and 80, up to burn-up levels as high as 70% FIMA. Unintentional gettering by SiC in TRISO coated particles with failed inner pyrocarbon layers results in CO reduction factors between 15 and 110. For ZrC, only somewhat ambiguous results have been obtained; most likely, ZrC results in CO reduction by a factor of about 40. Ce 2O 3 and La 2O 3 seem to be somewhat less effective than the three carbides; for Ce 2O 3, reduction factors between 3 and 15 have been found. However, these results are possibly incorrect due to premature oxidation of the getter already during fabrication. Addition of SiO 2 + Al 2O 3 has no influence on CO release at all.

In situ synthesis and characterization of uranium carbide using high temperature neutron diffraction

NASA Astrophysics Data System (ADS)

Reiche, H. Matthias; Vogel, Sven C.; Tang, Ming

2016-04-01

We investigated the formation of UCx from UO2+x and graphite in situ using neutron diffraction at high temperatures with particular focus on resolving the conflicting reports on the crystal structure of non-quenchable cubic UC2. The agents were UO2 nanopowder, which closely imitates nano grains observed in spent reactor fuels, and graphite powder. In situ neutron diffraction revealed the onset of the UO2 + 2C → UC + CO2 reaction at 1440 °C, with its completion at 1500 °C. Upon further heating, carbon diffuses into the uranium carbide forming C2 groups at the octahedral sites. This resulting high temperature cubic UC2 phase is similar to the NaCl-type structure as proposed by Bowman et al. Our novel experimental data provide insights into the mechanism and kinetics of formation of UC as well as characteristics of the high temperature cubic UC2 phase which agree with proposed rotational rehybridization found from simulations by Wen et al.

PM-1 NUCLEAR POWER PLANT PROGRAM. Quarterly Progress Report No. 2 for June 1 to August 31, 1959

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sieg, J.S.; Smith, E.H.

1959-10-01

The objective of the contract is the design, development, fabrication, installation, and initial testing and operation of a prepackaged air- transportable pressurized water reactor nuclear power plant, the PM-1. The specified output is 1 Mwe and 7 million Btu/hr of heat. The plant is to be operational by March 1962. The principal efforts were completion of the plant parametric study and preparation of the preliminary design. A summary of design parameters is given. Systems development work included study and selection of packages for full-scale testing, a survey of in-core instrumentation techniques, control and instrumentation development, and development of components formore » the steam generator, condenser, and turbine generator, which are not commercially available. Reactor development work included completion of the parametric zeropower experiments and preparrtions for a flexible zeropower test program, a revision of plans for irradiation testing PM-1 fuel elements, initiation of a reactor flow test program, outliring of a heat tnansfer test program, completion of the seven-tube test section (SETCH-1) tests, and evaluation of control rod actuators leading to specification of a magnetic jack-type control rod drive similar to that reported in ANL-5768. Completion of the prelimirary design led to initiation of the final design effort, which will be the principal activity during the next two project quarters. Preparations for core fabrication included procurement of core cladding material for the zero-power teat core, arrangement with a subcontractor to convent UF/sub 6/ to UO/sub 2/ and to commence delivery of the oxide during the next quarter, development of fuel element fabrication and ultrasonic testing techniques, study of control rod materials, UO/sub 2/ recovery techniques, and boron analysis methods. Preliminary work on site preparation was pursued with receipt of USAEC approval for a location on the eastern slope of Warren Peak at Sundance, Wyoming. A survey of this site is underway. A preliminary Hazards Summary Report is in preparation. (For preceding period see MND-M-1812.) (auth)« less

Simulation of xenon, uranium vacancy and interstitial diffusion and grain boundary segregation in UO 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andersson, Anders D.; Tonks, Michael R.; Casillas, Luis

2014-10-31

In light water reactor fuel, gaseous fission products segregate to grain boundaries, resulting in the nucleation and growth of large intergranular fission gas bubbles. Based on the mechanisms established from density functional theory (DFT) and empirical potential calculations 1, continuum models for diffusion of xenon (Xe), uranium (U) vacancies and U interstitials in UO 2 have been derived for both intrinsic conditions and under irradiation. Segregation of Xe to grain boundaries is described by combining the bulk diffusion model with a model for the interaction between Xe atoms and three different grain boundaries in UO 2 ( Σ5 tilt, Σ5more » twist and a high angle random boundary),as derived from atomistic calculations. All models are implemented in the MARMOT phase field code, which is used to calculate effective Xe and U diffusivities as well as redistribution for a few simple microstructures.« less

Validation of the new code package APOLLO2.8 for accurate PWR neutronics calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Santamarina, A.; Bernard, D.; Blaise, P.

2013-07-01

This paper summarizes the Qualification work performed to demonstrate the accuracy of the new APOLLO2.S/SHEM-MOC package based on JEFF3.1.1 nuclear data file for the prediction of PWR neutronics parameters. This experimental validation is based on PWR mock-up critical experiments performed in the EOLE/MINERVE zero-power reactors and on P.I. Es on spent fuel assemblies from the French PWRs. The Calculation-Experiment comparison for the main design parameters is presented: reactivity of UOX and MOX lattices, depletion calculation and fuel inventory, reactivity loss with burnup, pin-by-pin power maps, Doppler coefficient, Moderator Temperature Coefficient, Void coefficient, UO{sub 2}-Gd{sub 2}O{sub 3} poisoning worth, Efficiency ofmore » Ag-In-Cd and B4C control rods, Reflector Saving for both standard 2-cm baffle and GEN3 advanced thick SS reflector. From this qualification process, calculation biases and associated uncertainties are derived. This code package APOLLO2.8 is already implemented in the ARCADIA new AREVA calculation chain for core physics and is currently under implementation in the future neutronics package of the French utility Electricite de France. (authors)« less

Development of Impregnated Agglomerate Pelletization (IAP) process for fabrication of (Th,U)O 2 mixed oxide pellets

NASA Astrophysics Data System (ADS)

Khot, P. M.; Nehete, Y. G.; Fulzele, A. K.; Baghra, Chetan; Mishra, A. K.; Afzal, Mohd.; Panakkal, J. P.; Kamath, H. S.

2012-01-01

Impregnated Agglomerate Pelletization (IAP) technique has been developed at Advanced Fuel Fabrication Facility (AFFF), BARC, Tarapur, for manufacturing (Th, 233U)O 2 mixed oxide fuel pellets, which are remotely fabricated in hot cell or shielded glove box facilities to reduce man-rem problem associated with 232U daughter radionuclides. This technique is being investigated to fabricate the fuel for Indian Advanced Heavy Water Reactor (AHWR). In the IAP process, ThO 2 is converted to free flowing spheroids by powder extrusion route in an unshielded facility which are then coated with uranyl nitrate solution in a shielded facility. The dried coated agglomerate is finally compacted and then sintered in oxidizing/reducing atmosphere to obtain high density (Th,U)O 2 pellets. In this study, fabrication of (Th,U)O 2 mixed oxide pellets containing 3-5 wt.% UO 2 was carried out by IAP process. The pellets obtained were characterized using optical microscopy, XRD and alpha autoradiography. The results obtained were compared with the results for the pellets fabricated by other routes such as Coated Agglomerate Pelletization (CAP) and Powder Oxide Pelletization (POP) route.

Reactor physics behavior of transuranic-bearing TRISO-particle fuel in a pressurized water reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pope, M. A.; Sen, R. S.; Ougouag, A. M.

2012-07-01

Calculations have been performed to assess the neutronic behavior of pins of Fully-Ceramic Micro-encapsulated (FCM) fuel in otherwise-conventional Pressurized Water Reactor (PWR) fuel pins. The FCM fuel contains transuranic (TRU) - only oxide fuel in tri-isotropic (TRISO) particles with the TRU loading coming from the spent fuel of a conventional LWR after 5 years of cooling. Use of the TRISO particle fuel would provide an additional barrier to fission product release in the event of cladding failure. Depletion calculations were performed to evaluate reactivity-limited burnup of the TRU-only FCM fuel. These calculations showed that due to relatively little space availablemore » for fuel, the achievable burnup with these pins alone is quite small. Various reactivity parameters were also evaluated at each burnup step including moderator temperature coefficient (MTC), Doppler, and soluble boron worth. These were compared to reference UO{sub 2} and MOX unit cells. The TRU-only FCM fuel exhibits degraded MTC and Doppler coefficients relative to UO{sub 2} and MOX. Also, the reactivity effects of coolant voiding suggest that the behavior of this fuel would be similar to a MOX fuel of very high plutonium fraction, which are known to have positive void reactivity. In general, loading of TRU-only FCM fuel into an assembly without significant quantities of uranium presents challenges to the reactor design. However, if such FCM fuel pins are included in a heterogeneous assembly alongside LEU fuel pins, the overall reactivity behavior would be dominated by the uranium pins while attractive TRU destruction performance levels in the TRU-only FCM fuel pins is retained. From this work, it is concluded that use of heterogeneous assemblies such as these appears feasible from a preliminary reactor physics standpoint. (authors)« less

Reactor Physics Behavior of Transuranic-Bearing TRISO-Particle Fuel in a Pressurized Water Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Michael A. Pope; R. Sonat Sen; Abderrafi M. Ougouag

2012-04-01

Calculations have been performed to assess the neutronic behavior of pins of Fully-Ceramic Micro-encapsulated (FCM) fuel in otherwise-conventional Pressurized Water Reactor (PWR) fuel pins. The FCM fuel contains transuranic (TRU)-only oxide fuel in tri-isotropic (TRISO) particles with the TRU loading coming from the spent fuel of a conventional LWR after 5 years of cooling. Use of the TRISO particle fuel would provide an additional barrier to fission product release in the event of cladding failure. Depletion calculations were performed to evaluate reactivity-limited burnup of the TRU-only FCM fuel. These calculations showed that due to relatively little space available for fuel,more » the achievable burnup with these pins alone is quite small. Various reactivity parameters were also evaluated at each burnup step including moderator temperature coefficient (MTC), Doppler, and soluble boron worth. These were compared to reference UO{sub 2} and MOX unit cells. The TRU-only FCM fuel exhibits degraded MTC and Doppler coefficients relative to UO{sub 2} and MOX. Also, the reactivity effects of coolant voiding suggest that the behavior of this fuel would be similar to a MOX fuel of very high plutonium fraction, which are known to have positive void reactivity. In general, loading of TRU-only FCM fuel into an assembly without significant quantities of uranium presents challenges to the reactor design. However, if such FCM fuel pins are included in a heterogeneous assembly alongside LEU fuel pins, the overall reactivity behavior would be dominated by the uranium pins while attractive TRU destruction performance levels in the TRU-only FCM fuel pins is. From this work, it is concluded that use of heterogeneous assemblies such as these appears feasible from a preliminary reactor physics standpoint.« less

Thorium-based mixed oxide fuel in a pressurized water reactor: A feasibility analysis with MCNP

NASA Astrophysics Data System (ADS)

Tucker, Lucas Powelson

This dissertation investigates techniques for spent fuel monitoring, and assesses the feasibility of using a thorium-based mixed oxide fuel in a conventional pressurized water reactor for plutonium disposition. Both non-paralyzing and paralyzing dead-time calculations were performed for the Portable Spectroscopic Fast Neutron Probe (N-Probe), which can be used for spent fuel interrogation. Also, a Canberra 3He neutron detector's dead-time was estimated using a combination of subcritical assembly measurements and MCNP simulations. Next, a multitude of fission products were identified as candidates for burnup and spent fuel analysis of irradiated mixed oxide fuel. The best isotopes for these applications were identified by investigating half-life, photon energy, fission yield, branching ratios, production modes, thermal neutron absorption cross section and fuel matrix diffusivity. 132I and 97Nb were identified as good candidates for MOX fuel on-line burnup analysis. In the second, and most important, part of this work, the feasibility of utilizing ThMOX fuel in a pressurized water reactor (PWR) was first examined under steady-state, beginning of life conditions. Using a three-dimensional MCNP model of a Westinghouse-type 17x17 PWR, several fuel compositions and configurations of a one-third ThMOX core were compared to a 100% UO2 core. A blanket-type arrangement of 5.5 wt% PuO2 was determined to be the best candidate for further analysis. Next, the safety of the ThMOX configuration was evaluated through three cycles of burnup at several using the following metrics: axial and radial nuclear hot channel factors, moderator and fuel temperature coefficients, delayed neutron fraction, and shutdown margin. Additionally, the performance of the ThMOX configuration was assessed by tracking cycle length, plutonium destroyed, and fission product poison concentration.

Theoretical analysis of swelling characteristics of cylindrical uranium dioxide fuel pins with a niobium - 1-percent-zirconium clad

NASA Technical Reports Server (NTRS)

Saltsman, J. F.

1973-01-01

The relations between clad creep strain and fuel volume swelling are shown for cylindrical UO2 fuel pins with a Nb-1Zr clad. These relations were obtained by using the computer code CYGRO-2. These clad-strain - fuel-volume-swelling relations may be used with any fuel-volume-swelling model, provided the fuel volume swelling is isotropic and independent of the clad restraints. The effects of clad temperature (over a range from 118 to 1642 K (2010 to 2960 R)), pin diameter, clad thickness and central hole size in the fuel have been investigated. In all calculations the irradiation time was 500 hours. The burnup rate was varied.

Nuclear Energy Advanced Modeling and Simulation (NEAMS) Accident Tolerant Fuels High Impact Problem: Coordinate Multiscale FeCrAl Modeling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gamble, K. A.; Hales, J. D.; Zhang, Y.

Since the events at the Fukushima-Daiichi nuclear power plant in March 2011 significant research has unfolded at national laboratories, universities and other institutions into alternative materials that have potential enhanced ac- cident tolerance when compared to traditional UO2 fuel zircaloy clad fuel rods. One of the potential replacement claddings are iron-chromium-alunimum (FeCrAl) alloys due to their increased oxidation resistance [1–4] and higher strength [1, 2]. While the oxidation characteristics of FeCrAl are a benefit for accident tolerance, the thermal neu- tron absorption cross section of FeCrAl is about ten times that of Zircaloy. This neutronic penalty necessitates thinner cladding. Thismore » allows for slightly larger pellets to give the same cold gap width in the rod. However, the slight increase in pellet diameter is not sufficient to compensate for the neutronic penalty and enriching the fuel beyond the current 5% limit appears to be necessary [5]. Current estimates indicate that this neutronic penalty will impose an increase in fuel cost of 15-35% [1, 2]. In addition to the neutronic disadvantage, it is anticipated that tritium release to the coolant will be larger because the permeability of hydrogen in FeCrAl is about 100 times higher than in Zircaloy [6]. Also, radiation-induced hardening and embrittlement of FeCrAl need to be fully characterized experimentally [7]. Due to the aggressive development schedule for inserting some of the potential materials into lead test assemblies or rods by 2022 [8] multiscale multiphysics modeling approaches have been used to provide insight into these the use of FeCrAl as a cladding material. The purpose of this letter report is to highlight the multiscale modeling effort for iron-chromium-alunimum (FeCrAl) cladding alloys as part of the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program through its Accident Tolerant Fuel (ATF) High Impact Problem (HIP). The approach taken throughout the HIP is to utilize lower length scale approaches (e.g., density functional theory, cluster dynamics, rate theory, phase field, and Visco-Plastic- Self-Consistent (VPSC)) to develop more physically informed models at the engineering scale for use in the BISON [9] fuel performance code.« less

Irradiation behaviour of the large grained UO{sub 2} fuel pellet in the transient conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kosaka, Yuji; Watanabe, Seiichi; Arakawa, Yasushi

2007-07-01

In order to achieve a high duty fuel rod design, it is the key issue to suppress the fission gas release from the view point of the fuel rod inner pressure design. The large grain UO{sub 2} pellet is one of the candidates to meet such a requirement by reducing the fission gas release especially at high power and/or high burnup. We have demonstrated the fuel performance of the large grain pellet in the PWR irradiation conditions, which was fabricated with no additive but with active UO{sub 2} powder through the conventional pelletizing process for the normal grain size pellet.more » According to the mechanism of the fission gas retention, there may be a concern about the larger gas bubble swelling of the large grain pellet at the power transient conditions which may increase the potential of the PCMI failure. In this paper, we focus on the differences of the dimensional change in comparison among the pellets with the different grain sizes at the power transient conditions. The power ramp tests were carried out on the high burnup fuel rods of normal and large grain pellet with no additive, which had been irradiated in the PWR conditions up to around 60 GWd/t at peak position. The detailed PIE results revealed that the volume increment due to the power ramp clearly showed the dependence on the grain size as well as the fission gas release and suggested that the larger grain with no additive may suppress the gas bubble swelling at the power transient conditions. According to the experimental results, it is concluded that the large grain pellet with no additive does not deteriorate the irradiation performance during the power transient conditions from the view point of the gas bubble swelling. (authors)« less

Theoretical analysis of uranium-doped thorium dioxide: Introduction of a thoria force field with explicit polarization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shields, A. E.; Ruiz Hernandez, S. E.; Leeuw, N. H. de, E-mail: DeLeeuwN@Cardiff.ac.uk

2015-08-15

Thorium dioxide is used industrially in high temperature applications, but more insight is needed into the behavior of the material as part of a mixed-oxide (MOX) nuclear fuel, incorporating uranium. We have developed a new interatomic potential model including polarizability via a shell model, and commensurate with a prominent existing UO{sub 2} potential, to conduct configurational analyses and to investigate the thermophysical properties of uranium-doped ThO{sub 2}. Using the GULP and Site Occupancy Disorder (SOD) computational codes, we have analyzed the distribution of low concentrations of uranium in the bulk material, where we have not observed the formation of uraniummore » clusters or the dominance of a single preferred configuration. We have calculated thermophysical properties of pure thorium dioxide and Th{sub (1−x)}U{sub x}O{sub 2} which generated values in very good agreement with experimental data.« less

Space and Time Distribution of Pu Isotopes inside The First Experimental Fuel Pin Designed for PWR and Manufactured in Indonesia

NASA Astrophysics Data System (ADS)

Suwardi; Setiawan, J.; Susilo, J.

2017-01-01

The first short fuel pin containing natural UO2 pellet in Zry4 cladding has been prepared and planned to be tested in power ramp irradiation. An irradiation test should be designed to allow an experiment can be performed safely and giving maximum results of many performance aspects of design and manufacturing. Performance analysis to the fuel specimen shows that the specimen is not match to be used for power ramp testing. Enlargement by 0.20 mm of pellet diameter has been proposed. The present work is evaluation of modified design for important aspect of isotopic Pu distribution during irradiation test, because generated Pu isotopes in natural UO2 fuel, contribute more power relative to the contribution by enriched UO2 fuel. The axial profile of neutrons flux have been chosen from both experimental measurement and model calculation. The parameters of ramp power has been obtained from statistical experiment data. A simplified and typical base-load commercial PHWR profile of LHR history has been chosen, to determine the minimum irradiation time before ramp test can be performed. The data design and Mat pro XI materials properties models have been chosen. The axial profile of neutrons flux has been accommodated by 5 slices of discrete pin. The Pu distribution of slice-4 with highest power rate has been chosen to be evaluated. The radial discretion of pellet and cladding and numerical parameter have been used the default best practice of TU. The results shows that Pu 239 increased rapidly. The maximum burn up of slice 4 at upper the median slice, it reached nearly 90% of maximum value at about 6000 h with peak of 0.8%a Pu/HM at 22000 h, which is higher than initial U 235. Each 240, 241 and 240 Pu grows slower and ends up to 0.4, 0.2 and 0.18 % respectively. This results can be used for verification of other aspect of fuel behavior in the modeling results and also can be used as guide and comparison to the future post irradiation examination for Pu isotopes distribution.

NEAMS Update. Quarterly Report for January - March 2014

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stan, Marius

2014-08-01

This quarterly report covers the following points: A fully three-dimensional smeared cracking model has been implemented and tested in BISON; DAKOTA-BISON was used to study the parameters that govern heat transfer across the fuel-cladding; Calculations of grain boundary mobility in UO 2 have been extended to high temperatures; Mesh adaptivity is being employed in MARMOT simulations to increase computational efficiency; Molecular dynamics simulations have shown correlation between atomic displacements and the anisotropic thermal conductivity in UO 2; The SHARP team continues to address the application of the toolkit to assembly deformations driven by reactivity feedback; The Nek5000 team has extendedmore » the low-Machnumber capability to mixtures with multiple species; The generalized cross section library has been tested for various fuel assemblies and reactor types; and The subgroup cross-section interface was successfully implemented in PROTEUS-SN (page 6).« less

Modelling of pore coarsening in the high burn-up structure of UO2 fuel

NASA Astrophysics Data System (ADS)

Veshchunov, M. S.; Tarasov, V. I.

2017-05-01

The model for coalescence of randomly distributed immobile pores owing to their growth and impingement, applied by the authors earlier to consideration of the porosity evolution in the high burn-up structure (HBS) at the UO2 fuel pellet periphery (rim zone), was further developed and validated. Predictions of the original model, taking into consideration only binary impingements of growing immobile pores, qualitatively correctly describe the decrease of the pore number density with the increase of the fractional porosity, however notably underestimate the coalescence rate at high burn-ups attained in the outmost region of the rim zone. In order to overcome this discrepancy, the next approximation of the model taking into consideration triple impingements of growing pores was developed. The advanced model provides a reasonable consent with experimental data, thus demonstrating the validity of the proposed pore coarsening mechanism in the HBS.

Determination of gaseous fission product behavior near the cerium dioxide Σ 3 (111)/[11 bar0] tilt grain boundary via first-principles study

NASA Astrophysics Data System (ADS)

Xi, Jianqi; Liu, Bin; Xu, Haixuan; Zhang, Yanwen; Weber, William J.

2018-02-01

Grain boundaries (GBs) are the most abundant structural defects in nanostructured nuclear fuels and play an important role in determining fission product behavior, which further affects the performance of nuclear fuels. In this work, cerium dioxide (CeO2) is used as a surrogate material for mixed oxide fuels to understand gaseous fission product behavior, specifically Xe. First-principles calculations are employed to comprehensively study the behavior of Xe and trap sites for Xe near the Σ 3 (111)/[11 bar0] grain boundary in CeO2, which will provide guidance on overall trends for Xe stability and diffusion at grain boundaries vs in the bulk. Significant segregation behavior of trap sites, regardless of charge states, is observed near the GB. This is mainly ascribed to the local atomic structure near the GB, which results in weaker bond strength and more negative segregation energies. For Xe, however, the segregation profile near the GB is different. Our calculations show that, as the size of trap sites increases, the segregation propensity of Xe is reduced. In addition, under hyper-stoichiometric conditions, the solubility of Xe trapped at the GB is significantly higher than that in the bulk, suggesting higher Xe concentration than that in the bulk. The results of this work demonstrate that the diffusion mechanism of Xe in CeO2 is comparable to that in UO2. The diffusion activation energies of Xe atoms in the Σ 3 GB are lower than that in the bulk CeO2. These results suggest that the diffusivity of Xe atoms is higher along the GB than that in the bulk, which enhances the aggregation of Xe atoms near the GB.

Comparative density functional study of the complexes [UO2(CO3)3]4- and [(UO2)3(CO3)6]6- in aqueous solution.

PubMed

Schlosser, Florian; Moskaleva, Lyudmila V; Kremleva, Alena; Krüger, Sven; Rösch, Notker

2010-06-28

With a relativistic all-electron density functional method, we studied two anionic uranium(VI) carbonate complexes that are important for uranium speciation and transport in aqueous medium, the mononuclear tris(carbonato) complex [UO(2)(CO(3))(3)](4-) and the trinuclear hexa(carbonato) complex [(UO(2))(3)(CO(3))(6)](6-). Focusing on the structures in solution, we applied for the first time a full solvation treatment to these complexes. We approximated short-range effects by explicit aqua ligands and described long-range electrostatic interactions via a polarizable continuum model. Structures and vibrational frequencies of "gas-phase" models with explicit aqua ligands agree best with experiment. This is accidental because the continuum model of the solvent to some extent overestimates the electrostatic interactions of these highly anionic systems with the bulk solvent. The calculated free energy change when three mono-nuclear complexes associate to the trinuclear complex, agrees well with experiment and supports the formation of the latter species upon acidification of a uranyl carbonate solution.

Modernization at the Y-12 National Security Complex: A Case for Additional Experimental Benchmarks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thornbury, M. L.; Juarez, C.; Krass, A. W.

Efforts are underway at the Y-12 National Security Complex (Y-12) to modernize the recovery, purification, and consolidation of un-irradiated, highly enriched uranium metal. Successful integration of advanced technology such as Electrorefining (ER) eliminates many of the intermediate chemistry systems and processes that are the current and historical basis of the nuclear fuel cycle at Y-12. The cost of operations, the inventory of hazardous chemicals, and the volume of waste are significantly reduced by ER. It also introduces unique material forms and compositions related to the chemistry of chloride salts for further consideration in safety analysis and engineering. The work hereinmore » briefly describes recent investigations of nuclear criticality for 235UO2Cl2 (uranyl chloride) and 6LiCl (lithium chloride) in aqueous solution. Of particular interest is the minimum critical mass of highly enriched uranium as a function of the molar ratio of 6Li to 235U. The work herein also briefly describes recent investigations of nuclear criticality for 235U metal reflected by salt mixtures of 6LiCl or 7LiCl (lithium chloride), KCl (potassium chloride), and 235UCl3 or 238UCl3 (uranium tri-chloride). Computational methods for analysis of nuclear criticality safety and published nuclear data are employed in the absence of directly relevant experimental criticality benchmarks.« less

DEVELOPMENT OF PLUTONIUM-BEARING FUEL MATERIALS. Progress Report, October 1-December 31, 1961

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

1962-10-31

Continued effort is reported on preparation and characterization of PuO/ sub 2/ and UO/sub 2/-- PuO/sub 2/ mixtures. Sintering and characterization of pellets for irradiation tests was emphasized, and efforts were also devoted to plasma torch production of spherical PuO /sub 2/ and coating of oxide materials. PuO/sub 2/ produced by the oxalate process from low concentration feed contains agglomerates which are not readily broken down, while that produced from normal feed contains larger agglomerates which are easily dispersed ultrasonically, and are more easily calcined. The water filtration method for determining total porosity of powders was adapted for use withmore » PuO/sub 2/. Moisture pickup studies show that the problems encountered with PuO/sub 2/ are similar to those found in handling ceramic-grade UO/. Reproducibility tests carried out on UO/sub 2/--PuO/ sub 2/ mixtures indicate that production methods are satisfactory. Lab-scale experiments on production of PuO/sub 2/-- UO/sub 2/feed for the plasma torch indicate that further work is worthwhile. Adaptation of a potentiometric filtration for Pu is reported. A twophase microstructure found in PuO/ after sintering in N6% H atmosphere was identified as PuO/sub 2/ and cubic Pu/sub 2/O/ sub 3/. Spherical particles were produced in the plasma torch using crushed or preformed high-fired particles. Spherical particles of PuO/sub 2/ were also produced by a multi-step process of drying, pressing, granulation, sizing, shaping, and sintering. Reactor physics studies were continued to determine the effect of cross section assumptions on the calculated behavior of Pu-fueled near- thermal reactor systems. It was concluded that relatively long core life (reactivity limiting) is attainable with these systems. (J.R.D.)« less

Analysis of the TREAT LEU Conceptual Design

DOE Office of Scientific and Technical Information (OSTI.GOV)

Connaway, H. M.; Kontogeorgakos, D. C.; Papadias, D. D.

2016-03-01

Analyses were performed to evaluate the performance of the low enriched uranium (LEU) conceptual design fuel for the conversion of the Transient Reactor Test Facility (TREAT) from its current highly enriched uranium (HEU) fuel. TREAT is an experimental nuclear reactor designed to produce high neutron flux transients for the testing of reactor fuels and other materials. TREAT is currently in non-operational standby, but is being restarted under the U.S. Department of Energy’s Resumption of Transient Testing Program. The conversion of TREAT is being pursued in keeping with the mission of the Department of Energy National Nuclear Security Administration’s Material Managementmore » and Minimization (M3) Reactor Conversion Program. The focus of this study was to demonstrate that the converted LEU core is capable of maintaining the performance of the existing HEU core, while continuing to operate safely. Neutronic and thermal hydraulic simulations have been performed to evaluate the performance of the LEU conceptual-design core under both steady-state and transient conditions, for both normal operation and reactivity insertion accident scenarios. In addition, ancillary safety analyses which were performed for previous LEU design concepts have been reviewed and updated as-needed, in order to evaluate if the converted LEU core will function safely with all existing facility systems. Simulations were also performed to evaluate the detailed behavior of the UO 2-graphite fuel, to support future fuel manufacturing decisions regarding particle size specifications. The results of these analyses will be used in conjunction with work being performed at Idaho National Laboratory and Los Alamos National Laboratory, in order to develop the Conceptual Design Report project deliverable.« less

Calculation of Internal Pressures in the Fuel Tube of a Nuclear Reactor

NASA Technical Reports Server (NTRS)

Rosenbaum, B. M.; Allen, G.

1952-01-01

General procedures for computing internal pressures in fuel tubes of nuclear reactors are described and the effects on the pressure of varying neutron flux, fissioning material, and operating temperatures are discussed. A general proof is given that during pile operation each fission product is monotonically increasing and therefore a maximum amount of all elements is present at the time of shit down. The post-shutdown build-up of elements that are held in check during pile operation because of their inordinately high capture cross sections is calculated quantitatively. An account of chemical interactions between the many fission-product elements and the resulting effect on the total pressure completes the discussion. The general methods are illustrated by calculations applied to a system consisting of 90 percent enriched U235 in the form of UO2 packed into a hollow metal cylinder or "pin", operating at a flux of 8 x 10(exp 14) at 2000 F. Calculations of the pressure inside a pin are made with and without a sodium metal heat-transfer additive. The bulk of the pressure is shown to depend on the four elements, xenon, krypton, rubidium, and cesium; the amount of free oxygen, however, was also significant. For a shutdown time of 10(exp 6) seconds, the pressure was about 100 atmospheres.

Thermal conductivity of heterogeneous LWR MOX fuels

NASA Astrophysics Data System (ADS)

Staicu, D.; Barker, M.

2013-11-01

It is generally observed that the thermal conductivity of LWR MOX fuel is lower than that of pure UO2. For MOX, the degradation is usually only interpreted as an effect of the substitution of U atoms by Pu. This hypothesis is however in contradiction with the observations of Duriez and Philiponneau showing that the thermal conductivity of MOX is independent of the Pu content in the ranges 3-15 and 15-30 wt.% PuO2 respectively. Attributing this degradation to Pu only implies that stoichiometric heterogeneous MOX can be obtained, while we show that any heterogeneity in the plutonium distribution in the sample introduces a variation in the local stoichiometry which in turn has a strong impact on the thermal conductivity. A model quantifying this effect is obtained and a new set of experimental results for homogeneous and heterogeneous MOX fuels is presented and used to validate the proposed model. In irradiated fuels, this effect is predicted to disappear early during irradiation. The 3, 6 and 10 wt.% Pu samples have a similar thermal conductivity. Comparison of the results for this homogeneous microstructure with MIMAS (heterogeneous) fuel of the same composition showed no difference for the Pu contents of 3, 5.9, 6, 7.87 and 10 wt.%. A small increase of the thermal conductivity was obtained for 15 wt.% Pu. This increase is of about 6% when compared to the average of the values obtained for 3, 6 and 10 wt.% Pu. For comparison purposes, Duriez also measured the thermal conductivity of FBR MOX with 21.4 wt.% Pu with O/M = 1.982 and a density close to 95% TD and found a value in good agreement with the estimation obtained using the formula of Philipponneau [8] for FBR MOX, and significantly lower than his results corresponding to the range 3-15 wt.% Pu. This difference in thermal conductivity is of about 20%, i.e. higher than the measurement uncertainties.Thus, a significant difference was observed between FBR and PWR MOX fuels, but was not explained. This difference was observed for hypostoichiometric fuels, that correspond to the condition used for irradiation. However, if these two formulas are evaluated for O/M = 2.000, the difference between the predictions is negligible (Fig. 1). The difference becomes significant for non-stoichiometric fuels, as shown for O/M = 1.975 in Fig. 1. The microstructure of the FBR fuel with 21.4 wt.% Pu was not described in the paper of Duriez. Taking into account the rigorous experimental methodology used by Duriez (characterisation of the stoichiometry), a possible explanation is an interaction between the plutonium distribution and the stoichiometry. Another parameter having a strong impact on the conductivity is the porosity correction used to obtain the values for 95% TD. This correction is small in the work of Duriez as the samples density is very close to 95% TD. This was also the case for the samples selected by Philipponneau in order to obtain his recommendation. An effect due to differences in the pores shape can also be excluded, as the results are identical for stoichiometric fuels (Fig. 1). Usually the apparent stoichiometry is obtained by heat treatments and checked before and after the measurements, either by XRD or thermogravimetry. However, for non-perfectly homogeneous samples, the gradients in the plutonium distribution induce a non-uniform oxygen distribution, which is difficult to characterise experimentally. It has been proposed by Baron that the deviation from stoichiometry is the main cause for the differences observed between fresh UO2 and MOX [14,15], this effect is quantified in the next section. In the first model ("Model 1"), the effect of Pu is neglected over the entire relevant Pu compositions range (up to 24 wt.% PuO2), and a correlation obtained for non-stoichiometric homogeneous (U,Pu)O2 is used. In the second model ("Model 2", the effect of Pu is supposed to be present at all compositions, with the stoichiometry effect. The thermal conductivity is described by the correlations of Fink [16] for the UO2 matrix, Duriez at low PuO2 contents (coating phase) and of Philipponneau at high PuO2 contents (agglomerates). For the first model, applying a correlation for non-stoichiometric UO2 would be relevant, but such a correlation does not exist for physical reasons in the hypostoichiometric domain. A correlation for homogeneous (U,Pu)O2+x has to be obtained in order to predict the thermal conductivity of heterogeneous MOX fuel, supposing that the effect of Pu can be neglected, i.e. supposing that the thermal conductivities of homogeneous (U,Pu)O2 and UO2 are equal both for stoichiometric and non-stoichiometric fuels. Such a correlation has to be obtained considering reliable data for stoichiometric UO2 and stoichiometry dependence. Different correlations for non-stoichiometric fuels were reviewed [2,8,12,13,15,35,36]. The correlation of Martin [36], available for hyperstoichiometric UO2, was evaluated in the hypostoichiometric domain and the predictions were found to give a stoichiometry dependence very similar to a correlation already proposed [15]. Investigations by Molecular Dynamics [37] have confirmed the almost symmetric effect of the hypo- and hyper-stoichiometry in UO2. We therefore use the correlation of Martin, with however a correction, as for stoichiometric fuels it over predicts the conductivity of stoichiometric UO2 at high temperatures, when compared to the recommendation of Fink [16] (Fig. 4). Analysis has shown that this over-prediction was due to the high temperature term in the correlation of Martin, and that, if this term is removed, the predictions of Martin and Fink were identical for stoichiometric fuels in the temperature range 500-1500 K. The correlation proposed for homogeneous MOX is therefore given by the following equation. k=(0.035 The series and parallel bounds (Eq. (2)) were calculated using the thermal conductivity values given by Eq. (5) for the heterogeneous MOX constituents and the maximum difference between these two bounds is 2% over the considered temperature range. The predictions obtained with the equations of Maxwell-Eucken (Eq. (3)) and Bergman (Eq. (4)) are equal and are in the interval between the series and parallel bounds. This result shows that the use of a sophisticated analytical or numerical model to predict the thermal conductivity is not justified [38]. The model of Maxwell-Eucken [31] was therefore chosen to predict the equivalent thermal conductivity of the heterogeneous MOX.The equivalent thermal conductivity of the stoichiometric heterogeneous MOX with an average PuO2 content of 7.2 wt.% (constituted by a stoichiometric UO2 matrix containing 15 vol.% of (U0.76Pu0.24)O1.975 agglomerates and 55 vol.% of a coating phase of (U0.94Pu0.06)O1.995) was calculated. The results show that the apparent thermal conductivity of the heterogeneous MOX, calculated using homogeneous MOX data (Eq. (5)) with O/M = 2.000, 1.995 and 1.975 (labeled Model 1 in Fig. 4) is not significantly different from the values measured by Duriez. The latter values are also very similar to the thermal conductivity of homogeneous MOX with O/M = 1.995. This simple model shows that the stoichiometry effect is sufficient to explain the lower thermal conductivity of LWR MOX fuel as compared to UO2. The advantage of this simple model is its consistency, as the calculations for the heterogeneous MOX are based on a unique formula for non-stoichiometric homogeneous (U,Pu)O2.In the second model, the effect of the plutonium is taken into account for the coating phase and for the Pu-rich agglomerates. The thermal conductivity is described by the correlations of Fink [16] for UO2.000, of Duriez et al. [2] for (U0.94Pu0.06)O1.995 (coating phase with low PuO2 content) and of Philipponneau [8] for (U0.76Pu0.24)O1.975 (Pu-rich agglomerates with high PuO2 content). The results (labeled Model 2 in Fig. 5) show that the calculated thermal conductivity of the heterogeneous 'stoichiometric' MOX is lower than UO2 and also lower than for stoichiometric MOX as given by Duriez. Therefore taking into account both the heterogeneity in the oxygen distribution and the Pu content leads to an underprediction of the thermal conductivity of heterogeneous MOX. A possible cause for the lower thermal conductivity of unirradiated heterogeneous MOX is therefore the intrinsic fluctuations of the local stoichiometry and only to a lesser extent the perturbation of the heat transfer due to the substitution of the U by Pu atoms in the crystal lattice. This interpretation was already proposed by Baron [14,15]. This assumption is acceptable if the size of the heterogeneities is much smaller that the thickness of the sample. A theoretical criterion for the impact of these parameters, initially proposed by Kerrish [40], was checked experimentally by Lee and Taylor [41] and was found to be too restrictive. The conclusions resulting from the investigations of Lee are that for diffusivity ratios between 1 and 3.5 and volume fractions up to 30%, a ratio of 5 between the sample thickness and inclusions diameter is sufficient. Our heterogeneous samples fulfill this criterion, taking into account that the thermal diffusivity ratio is close to 1 in MOX, that the volume fraction of Pu rich agglomerates is under 30%, and that the agglomerates have a diameter of less than 200 μm compared to the sample (disc) thickness of 1 mm. The most severe requirement that one could use to define a medium behaving like a homogeneous material is that the heat transfer is not affected by the heterogeneities. This is the case for instance if we have a heterogeneous material where the two constituents have equal thermal diffusivity and no thermal resistance is present at the interfaces. This requirement is very close to be perfectly verified for the heterogeneous MOX, as UO2 and (U,Pu)O2 have very close values of the thermal diffusivity. An effect of the sample heterogeneity can also be excluded from the point of view of the location where the thermograms are recorded: the temperature transients on the rear face of the samples are measured with a pyrometer and the system is provided with a lens assembly which enables a 1 mm diameter spot of the sample surface to be focused onto the signal collecting fibre. The thermograms are therefore averaged over a 1 mm diameter surface, which is much larger than the size of the heterogeneities (Pu rich agglomerates with a size of less than 200 μm).The impact of sample thickness on the measured thermal diffusivity was experimentally investigated for the MIMAS MOX with 7.0 wt.% Pu. For this purpose, discs of 0.5, 1, 2, and 3 mm thickness were cut and the thermal diffusivity was measured. The same investigation was done for standard UO2, in order to verify the accuracy of the inverse technique used for the identification of the thermal diffusivity from the thermograms. The inverse technique [39] explicitly takes into account the sample thickness in the calculation of the heat losses. The results for UO2 (Fig. 6) show that the measured thermal diffusivity does not depend on sample thickness, and is in good agreement with the recommendation of Fink [16]. The results for the heterogeneous MOX (Fig. 7) also show no dependence on sample thickness.

Efficient uranium capture by polysulfide/layered double hydroxide composites.

PubMed

Ma, Shulan; Huang, Lu; Ma, Lijiao; Shim, Yurina; Islam, Saiful M; Wang, Pengli; Zhao, Li-Dong; Wang, Shichao; Sun, Genban; Yang, Xiaojing; Kanatzidis, Mercouri G

2015-03-18

There is a need to develop highly selective and efficient materials for capturing uranium (normally as UO2(2+)) from nuclear waste and from seawater. We demonstrate the promising adsorption performance of S(x)-LDH composites (LDH is Mg/Al layered double hydroxide, [S(x)](2-) is polysulfide with x = 2, 4) for uranyl ions from a variety of aqueous solutions including seawater. We report high removal capacities (q(m) = 330 mg/g), large K(d)(U) values (10(4)-10(6) mL/g at 1-300 ppm U concentration), and high % removals (>95% at 1-100 ppm, or ∼80% for ppb level seawater) for UO2(2+) species. The S(x)-LDHs are exceptionally efficient for selectively and rapidly capturing UO2(2+) both at high (ppm) and trace (ppb) quantities from the U-containing water including seawater. The maximum adsorption coeffcient value K(d)(U) of 3.4 × 10(6) mL/g (using a V/m ratio of 1000 mL/g) observed is among the highest reported for U adsorbents. In the presence of very high concentrations of competitive ions such as Ca(2+)/Na(+), S(x)-LDH exhibits superior selectivity for UO2(2+), over previously reported sorbents. Under low U concentrations, (S4)(2-) coordinates to UO2(2+) forming anionic complexes retaining in the LDH gallery. At high U concentrations, (S4)(2-) binds to UO2(2+) to generate neutral UO2S4 salts outside the gallery, with NO3(-) entering the interlayer to form NO3-LDH. In the presence of high Cl(-) concentration, Cl(-) preferentially replaces [S4](2-) and intercalates into LDH. Detailed comparison of U removal efficiency of S(x)-LDH with various known sorbents is reported. The excellent uranium adsorption ability along with the environmentally safe, low-cost constituents points to the high potential of S(x)-LDH materials for selective uranium capture.

Thermodynamics of fission products in dispersion fuel designs - first principles modeling of defect behavior in bulk and at interfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiang-yand; Uberuaga, Blas P; Nerikar, Pankaj

2009-01-01

Density functional theory (DFT) calculations of fission product (Xe, Sr, and Cs) incorporation and segregation in alkaline earth metal oxides, HfO{sub 2} and UO{sub 2} oxides, and the MgO/(U, Hf, Ce)O{sub 2} interfaces have been carried out. In the case of UO{sub 2}, the calculations were performed using spin polarization and with a Hubbard U term characterizing the on-sit Coulomb repulsion between the localized 5f electrons. The fission product solution energies in bulk UO{sub 2{+-}x} have been calculated as a function of non-stoichiometry x, and were compared to that in MgO. These calculations demonstrate that the fission product incorporation energiesmore » in MgO are higher than in HfO{sub 2}. However, this trend is reversed or reduced for alkaline earth oxides with larger cation sizes. The solution energies of fission products in MgO are substantially higher than in UO{sub 2{+-}x}, except for the case of Sr in the hypostoichiometric case. Due to size effects, the thermodynamic driving force of segregation for Xe and Cs from bulk MgO to the MgO/fluorite interface is strong. However, this driving force is relatively weak for Sr.« less

Uranium dioxide fuel cladding strain investigation with the use of CYGRO-2 computer program

NASA Technical Reports Server (NTRS)

Smith, J. R.

1973-01-01

Previously irradiated UO2 thermionic fuel pins in which gross fuel-cladding strain occurred were modeled with the use of a computer program to define controlling parameters which may contribute to cladding strain. The computed strain was compared with measured strain, and the computer input data were studied in an attempt to get agreement with measured strain. Because of the limitations of the program and uncertainties in input data, good agreement with measured cladding strain was not attained. A discussion of these limitations is presented.

Uncertainty and sensitivity analysis of fission gas behavior in engineering-scale fuel modeling

DOE PAGES

Pastore, Giovanni; Swiler, L. P.; Hales, Jason D.; ...

2014-10-12

The role of uncertainties in fission gas behavior calculations as part of engineering-scale nuclear fuel modeling is investigated using the BISON fuel performance code and a recently implemented physics-based model for the coupled fission gas release and swelling. Through the integration of BISON with the DAKOTA software, a sensitivity analysis of the results to selected model parameters is carried out based on UO2 single-pellet simulations covering different power regimes. The parameters are varied within ranges representative of the relative uncertainties and consistent with the information from the open literature. The study leads to an initial quantitative assessment of the uncertaintymore » in fission gas behavior modeling with the parameter characterization presently available. Also, the relative importance of the single parameters is evaluated. Moreover, a sensitivity analysis is carried out based on simulations of a fuel rod irradiation experiment, pointing out a significant impact of the considered uncertainties on the calculated fission gas release and cladding diametral strain. The results of the study indicate that the commonly accepted deviation between calculated and measured fission gas release by a factor of 2 approximately corresponds to the inherent modeling uncertainty at high fission gas release. Nevertheless, higher deviations may be expected for values around 10% and lower. Implications are discussed in terms of directions of research for the improved modeling of fission gas behavior for engineering purposes.« less

Pulsed activation measurement of the Doppler effect of uranium-238 over the temperature range 300 to 3115 K

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bhattacharyya, S.K.; Russell, G.J.; Foell, W.K.

The Doppler effect for /sup 235/U-enriched UO/sub 2/ fuel pellets has been measured by the Pulsed Activation Doppler (PAD) technique in a TRIGA reactor. A combination of static electrical preheating and pulsed fission heating during irradiation was used to perform the measurements at temperatures extending from 300 K to the melting point of UO/sub 2/ (3115 K). The /sup 235/U enrichment in the experimental samples investigated ranged from 0.22 to 12 percent by weight. Measurements were made at under partially molten conditions of UO/sub 2/. Two sizes of pellets were used, with nominal surface-to-mass ratio values of 0.63 and 1.08more » cm/sup 2//g, respectively. The experimentally determined values of the Doppler ratio were in good agreement with resonance integral ratios determined from GAROL calculations and extrapolations of the low-temperature Hellstrand correlation.« less

Dynamics and Tolerance of Superionics in Extreme Environment

NASA Astrophysics Data System (ADS)

Annamareddy, Venkata Ajay Krishna Choudary

Superionic conductors are multi-component solid-state systems in which one sub-lattice exhibits exceptional ionic conductivity, which is comparable to molten state; among other things, the high ionic conductivity facilitates their use as solid-state electrolytes. Uranium di-oxide (UO 2)--the material of choice for fuel in most nuclear reactors--also shows superionic behavior, although very little is understood currently on the fast ion transport in UO2, and its implication. This dissertation aims to provide a better understanding of the dynamical characteristics of superionic conductors under both equilibrium and non-equilibrium thermodynamic conditions. In the first part, the emphasis is on equilibrium fluctuations and associated properties of Type II superionic conductors. Using atomistic simulations as well as available neutron and x-ray scattering data, the order-disorder transition or onset of superionic state for Type II conductors at a certain characteristic temperature (Talpha) is first revealed. Talpha marks a structural and kinetic crossover from a crystalline state to a semi-ordered state and is clearly different from the well-known thermodynamic superionic transition (T lambda). Though not favored by entropic forces, collective and cooperative dynamical effects, reminiscent of glassy states, are manifested in the temperature range spanned by Talpha and T lambda. Using atomistic simulations, dynamical heterogeneity (DH)--presence of clustered mobile and immobile regions in a static-homogeneous system--a ubiquitous feature of supercooled liquids and glassy states, is shown to germinate at Talpha. Using reliable metrics, the DH is shown to strengthen with increasing temperature, peak at an intermediate temperature between Talpha and Tlambda , and then recede. This manifestation of DH in superionics markedly differs from that in supercooled liquids through its initial growth against the destabilizing entropic barriers. Atomistic simulations further show that DH in superionics arises from facilitated dynamics, or the phenomenon of dynamic facilitation (DF). Using mobility transfer function, which gives the probability of a neighbor of a mobile ion becoming mobile relative to that of a random ion becoming mobile, it is shown that mobility propagates continuously to the neighboring ions with the strength of the DF increasing at the order-disorder temperature ( Talpha), exhibiting a maximum at an intermediate temperature, and then decreasing as the temperature approaches T lambda. This waxing and waning behavior with temperature is nearly identical to the variation of DH. Thus the close correspondence between DH and DF strongly indicates that DF underpins the heterogeneous dynamics in Type II superionic conductors. In a dynamically facilitated system, a jammed region can become unjammed only if it is physically adjacent to a mobile region. Remarkably, a string-like displacement of ions, the quintessential mode of particle mobility in jammed systems, is shown to operate in Type II superionics as well. The probability distribution of the length of the string is shown to vary exponentially, which is identical to that observed in supercooled and jammed states. Thus the demonstration of DH, DF and string-like cooperative ionic displacements in superionics that closely parallel the dynamic characteristics of supercooled liquids and glassy states, significantly augments the already existing but scant list of phenomenological similarities between these two distinct types of materials. The second part of this dissertation deals with non-equilibrium displacement-cascade simulations of UO2 that is used as a nuclear fuel. UO2 is known to resist amorphization even when subjected to intense nuclear radiations; analysis based on structure and energy does explain this behavior from a thermodynamic perspective. Radiation is inherently dynamic (non-equilibrium), and thus it is pertinent to understand the dynamics of the displaced ions during the annealing process. In this dissertation, the mechanism of dynamic recovery following a radiation knock at the atomistic level is investigated. It is shown that oxygen ions following a radiation perturbation exhibit correlated motion, which is similar to that in high temperature superionic state. Quite remarkably, the displaced oxygen ions also undergo fast recovery to their native lattice sites through collective string-like displacements that show an exponential distribution. Thus the superionic characteristics of UO2 under equilibrium conditions are also instrumental in fast defect recovery following a radiation perturbation.

New insight into UO 2F 2 particulate structure by micro-Raman spectroscopy

DOE PAGES

Stefaniak, Elzbieta A.; Darchuk, Larysa; Sapundjiev, Danislav; ...

2013-02-19

Uranyl fluoride particles produced via hydrolysis of uranium hexafluoride have been deposited on different substrates: polished graphite disks, silver foil, stainless steel and gold-coated silicon wafer, and measured with micro-Raman spectroscopy (MRS). All three metallic substrates enhanced the Raman signal delivered by UO 2F 2 in comparison to graphite. The fundamental stretching of the U–O band appeared at 867 cm –1 in case of the graphite substrate, while in case of the others it was shifted to lower frequencies (down to 839 cm –1). All applied metallic substrates showed the expected effect of Raman signal enhancement; however the gold layermore » appeared to be most effective. Lastly, application of new substrates provides more information on the molecular structure of uranyl fluoride precipitation, which is interesting for nuclear safeguards and nuclear environmental analysis.« less

NMR shielding calculations across the periodic table: diamagnetic uranium compounds. 2. Ligand and metal NMR.

PubMed

Schreckenbach, Georg

2002-12-16

In this and a previous article (J. Phys. Chem. A 2000, 104, 8244), the range of application for relativistic density functional theory (DFT) is extended to the calculation of nuclear magnetic resonance (NMR) shieldings and chemical shifts in diamagnetic actinide compounds. Two relativistic DFT methods are used, ZORA ("zeroth-order regular approximation") and the quasirelativistic (QR) method. In the given second paper, NMR shieldings and chemical shifts are calculated and discussed for a wide range of compounds. The molecules studied comprise uranyl complexes, [UO(2)L(n)](+/-)(q); UF(6); inorganic UF(6) derivatives, UF(6-n)Cl(n), n = 0-6; and organometallic UF(6) derivatives, UF(6-n)(OCH(3))(n), n = 0-5. Uranyl complexes include [UO(2)F(4)](2-), [UO(2)Cl(4)](2-), [UO(2)(OH)(4)](2-), [UO(2)(CO(3))(3)](4-), and [UO(2)(H(2)O)(5)](2+). For the ligand NMR, moderate (e.g., (19)F NMR chemical shifts in UF(6-n)Cl(n)) to excellent agreement [e.g., (19)F chemical shift tensor in UF(6) or (1)H NMR in UF(6-n)(OCH(3))(n)] has been found between theory and experiment. The methods have been used to calculate the experimentally unknown (235)U NMR chemical shifts. A large chemical shift range of at least 21,000 ppm has been predicted for the (235)U nucleus. ZORA spin-orbit appears to be the most accurate method for predicting actinide metal chemical shifts. Trends in the (235)U NMR chemical shifts of UF(6-n)L(n) molecules are analyzed and explained in terms of the calculated electronic structure. It is argued that the energy separation and interaction between occupied and virtual orbitals with f-character are the determining factors.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rabin, S.A.; Martin, M.M.; Lotts, A.L.

The fabricability of dispersion fuels using UO/sub 2/ or UC as the dispersoid and uranium combined with 10 to 15 wt% Mo as the matrix was investigated. Cores containing l7.8 wt% UO/sub 2/ dispersed in U-- 15 wt.% Mo were successfully fabricated to about 80% of theoretical density by cold pressing at 50 tsi, sintering at 1100 deg C, and cold coining at 50 tsi. Comparable results were obtained with UC as the dispersoid. Core fabrication results varied greatly with the type of matrix powder used. Occluded gases, pour density, and surface cleanliness bore important relations to the fabrication behaviormore » of powders. Suitable pressing and sintering results were obtained with prealloyed, calcium-reduced U--Mo powder and with molybdenum and calcium-reduced uranium as elemental powders. Shotted prealloyed powders were difficult to press and sinter, as were elemental and prealloyed powders prepared by hydriding. The cores containing UO/sub 2/ were picture-frame, hot-roll-clad as miniature plates. Molybdenum, Fansteel 82, and Zr--3 wt% Al were investigated as cladding materials. While each bonded well to itself, only the molybdenum-clad core, rolled at 1150 deg C to 10/1 reduction, resulted in dispersions free of ruptures and UO/sub 2/ fragmentation and in strong bonding to the core, evaluated by metallography, mechanical peel, and thermal shock tests. The matrix phase was homogeneous, but the UO/sub 2/ dispersoid showed stringering characteristic of cores worked by hot rolling. Core densities as high as 99% of theoretical were obtained. (auth)« less

Critical review of carbon monoxide pressure measurements in the uranium carbon oxygen ternary system

NASA Astrophysics Data System (ADS)

Gossé, S.; Guéneau, C.; Chatillon, C.; Chatain, S.

2006-06-01

For high temperature reactors (HTR), the high level of fuel operating temperature in normal and accidental conditions requires to predict the possible chemical interactions between the fuel components. Among the concerns of the TRISO fuel particle thermomechanical behavior, it is necessary to better understand the carbon monoxide formation due to chemical interactions at the UO2 kernel and graphite buffer's interface. In a first step, the thermodynamic properties of the U-C-O system have to be assessed. The experimental data from literature on the equilibrium CO gas pressure measurements in the UO2-UC2-C ternary section of the U-C-O system are critically reviewed. Discrepancies between the different determinations can be explained - (i) by the different gaseous flow regimes in the experiments and - (ii) by the location of the measuring pressure gauge away from the reaction site. Experimental values are corrected - (i) from the gaseous flow type (molecular, transition or viscous) defined by the Knudsen number and - (ii) from the thermomolecular effect due to the temperature gradient inside the experimental vessels. Taking account of the selected and corrected values improves greatly the consistency of the original set of measurements.

Grain Size and Phase Purity Characterization of U 3Si 2 Pellet Fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoggan, Rita E.; Tolman, Kevin R.; Cappia, Fabiola

Characterization of U 3Si 2 fresh fuel pellets is important for quality assurance and validation of the finished product. Grain size measurement methods, phase identification methods using scanning electron microscopes equipped with energy dispersive spectroscopy and x-ray diffraction, and phase quantification methods via image analysis have been developed and implemented on U 3Si 2 pellet samples. A wide variety of samples have been characterized including representative pellets from an initial irradiation experiment, and samples produced using optimized methods to enhance phase purity from an extended fabrication effort. The average grain size for initial pellets was between 16 and 18 µm.more » The typical average grain size for pellets from the extended fabrication was between 20 and 30 µm with some samples exhibiting irregular grain growth. Pellets from the latter half of extended fabrication had a bimodal grain size distribution consisting of coarsened grains (>80 µm) surrounded by the typical (20-30 µm) grain structure around the surface. Phases identified in initial uranium silicide pellets included: U 3Si 2 as the main phase composing about 80 vol. %, Si rich phases (USi and U 5Si 4) composing about 13 vol. %, and UO 2 composing about 5 vol. %. Initial batches from the extended U 3Si 2 pellet fabrication had similar phases and phase quantities. The latter half of the extended fabrication pellet batches did not contain Si rich phases, and had between 1-5% UO 2: achieving U 3Si 2 phase purity between 95 vol. % and 98 vol. % U 3Si 2. The amount of UO 2 in sintered U 3Si 2 pellets is correlated to the length of time between U 3Si 2 powder fabrication and pellet formation. These measurements provide information necessary to optimize fabrication efforts and a baseline for future work on this fuel compound.« less

Parametric Evaluation of SiC/SiC Composite Cladding with UO2 Fuel for LWR Applications: Fuel Rod Interactions and Impact of Nonuniform Power Profile in Fuel Rod

NASA Astrophysics Data System (ADS)

Singh, G.; Sweet, R.; Brown, N. R.; Wirth, B. D.; Katoh, Y.; Terrani, K.

2018-02-01

SiC/SiC composites are candidates for accident tolerant fuel cladding in light water reactors. In the extreme nuclear reactor environment, SiC-based fuel cladding will be exposed to neutron damage, significant heat flux, and a corrosive environment. To ensure reliable and safe operation of accident tolerant fuel cladding concepts such as SiC-based materials, it is important to assess thermo-mechanical performance under in-reactor conditions including irradiation and realistic temperature distributions. The effect of non-uniform dimensional changes caused by neutron irradiation with spatially varying temperatures, along with the closing of the fuel-cladding gap, on the stress development in the cladding over the course of irradiation were evaluated. The effect of non-uniform circumferential power profile in the fuel rod on the mechanical performance of the cladding is also evaluated. These analyses have been performed using the BISON fuel performance modeling code and the commercial finite element analysis code Abaqus. A constitutive model is constructed and solved numerically to predict the stress distribution in the cladding under normal operating conditions. The dependence of dimensions and thermophysical properties on irradiation dose and temperature has been incorporated into the models. Initial scoping results from parametric analyses provide time varying stress distributions in the cladding as well as the interaction of fuel rod with the cladding under different conditions of initial fuel rod-cladding gap and linear heat rate. It is found that a non-uniform circumferential power profile in the fuel rod may cause significant lateral bowing in the cladding, and motivates further analysis and evaluation.

In-pile and out-of-pile testing of a molybdenum-uranium dioxide cermet fueled themionic diode

NASA Technical Reports Server (NTRS)

Diianni, D. C.

1972-01-01

The behavior of Mo-UO2 cermet fuel in a diode for thermionic reactor application was studied. The diode had a Mo-0.5 Ti emitter and niobium collector. Output power ranged from 1.4 to 2.8 W/cm squared at emitter and collector temperatures of 1500 deg and 540 C. Thermionic performance was stable within the limits of the instrumentation sensitivity. Through 1000 hours of in-pile operation the emitter was dimensionally stable. However, some fission gases (15 percent) leaked through an inner clad imperfection that occurred during fuel fabrication.

Neutronic performance of high-density LEU fuels in water-moderated and water-reflected research reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bretscher, M.M.; Matos, J.E.

At the Reduced Enrichment for Research and Test Reactors (RERTR) meeting in September 1994, Durand reported that the maximum uranium loading attainable with U{sub 3}Si{sub 2} fuel is about 6.0 g U/cm{sup 3}. The French Commissariat a l`Energie Atomique (CEA) plan to perform irradiation tests with 5 plates at this loading. Compagnie pour L`Etude et La Realisation de Combustibles Atomiques (CERCA) has also fabricated a few uranium nitride (UN) plates with a uranium density in the fuel meat of 7.0 g/cm{sup 3} and found that UN is compatible with the aluminum matrix at temperatures below 500 C. High density dispersionmore » fuels proposed for development include U-Zr(4 wt%)-Nb(2 wt%), U-Mo(5 wt%), and U-Mo(9 wt%). The purpose of this note is to examine the relative neutronic behavior of these high density fuels in a typical light water-reflected and water-moderated MTR-type research reactor. The results show that a dispersion of the U-Zr-Nb alloy has the most favorable neutronic properties and offers the potential for uranium densities greater than 8.0 g/cm{sup 3}. On the other hand, UN is the least reactive fuel because of the relatively large {sup 14}N(n,p) cross section. For a fixed value of k{sub eff}, the required {sup 235}U loading per fuel element is least for the U-Zr-Nb fuel and steadily increases for the U-Mo(5%), U-Mo(9%), and UN fuels. Because of volume fraction limitations, the UO{sub 2} dispersions are only useful for uranium densities below 5.0 g/cm{sup 3}. In this density range, however, UO{sub 2} is more reactive than U{sub 3}Si{sub 2}.« less

Material distribution in light water reactor-type bundles tested under severe accident conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Noack, V.; Hagen, S.J.L.; Hofmann, P.

1997-02-01

Severe fuel damage experiments simulating small-break loss-of-coolant accidents have been carried out in the CORA out-of-pile test facility at Forschungszentrum Karlsruhe. Rod bundles with electrically heated fuel rod simulators containing annular UO{sub 2} pellets, UO{sub 2} full pellet rods, and absorber rods of two kinds (Ag/In/Cd to represent pressurized water reactor conditions and B{sub 4}C to represent boiling water reactor and VVER-1000 fuel elements) were subjected to temperature transients up to 2,300 K. A special method was applied to determine the axial mass distribution of bundle materials. The low-temperature melt formation by various interactions between zirconium and components of absorbermore » and spacer grids strongly influences the bundle degradation and material relocation. Absorber materials can separate from the fuel by a noncoherent relocation of the materials at different temperatures. The distributions of solidified materials in the different test bundles show a clear dependence on the axial temperature profile. Coolant channel blockages are observed mainly at the lower end of the bundle, i.e., near the lowest elevation at which an oxidation excursion resulting from the highly exothermic zirconium-steam reaction had been experienced. This elevation corresponds with a steep axial temperature gradient in the maximum temperature attained. Oxide layers on Zircaloy result in reduced melt formation.« less

Novel fabrication of silicon carbide based ceramics for nuclear applications

NASA Astrophysics Data System (ADS)

Singh, Abhishek Kumar

Advances in nuclear reactor technology and the use of gas-cooled fast reactors require the development of new materials that can operate at the higher temperatures expected in these systems. These materials include refractory alloys based on Nb, Zr, Ta, Mo, W, and Re; ceramics and composites such as SiC--SiCf; carbon--carbon composites; and advanced coatings. Besides the ability to handle higher expected temperatures, effective heat transfer between reactor components is necessary for improved efficiency. Improving thermal conductivity of the fuel can lower the center-line temperature and, thereby, enhance power production capabilities and reduce the risk of premature fuel pellet failure. Crystalline silicon carbide has superior characteristics as a structural material from the viewpoint of its thermal and mechanical properties, thermal shock resistance, chemical stability, and low radioactivation. Therefore, there have been many efforts to develop SiC based composites in various forms for use in advanced energy systems. In recent years, with the development of high yield preceramic precursors, the polymer infiltration and pyrolysis (PIP) method has aroused interest for the fabrication of ceramic based materials, for various applications ranging from disc brakes to nuclear reactor fuels. The pyrolysis of preceramic polymers allow new types of ceramic materials to be processed at relatively low temperatures. The raw materials are element-organic polymers whose composition and architecture can be tailored and varied. The primary focus of this study is to use a pyrolysis based process to fabricate a host of novel silicon carbide-metal carbide or oxide composites, and to synthesize new materials based on mixed-metal silicocarbides that cannot be processed using conventional techniques. Allylhydridopolycarbosilane (AHPCS), which is an organometal polymer, was used as the precursor for silicon carbide. Inert gas pyrolysis of AHPCS produces near-stoichiometric amorphous silicon carbide (a-SiC) at 900--1150 °C. Results indicated that this processing technique can be effectively used to fabricate various silicon carbide composites with UC or UO2 as the nuclear component.

Update of the α - n Yields for Reactor Fuel Materials for the Interest of Nuclear Safeguards

NASA Astrophysics Data System (ADS)

Simakov, S. P.; van den Berg, Q. Y.

2017-01-01

The neutron yields caused by spontaneous α-decay of actinides and subsequent (α,xn) reactions were re-evaluated for the reactor fuel materials UO2, UF6, PuO2 and PuF4. For this purpose, the most recent reference data for decay parameters, α-particle stopping powers and (α,xn) cross sections were collected, analysed and used in calculations. The input data and elaborated code were validated against available thick target neutron yields in pure and compound materials measured at accelerators or with radioactive sources. This paper provides the specific neutron yields and their uncertainties resultant from α-decay of actinides 241Am, 249Bk, 252Cf, 242,244Cm, 237Np, 238-242Pu, 232Th and 232-236,238U in oxide and fluoride compounds. The obtained results are an update of previous reference tables issued by the Los Alamos National Laboratory in 1991 which were used for the safeguarding of radioactive materials by passive non-destructive techniques. The comparison of the updated values with previous ones shows an agreement within one estimated uncertainty (≈ 10%) for oxides, and deviations of up to 50% for fluorides.

Overview of the U.S. DOE Accident Tolerant Fuel Development Program

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jon Carmack; Frank Goldner; Shannon M. Bragg-Sitton

2013-09-01

The United States Fuel Cycle Research and Development Advanced Fuels Campaign has been given the responsibility to conduct research and development on enhanced accident tolerant fuels with the goal of performing a lead test assembly or lead test rod irradiation in a commercial reactor by 2022. The Advanced Fuels Campaign has defined fuels with enhanced accident tolerance as those that, in comparison with the standard UO2-Zircaloy system currently used by the nuclear industry, can tolerate loss of active cooling in the reactor core for a considerably longer time period (depending on the LWR system and accident scenario) while maintaining ormore » improving the fuel performance during normal operations and operational transients, as well as design-basis and beyond design-basis events. This paper provides an overview of the FCRD Accident Tolerant Fuel program. The ATF attributes will be presented and discussed. Attributes identified as potentially important to enhance accident tolerance include reduced hydrogen generation (resulting from cladding oxidation), enhanced fission product retention under severe accident conditions, reduced cladding reaction with high-temperature steam, and improved fuel-cladding interaction for enhanced performance under extreme conditions. To demonstrate the enhanced accident tolerance of candidate fuel designs, metrics must be developed and evaluated using a combination of design features for a given LWR design, potential improvements to that design, and the design of an advanced fuel/cladding system. The aforementioned attributes provide qualitative guidance for parameters that will be considered for fuels with enhanced accident tolerance. It may be unnecessary to improve in all attributes and it is likely that some attributes or combination of attributes provide meaningful gains in accident tolerance, while others may provide only marginal benefits. Thus, an initial step in program implementation will be the development of quantitative metrics. A companion paper in these proceedings provides an update on the status of establishing these quantitative metrics for accident tolerant LWR fuel.1 The United States FCRD Advanced Fuels Campaign has embarked on an aggressive schedule for development of enhanced accident tolerant LWR fuels. The goal of developing such a fuel system that can be deployed in the U.S. LWR fleet in the next 10 to 20 years supports the sustainability of clean nuclear power generation in the United States.« less

Uranium nitride fuel fabrication for SP-100 reactors

NASA Technical Reports Server (NTRS)

Mason, Richard E.; Chidester, Kenneth M.; Hoth, Carl W.; Matthews, Bruce R.

1987-01-01

Fuel pins of uranium mononitride clad in Nb-1 percent Zr were fabricated for irradiation tests in EBR-II. Laboratory scale process parameters to synthesize UN powders and fabricate UN pellets were developed. Uranium mononitride was prepared by converting UO2 to UN. Fuel pellets were prepared by communition of UN briquettes, uniaxial pressing, and high temperature sintering. Techniques for machining, cleaning, and welding Nb-1 percent Zr cladding components were developed. End caps were electron beam welded to the tubing. Helium back-fill holes were sealed with a laser weld.

Uranium nitride fuel fabrication for SP-100 reactors

NASA Astrophysics Data System (ADS)

Mason, Richard E.; Chidester, Kenneth M.; Hoth, Carl W.; Matthews, Bruce R.

Fuel pins of uranium mononitride clad in Nb-1 percent Zr were fabricated for irradiation tests in EBR-II. Laboratory scale process parameters to synthesize UN powders and fabricate UN pellets were developed. Uranium mononitride was prepared by converting UO2 to UN. Fuel pellets were prepared by communition of UN briquettes, uniaxial pressing, and high temperature sintering. Techniques for machining, cleaning, and welding Nb-1 percent Zr cladding components were developed. End caps were electron beam welded to the tubing. Helium back-fill holes were sealed with a laser weld.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rothman, A.; Graczyk, D.; Chemical Sciences and Engineering Division

In the ammonium diuranate (ADU) process, UF{sub 6} is reacted with water, and the acidic solution of uranyl fluoride is treated with aqueous ammonia to precipitate ammonium polyuranate for subsequent reduction to UO{sub 2} and production of fuel pellets for commercial nuclear reactors. Our experiments simulated adding aqueous ammonia to the reaction products of UF{sub 6} and water in typical ADU processes. Chemical and X-ray diffraction analysis of products from the experiments are consistent with postulated chemical equilibria in which solids with structures close to that of ammonium polyuranate are formed from co-precipitation of the NH{sub 4}{sup +}(aq) cation withmore » (previously unreported) anions of the form UO{sub 2}F{sub 3-x}(OH){sub x}{sup -}(aq). More efficient separations of solid products were obtained at NH{sub 4}OH:UF{sub 6} ratios of 19 or greater, with x closer to the value of 3 for the hypothetical formation of pure ammonium polyuranate. Supplementary experiments in the current study and a previous study in our laboratory indicated that nominal uranium concentrations of 90 mg/l in the filtrate resulting from such separations could be reduced to microgram per liter levels by batch mixing a 1-to-2.5 aqueous diluate of the filtrate with the Diphonix{reg_sign} ion exchange resin. Our study further demonstrated that reaction of the purified NH{sub 4}OH-NH{sub 4}F diluate with aqueous Ca(OH){sub 2} at 80 to 90 C could produce essentially uranium-free CaF{sub 2} and an ammonia distillate, as useful waste-conversion end products from a modified ADU process.« less

Thermal and X-ray diffraction analysis studies during the decomposition of ammonium uranyl nitrate.

PubMed

Kim, B H; Lee, Y B; Prelas, M A; Ghosh, T K

Two types of ammonium uranyl nitrate (NH 4 ) 2 UO 2 (NO 3 ) 4 ·2H 2 O and NH 4 UO 2 (NO 3 ) 3 , were thermally decomposed and reduced in a TG-DTA unit in nitrogen, air, and hydrogen atmospheres. Various intermediate phases produced by the thermal decomposition and reduction process were investigated by an X-ray diffraction analysis and a TG/DTA analysis. Both (NH 4 ) 2 UO 2 (NO 3 ) 4 ·2H 2 O and NH 4 UO 2 (NO 3 ) 3 decomposed to amorphous UO 3 regardless of the atmosphere used. The amorphous UO 3 from (NH 4 ) 2 UO 2 (NO 3 ) 4 ·2H 2 O was crystallized to γ-UO 3 regardless of the atmosphere used without a change in weight. The amorphous UO 3 obtained from decomposition of NH 4 UO 2 (NO 3 ) 3 was crystallized to α-UO 3 under a nitrogen and air atmosphere, and to β-UO 3 under a hydrogen atmosphere without a change in weight. Under each atmosphere, the reaction paths of (NH 4 ) 2 UO 2 (NO 3 ) 4 ·2H 2 O and NH 4 UO 2 (NO 3 ) 3 were as follows: under a nitrogen atmosphere: (NH 4 ) 2 UO 2 (NO 3 ) 4 ·2H 2 O → (NH 4 ) 2 UO 2 (NO 3 ) 4 ·H 2 O → (NH 4 ) 2 UO 2 (NO 3 ) 4  → NH 4 UO 2 (NO 3 ) 3  → A-UO 3  → γ-UO 3  → U 3 O 8 , NH 4 UO 2 (NO 3 ) 3  → A-UO 3  → α-UO 3  → U 3 O 8 ; under an air atmosphere: (NH 4 ) 2 UO 2 (NO 3 ) 4 ·2H 2 O → (NH 4 ) 2 UO 2 (NO 3 ) 4 ·H 2 O → (NH 4 ) 2 UO 2 (NO 3 ) 4  → NH 4 UO 2 (NO 3 ) 3  → A-UO 3  → γ-UO 3  → U 3 O 8 , NH 4 UO 2 (NO 3 ) 3  → A-UO 3  → α-UO 3  → U 3 O 8 ; and under a hydrogen atmosphere: (NH 4 ) 2 UO 2 (NO 3 ) 4 ·2H 2 O → (NH 4 ) 2 UO 2 (NO 3 ) 4 ·H 2 O → (NH 4 ) 2 UO 2 (NO 3 ) 4  → NH 4 UO 2 (NO 3 ) 3  → A-UO 3  → γ-UO 3  → α-U 3 O 8  → UO 2 , NH 4 UO 2 (NO 3 ) 3  → A-UO 3  → β-UO 3  → α-U 3 O 8  → UO 2 .

DOE Office of Scientific and Technical Information (OSTI.GOV)

Campbell, Keri R.; Judge, Elizabeth J.; Barefield, James E.

We show the analysis of light water reactor simulated used nuclear fuel using laser-induced breakdown spectroscopy (LIBS) is explored using a simplified version of the main oxide phase. The main oxide phase consists of the actinides, lanthanides, and zirconium. The purpose of this study is to develop a rapid, quantitative technique for measuring zirconium in a uranium dioxide matrix without the need to dissolve the material. A second set of materials including cerium oxide is also analyzed to determine precision and limit of detection (LOD) using LIBS in a complex matrix. Two types of samples are used in this study:more » binary and ternary oxide pellets. The ternary oxide, (U,Zr,Ce)O 2 pellets used in this study are a simplified version the main oxide phase of used nuclear fuel. The binary oxides, (U,Ce)O 2 and (U,Zr)O 2 are also examined to determine spectral emission lines for Ce and Zr, potential spectral interferences with uranium and baseline LOD values for Ce and Zr in a UO 2 matrix. In the spectral range of 200 to 800 nm, 33 cerium lines and 25 zirconium lines were identified and shown to have linear correlation values (R 2) > 0.97 for both the binary and ternary oxides. The cerium LOD in the (U,Ce)O 2 matrix ranged from 0.34 to 1.08 wt% and 0.94 to 1.22 wt% in (U,Ce,Zr)O 2 for 33 of Ce emission lines. The zirconium limit of detection in the (U,Zr)O 2 matrix ranged from 0.84 to 1.15 wt% and 0.99 to 1.10 wt% in (U,Ce,Zr)O 2 for 25 Zr lines. Finally, the effect of multiple elements in the plasma and the impact on the LOD is discussed.« less

PEROXIDE-INHIBITED DECONTAMINATION SOLUTIONS FOR CARBON STEEL AND OTHER METALS IN THE GAS-COOLED REACTOR PROGRAM. Progress Report, November 1959-July 1962

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meservey, A.B.

1963-01-01

A search for solutions suitable for dissolving uranium dioxide powder or lumps and yet noncorrosive enough to be used for decontaminating the carbon steel EGCR charge and service machines resulted in the development of buffered oxalate solutions of controlled temperature and pH, with hydrogen peroxide added to act as corrosion inhibitor, UO/sub 2/ oxidizer, and decontamination aid. Hydrogen peroxide acts either as a corrosion promoter or inhibitor, depending on factors such as its concentration, the ratio to other ingredients, acidity, temperature, the presence of complexing agents, and the ferric ion content of the solution. In general, oxalate-peroxide solutions for fissionmore » product decontamination from metal surfaces were superior to more conventional decontaminating solutions and had attractively low corrosion rates on carbon steel (less than 0.01 mil/hr), Solution instability, initially a serious drawback, was largely overcome. Of nearly a hundred formulations studied, the one having the best combination of long life, low corrosivity, high solvency for UO/sub 2/, decontamination power, safety, and ease of waste disposal was an aqueous solution of 0.4M oxalic acid, 0.18M ammonium citrate, and 0.34M H/sub 2/O/sub 2/, adjusted to pH 4.00 with ammonium hydroxide and used at 85 to 95 deg C. Similar solutions at lower pH, with increased H/sub 2/O/sub 2/ concentration to maintain noncorrosiveness, were successful decontaminants at 60 deg C when contact times were increased to several hours. Contaminated stainless steels heated to 500 deg C in helium resisted decontamination in noncorrosive reagents. Oxalate-peroxide soluttons are currently recommended as UO/sub 2/ solvents and as general decontaminants for mild steel and aluminum surfaces in the GCR program, and for stainless steels which were not strongly heated while contaminated. These solutions may also find application in the decontamination of metals used in the aqueous reprocessing of radioactive nuclear fuels. (auth)« less

Iron-chrome-aluminum alloy cladding for increasing safety in nuclear power plants

NASA Astrophysics Data System (ADS)

Rebak, Raul B.

2017-12-01

After a tsunami caused plant black out at Fukushima, followed by hydrogen explosions, the US Department of Energy partnered with fuel vendors to study safer alternatives to the current UO2-zirconium alloy system. This accident tolerant fuel alternative should better tolerate loss of cooling in the core for a considerably longer time while maintaining or improving the fuel performance during normal operation conditions. General electric, Oak ridge national laboratory, and their partners are proposing to replace zirconium alloy cladding in current commercial light water power reactors with an iron-chromium-aluminum (FeCrAl) cladding such as APMT or C26M. Extensive testing and evaluation is being conducted to determine the suitability of FeCrAl under normal operation conditions and under severe accident conditions. Results show that FeCrAl has excellent corrosion resistance under normal operation conditions and FeCrAl is several orders of magnitude more resistant than zirconium alloys to degradation by superheated steam under accident conditions, generating less heat of oxidation and lower amount of combustible hydrogen gas. Higher neutron absorption and tritium release effects can be minimized by design changes. The implementation of FeCrAl cladding is a near term solution to enhance the safety of the current fleet of commercial light water power reactors.

Russian-US collaboration on implementation of the active well coincidence counter (AWCC)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mozhajev, V.; Pshakin, G.; Stewart, J.

The feasibility of using a standard AWCC at the Obninsk IPPE has been demonstrated through active measurements of single UO{sub 2} (36% enriched) disks and through passive measurements of plutonium metal disks used for simulating reactor cores. The role of the measurements is to verify passport values assigned to the disks by the facility, and thereby facilitate the mass accountability procedures developed for the very large inventory of fuel disks at the facility. The AWCC is a very flexible instrument for verification measurements of the large variety of nuclear material items at the Obninsk IPPE and other Russian facilities. Futuremore » work at the IPPE will include calibration and verification measurements for other materials, both in individual disks and in multi-disk storage tubes; it will also include training in the use of the AWCC.« less

A Jacobian-free Newton Krylov method for mortar-discretized thermomechanical contact problems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hansen, Glen, E-mail: Glen.Hansen@inl.gov

2011-07-20

Multibody contact problems are common within the field of multiphysics simulation. Applications involving thermomechanical contact scenarios are also quite prevalent. Such problems can be challenging to solve due to the likelihood of thermal expansion affecting contact geometry which, in turn, can change the thermal behavior of the components being analyzed. This paper explores a simple model of a light water reactor nuclear fuel rod, which consists of cylindrical pellets of uranium dioxide (UO{sub 2}) fuel sealed within a Zircalloy cladding tube. The tube is initially filled with helium gas, which fills the gap between the pellets and cladding tube. Themore » accurate modeling of heat transfer across the gap between fuel pellets and the protective cladding is essential to understanding fuel performance, including cladding stress and behavior under irradiated conditions, which are factors that affect the lifetime of the fuel. The thermomechanical contact approach developed here is based on the mortar finite element method, where Lagrange multipliers are used to enforce weak continuity constraints at participating interfaces. In this formulation, the heat equation couples to linear mechanics through a thermal expansion term. Lagrange multipliers are used to formulate the continuity constraints for both heat flux and interface traction at contact interfaces. The resulting system of nonlinear algebraic equations are cast in residual form for solution of the transient problem. A Jacobian-free Newton Krylov method is used to provide for fully-coupled solution of the coupled thermal contact and heat equations.« less

A Jacobian-Free Newton Krylov Method for Mortar-Discretized Thermomechanical Contact Problems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Glen Hansen

2011-07-01

Multibody contact problems are common within the field of multiphysics simulation. Applications involving thermomechanical contact scenarios are also quite prevalent. Such problems can be challenging to solve due to the likelihood of thermal expansion affecting contact geometry which, in turn, can change the thermal behavior of the components being analyzed. This paper explores a simple model of a light water reactor nuclear reactor fuel rod, which consists of cylindrical pellets of uranium dioxide (UO2) fuel sealed within a Zircalloy cladding tube. The tube is initially filled with helium gas, which fills the gap between the pellets and cladding tube. Themore » accurate modeling of heat transfer across the gap between fuel pellets and the protective cladding is essential to understanding fuel performance, including cladding stress and behavior under irradiated conditions, which are factors that affect the lifetime of the fuel. The thermomechanical contact approach developed here is based on the mortar finite element method, where Lagrange multipliers are used to enforce weak continuity constraints at participating interfaces. In this formulation, the heat equation couples to linear mechanics through a thermal expansion term. Lagrange multipliers are used to formulate the continuity constraints for both heat flux and interface traction at contact interfaces. The resulting system of nonlinear algebraic equations are cast in residual form for solution of the transient problem. A Jacobian-free Newton Krylov method is used to provide for fully-coupled solution of the coupled thermal contact and heat equations.« less

THE CALCULATION OF BURNABLE POISON CORRECTION FACTORS FOR PWR FRESH FUEL ACTIVE COLLAR MEASUREMENTS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Croft, Stephen; Favalli, Andrea; Swinhoe, Martyn T.

2012-06-19

Verification of commercial low enriched uranium light water reactor fuel takes place at the fuel fabrication facility as part of the overall international nuclear safeguards solution to the civilian use of nuclear technology. The fissile mass per unit length is determined nondestructively by active neutron coincidence counting using a neutron collar. A collar comprises four slabs of high density polyethylene that surround the assembly. Three of the slabs contain {sup 3}He filled proportional counters to detect time correlated fission neutrons induced by an AmLi source placed in the fourth slab. Historically, the response of a particular collar design to amore » particular fuel assembly type has been established by careful cross-calibration to experimental absolute calibrations. Traceability exists to sources and materials held at Los Alamos National Laboratory for over 35 years. This simple yet powerful approach has ensured consistency of application. Since the 1980's there has been a steady improvement in fuel performance. The trend has been to higher burn up. This requires the use of both higher initial enrichment and greater concentrations of burnable poisons. The original analytical relationships to correct for varying fuel composition are consequently being challenged because the experimental basis for them made use of fuels of lower enrichment and lower poison content than is in use today and is envisioned for use in the near term. Thus a reassessment of the correction factors is needed. Experimental reassessment is expensive and time consuming given the great variation between fuel assemblies in circulation. Fortunately current modeling methods enable relative response functions to be calculated with high accuracy. Hence modeling provides a more convenient and cost effective means to derive correction factors which are fit for purpose with confidence. In this work we use the Monte Carlo code MCNPX with neutron coincidence tallies to calculate the influence of Gd{sub 2}O{sub 3} burnable poison on the measurement of fresh pressurized water reactor fuel. To empirically determine the response function over the range of historical and future use we have considered enrichments up to 5 wt% {sup 235}U/{sup tot}U and Gd weight fractions of up to 10 % Gd/UO{sub 2}. Parameterized correction factors are presented.« less

ESCORT: A Pratt & Whitney nuclear thermal propulsion and power system for manned mars missions

NASA Astrophysics Data System (ADS)

Feller, Gerald J.; Joyner, Russell

1999-01-01

The purpose of this paper is to describe the conceptual design of an upgrade to the Pratt & Whitney ESCORT nuclear thermal rocket engine. The ESCORT is a bimodal engine capable of supporting a wide range of vehicle propulsive and electrical power requirements. The ESCORT engine is powered by a fast-spectrum beryllium-reflected CERMET-fueled nuclear reactor. In propulsive mode, the reactor is used to heat hot hydrogen to approximately 2700 K which is expanded through a converging/diverging nozzle to generate thrust. Heat pickup in the nozzle and the radial beryllium reflectors is used to drive the turbomachinery in the ESCORT expander cycle. In electrical mode, the reactor is used to heat a mixture of helium and xenon to drive a closed-loop Brayton cycle in order to generate electrical energy. This closed loop system has the additional function of a decay heat removal system after the propulsive mode operation is discontinued. The original ESCORT design was capable of delivering 4448.2 N (1000 lbf) of thrust at a vacuum impulse level of approximately 900 s. Design Reference Mission requirements (DRM) from NASA Johnson Space Center and NASA Lewis Research Center studies in 1997 and 1998 have detailed upgraded requirements for potential manned Mars missions. The current NASA DRM requires a nuclear thermal propulsion system capable of delivering total mission requirements of 200170 N (45000 lbf) thrust and 50 kWe of spacecraft electrical power. This is met assuming three engines capable of each delivering 66723 N (15000 lbf) of vacuum thrust and 25 kWe of electrical power. The individual engine requirements were developed assuming three out of three engine reliability for propulsion and two out of three engine reliability for spacecraft electrical power. The approximate target vacuum impulse is 925 s. The Pratt & Whitney ESCORT concept was upgraded to meet these requirements. The hexagonal prismatic fuel elements were modified to address the uprated power requirements while maintaining the peak fuel temperature below the 2880 K limit for W-UO2 CERMET fuels. A system integrated performance methodology was developed to assess the sensitivity to weight, thrust and impulse to the DRM requirements. Propellant tanks, shielding, and Brayton cycle power conversion unit requirements were included in this evaluation.

Estimation of weekly 99Mo production by AHR 200 kW

NASA Astrophysics Data System (ADS)

Siregar, I. H.; Suharyana; Khakim, A.; Siregar, D.; Frida, A. R.

2016-11-01

The estimation of weekly 99Mo production by AHR 200 kW fueled with Low Enriched Uranium Uranyl Nitrate solution has been simulated by using MCNPX computer code. We have employed the AHR design of Babcock & Wilcox Medical Isotope Production System with 9Be Reflector and Stainless steel vessel. We found that when the concentration of uranium in the fresh fuel was 108 gr U/L of UO2(NO3)2 fuel solution, the multiplication factor was 1.0517. The 99Mo concentration reached saturated at tenth day operation. The AHR can produce approximately 1.96×103 6-day-Ci weekly.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ikeuchi, Hirotomo; Yano, Kimihiko; Kaji, Naoya

For the decommissioning of the Fukushima-Daiichi Nuclear Power Station (1F), the characterization of fuel-debris in cores of Units 1-3 is necessary. In this study, typical phases of the in-vessel fuel-debris were estimated using a thermodynamic equilibrium (TDE) calculation. The FactSage program and NUCLEA database were applied to estimate the phase equilibria of debris. It was confirmed that the TDE calculation using the database can reproduce the phase separation behavior of debris observed in the Three Mile Island accident. In the TDE calculation of 1F, the oxygen potential [G(O{sub 2})] was assumed to be a variable. At low G(O{sub 2}) wheremore » metallic zirconium remains, (U,Zr)O{sub 2}, UO{sub 2}, and ZrO{sub 2} were found as oxides, and oxygen-dispersed Zr, Fe{sub 2}(Zr,U), and Fe{sub 3}UZr{sub 2} were found as metals. With an increase in zirconium oxidation, the mass of those metals, especially Fe{sub 3}UZr{sub 2}, decreased, but the other phases of metals hardly changed qualitatively. Consequently, (U,Zr)O{sub 2} is suggested as a typical phase of oxide, and Fe{sub 2}(Zr,U) is suggested as that of metal. However, a more detailed estimation is necessary to consider the distribution of Fe in the reactor pressure vessel through core-melt progression. (authors)« less

In-situ TEM observation of nano-void formation in UO2 under irradiation

NASA Astrophysics Data System (ADS)

Sabathier, C.; Martin, G.; Michel, A.; Carlot, G.; Maillard, S.; Bachelet, C.; Fortuna, F.; Kaitasov, O.; Oliviero, E.; Garcia, P.

2014-05-01

Transmission electron microscopy (TEM) observations of UO2 polycrystals irradiated in situ with 4 MeV Au ions were performed at room temperature (RT) to better understand the mechanisms of cavity and ultimately fission products nucleation in UO2. Experiments were carried out at the JANNuS Orsay facility that enables in situ ion irradiations inside the microscope to be carried out. The majority of 4 MeV gold ions were transmitted through the thin foil, and the induced radiation defects were investigated by TEM. Observations showed that nano-void formation occurs at ambient temperature in UO2 thin foils irradiated with energetic heavy ions under an essentially nuclear energy loss regime. The diameter and density of nano-objects were measured as a function of the gold irradiation dose at RT. A previous paper has also revealed a similar nano-object population after a Xe implantation performed at 390 keV at 870 K. The nano-object density was modelled using simple concepts derived from Classical Molecular Dynamics simulations. The results are in good agreement, which suggests a mechanism of heterogeneous nucleation induced by energetic cascade overlaps. This indicates that nano-void formation mechanism is controlled by radiation damage. Such nanovoids are likely to act as sinks for mobile fission products during reactor operation.

Irradiation performance of HTGR recycle fissile fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Homan, F.J.; Long, E.L. Jr.

1976-08-01

The irradiation performance of candidate HTGR recycle fissile fuel under accelerated testing conditions is reviewed. Failure modes for coated-particle fuels are described, and the performance of candidate recycle fissile fuels is discussed in terms of these failure modes. The bases on which UO/sub 2/ and (Th,U)O/sub 2/ were rejected as candidate recycle fissile fuels are outlined, along with the bases on which the weak-acid resin (WAR)-derived fissile fuel was selected as the reference recycle kernel. Comparisons are made relative to the irradiation behavior of WAR-derived fuels of varying stoichiometry and conclusions are drawn about the optimum stoichiometry and the rangemore » of acceptable values. Plans for future testing in support of specification development, confirmation of the results of accelerated testing by real-time experiments, and improvement in fuel performance and reliability are described.« less

AFM characterization of model nuclear fuel oxide multilayer structures modified by heavy ion beam irradiation

NASA Astrophysics Data System (ADS)

Hawley, M. E.; Devlin, D. J.; Reichhardt, C. J.; Sickafus, K. E.; Usov, I. O.; Valdez, J. A.; Wang, Y. Q.

2010-10-01

This work explored a potential new model dispersion fuel form consisting of an actinide material embedded in a radiation tolerant matrix that captures fission products (FPs) and is easily separated chemically as waste from the fuel material. To understand the stability of this proposed dispersion fuel form design, an idealized model system composed of a multilayer film was studied. This system consisted of a tri-layer structure of an MgO layer sandwiched between two HfO 2 layers. HfO 2 served as a surrogate fissile material for UO 2 while MgO represented a stable, fissile product (FP) getter that is easily separated from the fissile material. This type of multilayer film structure allowed us to control the size of and spacing between each layer. The films were grown at room temperature by e-beam deposition on a Si(1 1 1) substrate and post-annealed annealing at a range of temperatures to crystallize the HfO 2 layers. The 550 °C annealed sample was subsequently irradiated with 10 MeV Au 3+ ions at a range of fluences from 5 × 10 13 to 3.74 × 10 16 ions/cm 2. Separate single layer constituent films and the substrate were also irradiated at 5 × 10 15 and 8 × 10 14 and 2 × 10 16, respectively. After annealing and irradiation, the samples were characterized using atomic force imaging techniques to determine local changes in microstructure and mechanical properties. All samples annealed above 550 °C cracked. From the AFM results we observed both crack healing and significant modification of the surface at higher fluences.

Determination of gaseous fission product behavior near the cerium dioxide Σ 3 (111)/[1 1 ¯ 0] tilt grain boundary via first-principles study

DOE PAGES

Xi, Jianqi; Liu, Bin; Xu, Haixuan; ...

2017-12-02

We presenmore » t that grain boundaries (GBs) are the most abundant structural defects in nanostructured nuclear fuels and play an important role in determining fission product behavior, which further affects the performance of nuclear fuels. In this work, cerium dioxide (CeO 2) is used as a surrogate material for mixed oxide fuels to understand gaseous fission product behavior, specifically Xe. First-principles calculations are employed to comprehensively study the behavior of Xe and trap sites for Xe near the Σ 3 (111)/[1 1 ¯ 0] grain boundary in CeO 2, which will provide guidance on overall trends for Xe stability and diffusion at grain boundaries vs in the bulk. Significant segregation behavior of trap sites, regardless of charge states, is observed near the GB. This is mainly ascribed to the local atomic structure near the GB, which results in weaker bond strength and more negative segregation energies. For Xe, however, the segregation profile near the GB is different. Our calculations show that, as the size of trap sites increases, the segregation propensity of Xe is reduced. In addition, under hyper-stoichiometric conditions, the solubility of Xe trapped at the GB is significantly higher than that in the bulk, suggesting higher Xe concentration than that in the bulk. The results of this work demonstrate that the diffusion mechanism of Xe in CeO 2 is comparable to that in UO 2. The diffusion activation energies of Xe atoms in the Σ3GB are lower than that in the bulk CeO 2. Lastly, these results suggest that the diffusivity of Xe atoms is higher along the GB than that in the bulk, which enhances the aggregation of Xe atoms near the GB.« less

Determination of gaseous fission product behavior near the cerium dioxide Σ 3 (111)/[1 1 ¯ 0] tilt grain boundary via first-principles study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xi, Jianqi; Liu, Bin; Xu, Haixuan

We presenmore » t that grain boundaries (GBs) are the most abundant structural defects in nanostructured nuclear fuels and play an important role in determining fission product behavior, which further affects the performance of nuclear fuels. In this work, cerium dioxide (CeO 2) is used as a surrogate material for mixed oxide fuels to understand gaseous fission product behavior, specifically Xe. First-principles calculations are employed to comprehensively study the behavior of Xe and trap sites for Xe near the Σ 3 (111)/[1 1 ¯ 0] grain boundary in CeO 2, which will provide guidance on overall trends for Xe stability and diffusion at grain boundaries vs in the bulk. Significant segregation behavior of trap sites, regardless of charge states, is observed near the GB. This is mainly ascribed to the local atomic structure near the GB, which results in weaker bond strength and more negative segregation energies. For Xe, however, the segregation profile near the GB is different. Our calculations show that, as the size of trap sites increases, the segregation propensity of Xe is reduced. In addition, under hyper-stoichiometric conditions, the solubility of Xe trapped at the GB is significantly higher than that in the bulk, suggesting higher Xe concentration than that in the bulk. The results of this work demonstrate that the diffusion mechanism of Xe in CeO 2 is comparable to that in UO 2. The diffusion activation energies of Xe atoms in the Σ3GB are lower than that in the bulk CeO 2. Lastly, these results suggest that the diffusivity of Xe atoms is higher along the GB than that in the bulk, which enhances the aggregation of Xe atoms near the GB.« less

Structure and Reactivity of X-ray Amorphous Uranyl Peroxide, U 2O 7

DOE PAGES

Odoh, Samuel O.; Shamblin, Jacob; Colla, Christopher A.; ...

2016-03-14

Recent accidents resulting in worker injury and radioactive contamination occurred due to pressurization of uranium yellowcake drums produced in the western USA. The drums contained an unexpected X-ray amorphous reactive form of uranium oxide, U 2O7. Heating hydrated uranyl peroxides produced during in situ mining unintentionally produced U 2O 7. It is a hygroscopic anhydrous uranyl peroxide that reacts rapidly with water to release O 2 gas and form metaschoepite, a uranyl-oxide hydrate. Quantum chemical calculations indicate that the most stable U 2O 7 conformer consists of two bent (UO 2) 2+ uranyl ions bridged by a peroxide group bidentatemore » and parallel to each uranyl ion, and a μ2-O atom, resulting in charge neutrality. A pair distribution function from neutron total scattering supports this structural model. The reactivity of U 2O 7 in water and with water in air is much higher than other uranium oxides, and this can be both hazardous and potentially advantageous in the nuclear fuel cycle.« less

Estimated critical conditions for UF{sub 4}-oil systems in fully oil-reflected spherical geometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Plaster, M.J.

Paraffinic oil has been exposed to UF{sub 6} gas in seal exhaust pumps and cascade equipment at the Portsmouth Gaseous Diffusion Plant. The resulting mixture is more nuclearly reactive than mixtures of UO{sub 2}F{sub 2} and H{sub 2}O and is not bounded by the subcritical mass limits presented in several nuclear criticality safety guides. The purpose of this analysis is to determine several critical parameters; specifically, (1) k{sub {infinity}} and the critical mass for several enrichments and moderation levels and (2) the mass limits for these mixtures. The estimated critical masses for the UF{sub 4}-oil systems are smaller than formore » the UO{sub 2}F{sub 2}-H{sub 2}O systems. The suggested mass limits for the UF{sub 4}-oil systems are 0.240, 0.280, 0.350, 0.430, and 0.670, and 1.170 kg {sup 235}U for enrichments of 100, 50, 20, 10, 5, and 3 wt.% {sup 235}U respectively.« less

U(v) in metal uranates: A combined experimental and theoretical study of MgUO 4, CrUO 4, and FeUO 4

DOE PAGES

Guo, Xiaofeng; Tiferet, Eitan; Qi, Liang; ...

2016-01-01

Although pentavalent uranium can exist in aqueous solution, its presence in the solid state is uncommon. Metal monouranates, MgUO 4, CrUO 4 and FeUO 4 were synthesized for detailed structural and energetic investigations. Structural characteristics of these uranates used powder X-ray diffraction, synchrotron X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and 57Fe-Mossbauer spectroscopy. Enthalpies of formation were measured by high temperature oxide melt solution calorimetry. Density functional theory (DFT) calculations provided both structural and energetic information. The measured structural and thermodynamic properties show good consistency with those predicted from DFT. The presence of U 5+ has been solidly confirmed in CrUOmore » 4 and FeUO 4, which are thermodynamically stable compounds, and the origin and stability of U 5+ in the system was elaborated by DFT. Lastly, the structural and thermodynamic behaviour of U 5+ elucidated in this work is relevant to fundamental actinide redox chemistry and to applications in the nuclear industry and radioactive waste disposal.« less

The effect of aluminum additions on the oxidation resistance of U 3Si 2

DOE PAGES

Wood, E. Sooby; White, J. T.; Nelson, A. T.

2017-04-01

The effect of aluminum additions to U 3Si 2 is investigated in this paper as a means to improve the oxidation resistance of this nuclear fuel form. Four U-Si-Al compositions have been synthesized and characterized using scanning electron microscopy, energy dispersive spectroscopy, and x-ray diffraction. The onsets of breakaway oxidation are identified in air thermal ramp tests using thermogravimetric analysis. The final oxidation products following 1000° C air exposure are identified using x-ray diffraction and compared to those of UO 2 and U metal oxidized in the same manner. Finally, thermogravimetric data acquired in this study indicates that increasing amountsmore » of Al in U 3Si 2 further delays the onset of breakaway oxidation, providing enhanced oxidation resistance in air. Al 2O 3 formation on U 3Al 2Si 3 is observed following a heat treatment performed at 500° C in air, demonstrating the potential of Al additions to improve the oxidation resistance of U 3Si 2.« less

The effect of aluminum additions on the oxidation resistance of U 3Si 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wood, E. Sooby; White, J. T.; Nelson, A. T.

The effect of aluminum additions to U 3Si 2 is investigated in this paper as a means to improve the oxidation resistance of this nuclear fuel form. Four U-Si-Al compositions have been synthesized and characterized using scanning electron microscopy, energy dispersive spectroscopy, and x-ray diffraction. The onsets of breakaway oxidation are identified in air thermal ramp tests using thermogravimetric analysis. The final oxidation products following 1000° C air exposure are identified using x-ray diffraction and compared to those of UO 2 and U metal oxidized in the same manner. Finally, thermogravimetric data acquired in this study indicates that increasing amountsmore » of Al in U 3Si 2 further delays the onset of breakaway oxidation, providing enhanced oxidation resistance in air. Al 2O 3 formation on U 3Al 2Si 3 is observed following a heat treatment performed at 500° C in air, demonstrating the potential of Al additions to improve the oxidation resistance of U 3Si 2.« less

FCI experiments in the corium/water system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Huhtiniemi, I.; Hohmann, H.; Magallon, D.

The KROTOS fuel coolant interaction (FCI) tests aim at providing benchmark data to examine the effect of fuel/coolant initial conditions and mixing on explosion energetics. Experiments, fundamental in nature, are performed in well-controlled geometries and are complementary to the FARO large scale tests. Recently, a new test series was started using 3 kg of prototypical core material (80 w/o UO{sub 2}, 20 w/o ZrO{sub 2}) which was poured into a water column of {le} 1.25 m in height (95 mm and 200 mm in diameter) under 0.1 MPa ambient pressure. Four tests have been performed in the test section ofmore » 95 mm in diameter (ID) with different subcooling levels (10-80K) and with and without an external trigger. Additionally, one test has been performed with a test section of 200 mm in diameter (ID) and with an external trigger. No spontaneous or triggered energetic FCIs (steam explosions) have been observed in these corium tests. This is in sharp contrast with the steam explosions observed in the previously reported Al{sub 2}O{sub 3} test series which had the same initial conditions of ambient pressure and subcooling. The post-test analysis of the corium experiments indicated that strong vaporisation at the melt/water contact led to a partial expulsion of the melt from the test section into the pressure vessel. In order to avoid this and to obtain a good penetration and premixing os the corium melt, an additional test has been performed with a larger diameter test section. In all the UO{sub 2}-ZrO{sub 2} tests an efficient quenching process (0.7-1.2 MW/kg-melt) with total fuel fragmentation (mass mean diameter 1.4-2.5 mm) was observed. Results from Al{sub 2}O{sub 3} tests under the same initial conditions are also presented for further confirmation of the observed differences in behaviour between Al{sub 2}O{sub 3} and UO{sub 2}-ZrO{sub 2} melts.« less

Conceptual designs of NDA instruments for the NRTA system at the Rokkasho Reprocessing Plant

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, T.K.; Klosterbuer, S.F.; Menlove, H.O.

The authors are studying conceptual designs of selected nondestructive assay (NDA) instruments for the near-real-time accounting system at the rokkasho Reprocessing Plant (RRP) of Japan Nuclear Fuel Limited (JNFL). The JNFL RRP is a large-scale commercial reprocessing facility for spent fuel from boiling-water and pressurized-water reactors. The facility comprises two major components: the main process area to separate and produce purified plutonium nitrate and uranyl nitrate from irradiated reactor spent fuels, and the co-denitration process area to combine and convert the plutonium nitrate and uranyl nitrate into mixed oxide (MOX). The selected NDA instruments for conceptual design studies are themore » MOX-product canister counter, holdup measurement systems for calcination and reduction furnaces and for blenders in the co-denitration process, the isotope dilution gamma-ray spectrometer for the spent fuel dissolver solution, and unattended verification systems. For more effective and practical safeguards and material control and accounting at RRP, the authors are also studying the conceptual design for the UO{sub 3} large-barrel counter. This paper discusses the state-of-the-art NDA conceptual design and research and development activities for the above instruments.« less

Universal fuel basket for use with an improved oxide reduction vessel and electrorefiner vessel

DOEpatents

Herrmann, Steven D.; Mariani, Robert D.

2002-01-01

A basket, for use in the reduction of UO.sub.2 to uranium metal and in the electrorefining of uranium metal, having a continuous annulus between inner and outer perforated cylindrical walls, with a screen adjacent to each wall. A substantially solid bottom and top plate enclose the continuous annulus defining a fuel bed. A plurality of scrapers are mounted adjacent to the outer wall extending longitudinally thereof, and there is a mechanism enabling the basket to be transported remotely.

On the effect of irradiation-induced resolution in modelling fission gas release in UO2 LWR fuel

NASA Astrophysics Data System (ADS)

Lösönen, Pekka

2017-12-01

Irradiation resolution of gas atoms and vacancies from intra- and intergranular bubbles in sintered UO2 fuel was studied by comparing macroscopic models with a more mechanistic approach. The applied macroscopic models imply the resolution rate of gas atoms to be proportional to gas concentration in intragranular bubbles and at grain boundary (including intergranular bubbles). A relation was established between the macroscopic models and a single encounter of an energetic fission fragment with a bubble. The effect of bubble size on resolution was quantified. The number of resoluted gas atoms per encounter of a fission fragment per bubble was of the same order of magnitude for intra- and intergranular bubbles. However, the resulting macroscopic resolution rate of gas atoms was about two orders of magnitude larger from intragranular bubbles. The number of vacancies resoluted from a grain face bubble by a passing fission fragment was calculated. The obtained correlations for resolution of gas atoms from intragranular bubbles and grain boundaries and for resolution of vacancies from grain face bubbles were used to demonstrate the effect of irradiation resolution on fission gas release.

Trimolecular reactions of uranium hexafluoride with water.

PubMed

Lind, Maria C; Garrison, Stephen L; Becnel, James M

2010-04-08

The hydrolysis reaction of uranium hexafluoride (UF(6)) is a key step in the synthesis of uranium dioxide (UO(2)) powder for nuclear fuels. Mechanisms for the hydrolysis reactions are studied here with density functional theory and the Stuttgart small-core scalar relativistic pseudopotential and associated basis set for uranium. The reaction of a single UF(6) molecule with a water molecule in the gas phase has been previously predicted to proceed over a relatively sizable barrier of 78.2 kJ x mol(-1), indicating this reaction is only feasible at elevated temperatures. Given the observed formation of a second morphology for the UO(2) product coupled with the observations of rapid, spontaneous hydrolysis at ambient conditions, an alternate reaction pathway must exist. In the present work, two trimolecular hydrolysis mechanisms are studied with density functional theory: (1) the reaction between two UF(6) molecules and one water molecule, and (2) the reaction of two water molecules with a single UF(6) molecule. The predicted reaction of two UF(6) molecules with one water molecule displays an interesting "fluorine-shuttle" mechanism, a significant energy barrier of 69.0 kJ x mol(-1) to the formation of UF(5)OH, and an enthalpy of reaction (DeltaH(298)) of +17.9 kJ x mol(-1). The reaction of a single UF(6) molecule with two water molecules displays a "proton-shuttle" mechanism, and is more favorable, having a slightly lower computed energy barrier of 58.9 kJ x mol(-1) and an exothermic enthalpy of reaction (DeltaH(298)) of -13.9 kJ x mol(-1). The exothermic nature of the overall UF(6) + 2H(2)O trimolecular reaction and the lowering of the barrier height with respect to the bimolecular reaction are encouraging.

New insight into the ternary complexes of uranyl carbonate in seawater.

PubMed

Beccia, M R; Matara-Aho, M; Reeves, B; Roques, J; Solari, P L; Monfort, M; Moulin, C; Den Auwer, C

2017-11-01

Uranium is naturally present in seawater at trace levels and may in some cases be present at higher concentrations, due to anthropogenic nuclear activities. Understanding uranium speciation in seawater is thus essential for predicting and controlling its behavior in this specific environmental compartment and consequently, its possible impact on living organisms. The carbonato calcic complex Ca 2 UO 2 (CO 3 ) 3 was previously identified as the main uranium species in natural seawater, together with CaUO 2 (CO 3 ) 3 2- . In this work, we further investigate the role of the alkaline earth cation in the structure of the ternary uranyl-carbonate complexes. For this purpose, artificial seawater, free of Mg 2+ and Ca 2+ , using Sr 2+ as a spectroscopic probe was prepared. Combining TRLIF and EXAFS spectroscopy, together with DFT and theoretical thermodynamic calculations, evidence for the presence of Sr alkaline earth counter ion in the complex structure can be asserted. Furthermore, data suggest that when Ca 2+ is replaced by Sr 2+ , SrUO 2 (CO 3 ) 3 2- is the main complex in solution and it occurs with the presence of at least one monodentate carbonate in the uranyl coordination sphere. Copyright © 2017 Elsevier Ltd. All rights reserved.

Status of Wrought FeCrAl-UO 2 Capsules Irradiated in the Advanced Test Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Field, Kevin G.; Harp, J.; Core, G.

2017-07-01

Candidate cladding materials for accident tolerant fuel applications require extensive testing and validation prior to commercial deployment within the nuclear power industry. One class of cladding materials, FeCrAl alloys, is currently undergoing such effort. Within these activities is a series of irradiation programs within the Advanced Test Reactor. These programs are developed to aid in commercial maturation and understand the fundamental mechanisms controlling the cladding performance during normal operation of a typical light water reactor. Three different irradiation programs are on-going; one designed as a simple proof-of-principle concept, the other to evaluate the susceptibility of FeCrAl to fuel-cladding chemical interaction,more » and the last to fully simulate the conditions of a pressurized water reactor experimentally. To date, nondestructive post-irradiation examination has been completed on the rodlet deemed FCA-L3 from the simple proof-of-concept irradiation program. Initial results show possible breach of the rodlet under irradiation but further studies are needed to conclusively determine whether breach has occurred and the underlying reasons for such a possible failure. Further work includes characterizing additional rodlets following irradiation.« less

Abilities of helium immobilization by the UO2 surface using the “ab initio” method

NASA Astrophysics Data System (ADS)

Dąbrowski, Ludwik; Szuta, Marcin

2016-09-01

We present density functional theory calculation results concerning the uranium dioxide crystals with a helium atom incorporated in the octahedral sites on a nano superficial layer of UO2 fuel element. In order to quantify the capability of helium immobilization we propose a quantum model of adsorption and desorption which we compare with the classical model of Langmuir. Significant differences between the models are maintained in a wide temperature range including high temperatures of the order of 1000 K. By the proposed method of quantum isotherms it was established that the octahedral positions near the metal surface are good traps for helium atoms. While in a temperature close to 1089 K it predicts an intensive release of helium, which is consistent with the experimental results.

Effects of ionizing radiation and temperature on uranyl silicates: soddyite (UO2)2(SiO4)(H2O)2 and Uranophane Ca(UO2)2(SiO3OH)2·5H2O.

PubMed

Sureda, R; Casas, I; Giménez, J; de Pablo, J; Quiñones, J; Zhang, J; Ewing, R C

2011-03-15

The stability of soddyite under electron irradiation has been studied over the temperature range of 25-300 °C. At room temperature, soddyite undergoes a crystalline-to-amorphous transformation (amorphization) at a total dose of 6.38 × 10(8) Gy. The electron beam irradiation results suggest that the soddyite structure is susceptible to radiation-induced nanocrystallization of UO(2). The temperature dependence of amorphization dose increases linearly up to 300 °C. A thermogravimetric and calorimetric analysis (TGA-DSC) combined with X-ray diffraction (XRD) indicates that soddyite retains its water groups up to 400 °C, followed by the collapse of the structure. Based on thermal analysis of uranophane, the removal of some water groups at relatively low temperatures provokes the collapse of the uranophane structure. This structural change appears to be the reason for the increase of amorphization dose at 140 °C. According to the results obtained, radiation field of a nuclear waste repository, rather than temperature effects, may cause changes in the crystallinity of soddyite and affect its stability during long-term storage.

Pellet cladding mechanical interactions of ceramic claddings fuels under light water reactor conditions

NASA Astrophysics Data System (ADS)

Li, Bo-Shiuan

Ceramic materials such as silicon carbide (SiC) are promising candidate materials for nuclear fuel cladding and are of interest as part of a potential accident tolerant fuel design due to its high temperature strength, dimensional stability under irradiation, corrosion resistance, and lower neutron absorption cross-section. It also offers drastically lower hydrogen generation in loss of coolant accidents such as that experienced at Fukushima. With the implementation of SiC material properties to the fuel performance code, FRAPCON, performances of the SiC-clad fuel are compared with the conventional Zircaloy-clad fuel. Due to negligible creep and high stiffness, SiC-clad fuel allows gap closure at higher burnup and insignificant cladding dimensional change. However, severe degradation of SiC thermal conductivity with neutron irradiation will lead to higher fuel temperature with larger fission gas release. High stiffness of SiC has a drawback of accumulating large interfacial pressure upon pellet-cladding mechanical interactions (PCMI). This large stress will eventually reach the flexural strength of SiC, causing failure of SiC cladding instantly in a brittle manner instead of the graceful failure of ductile metallic cladding. The large interfacial pressure causes phenomena that were previously of only marginal significance and thus ignored (such as creep of the fuel) to now have an important role in PCMI. Consideration of the fuel pellet creep and elastic deformation in PCMI models in FRAPCON provide for an improved understanding of the magnitude of accumulated interfacial pressure. Outward swelling of the pellet is retarded by the inward irradiation-induced creep, which then reduces the rate of interfacial pressure buildup. Effect of PCMI can also be reduced and by increasing gap width and cladding thickness. However, increasing gap width and cladding thickness also increases the overall thermal resistance which leads to higher fuel temperature and larger fission gas release. An optimum design is sought considering both thermal and mechanical models of this ceramic cladding with UO2 and advanced high density fuels.

Electrical heating tests of uranium dioxide external fuel configuration at emitter temperature of 1900 K

NASA Technical Reports Server (NTRS)

Diianni, D. C.; Mayer, J. T.

1974-01-01

Testing of two fuel clad specimens for thermionic reactor application is described. The annular UO2 fuel was clad on both sides with tungsten; heat rejection was radially inward. The tests were intended to study inner clad stability, fuel redistribution, and fuel melting problems. The specimens were tested in a vacuum chamber using electron bombardment heating. Fuel structural changes were studied using periodic gammagraphs and posttest metallography. The first specimen test was terminated at 50 hours because of a braze failure. The second specimen was tested for 240 hours when an outer clad leak developed due to a tungsten-water reaction. The fuel developed numerous cracks on cooldown but the inner clad remained dimensionally stable. The fuel cover gas did not impede the rate of fuel redistribution. Posttest examination showed the fuel had not melted during operation.

Mars Mission Analysis Trades Based on Legacy and Future Nuclear Propulsion Options

NASA Astrophysics Data System (ADS)

Joyner, Russell; Lentati, Andrea; Cichon, Jaclyn

2007-01-01

The purpose of this paper is to discuss the results of mission-based system trades when using a nuclear thermal propulsion (NTP) system for Solar System exploration. The results are based on comparing reactor designs that use a ceramic-metallic (CERMET), graphite matrix, graphite composite matrix, or carbide matrix fuel element designs. The composite graphite matrix and CERMET designs have been examined for providing power as well as propulsion. Approaches to the design of the NTP to be discussed will include an examination of graphite, composite, carbide, and CERMET core designs and the attributes of each in regards to performance and power generation capability. The focus is on NTP approaches based on tested fuel materials within a prismatic fuel form per the Argonne National Laboratory testing and the ROVER/NERVA program. NTP concepts have been examined for several years at Pratt & Whitney Rocketdyne for use as the primary propulsion for human missions beyond earth. Recently, an approach was taken to examine the design trades between specific NTP concepts; NERVA-based (UC)C-Graphite, (UC,ZrC)C-Composite, (U,Zr)C-Solid Carbide and UO2-W CERMET. Using Pratt & Whitney Rocketdyne's multidisciplinary design analysis capability, a detailed mission and vehicle model has been used to examine how several of these NTP designs impact a human Mars mission. Trends for the propulsion system mass as a function of power level (i.e. thrust size) for the graphite-carbide and CERMET designs were established and correlated against data created over the past forty years. These were used for the mission trade study. The resulting mission trades presented in this paper used a comprehensive modeling approach that captures the mission, vehicle subsystems, and NTP sizing.

Validation of updated neutronic calculation models proposed for Atucha-II PHWR. Part I: Benchmark comparisons of WIMS-D5 and DRAGON cell and control rod parameters with MCNP5

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mollerach, R.; Leszczynski, F.; Fink, J.

2006-07-01

In 2005 the Argentine Government took the decision to complete the construction of the Atucha-II nuclear power plant, which has been progressing slowly during the last ten years. Atucha-II is a 745 MWe nuclear station moderated and cooled with heavy water, of German (Siemens) design located in Argentina. It has a pressure-vessel design with 451 vertical coolant channels, and the fuel assemblies (FA) are clusters of 37 natural UO{sub 2} rods with an active length of 530 cm. For the reactor physics area, a revision and update calculation methods and models (cell, supercell and reactor) was recently carried out coveringmore » cell, supercell (control rod) and core calculations. As a validation of the new models some benchmark comparisons were done with Monte Carlo calculations with MCNP5. This paper presents comparisons of cell and supercell benchmark problems based on a slightly idealized model of the Atucha-I core obtained with the WIMS-D5 and DRAGON codes with MCNP5 results. The Atucha-I core was selected because it is smaller, similar from a neutronic point of view, and more symmetric than Atucha-II Cell parameters compared include cell k-infinity, relative power levels of the different rings of fuel rods, and some two-group macroscopic cross sections. Supercell comparisons include supercell k-infinity changes due to the control rods (tubes) of steel and hafnium. (authors)« less

Enhancing the ABAQUS Thermomechanics Code to Simulate Steady and Transient Fuel Rod Behavior

DOE Office of Scientific and Technical Information (OSTI.GOV)

R. L. Williamson; D. A. Knoll

2009-09-01

A powerful multidimensional fuels performance capability, applicable to both steady and transient fuel behavior, is developed based on enhancements to the commercially available ABAQUS general-purpose thermomechanics code. Enhanced capabilities are described, including: UO2 temperature and burnup dependent thermal properties, solid and gaseous fission product swelling, fuel densification, fission gas release, cladding thermal and irradiation creep, cladding irradiation growth , gap heat transfer, and gap/plenum gas behavior during irradiation. The various modeling capabilities are demonstrated using a 2D axisymmetric analysis of the upper section of a simplified multi-pellet fuel rod, during both steady and transient operation. Computational results demonstrate the importancemore » of a multidimensional fully-coupled thermomechanics treatment. Interestingly, many of the inherent deficiencies in existing fuel performance codes (e.g., 1D thermomechanics, loose thermo-mechanical coupling, separate steady and transient analysis, cumbersome pre- and post-processing) are, in fact, ABAQUS strengths.« less

Structural characterization of environmentally relevant ternary uranyl citrate complexes present in aqueous solutions and solid state materials.

PubMed

Basile, Madeline; Unruh, Daniel K; Flores, Erin; Johns, Adam; Forbes, Tori Z

2015-02-14

Organic acids are important metal chelators in environmental systems and tend to form soluble complexes in aqueous solutions, ultimately influencing the transport and bioavailability of contaminants in surface and subsurface waters. This is particularly true for the formation of uranyl citrate complexes, which have been utilized in advanced photo- and bioremediation strategies for soils contaminated with nuclear materials. Given the complexity of environmental systems, the formation of ternary or heterometallic uranyl species in aqueous solutions are also expected, particularly with Al(iii) and Fe(iii) cations. These ternary forms are reported to be more stable in aqueous solutions, potentially enhancing contaminant mobility and uptake by organisms, but the exact coordination geometries of these soluble molecular complexes have not been elucidated. To provide insight into the nature of these species, we have developed a series of geochemical model compounds ([(UO(2))(2)Al(2)(C(6)H(4)O(7))(4)](6-) (U(2)Al(2)), [(UO(2))(2)Fe(2)(C(6)H(4)O(7))(4)](6-) (U(2)Fe(2)-1) and [(UO(2))(2)Fe(2)(C(6)H(4)O(7))(4)(H(2)O)(2)](6-) (U(2)Fe(2)-2) and [(UO(2))(2)Fe(4)(OH)(4)(C(6)H(4)O(7))(4)](8-) (U(2)Fe(4))) that were characterized by single-crystal X-ray diffraction and vibrational spectroscopy. Mass spectroscopy was then employed to compare the model compounds to species present in aqueous solutions to provide an enhanced understanding of the ternary uranyl citrate complexes that could be relevant in natural systems.

Electron Microscopic Examination of Irradiated TRISO Coated Particles of Compact 6-3-2 of AGR-1 Experiment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Van Rooyen, Isabella Johanna; Demkowicz, Paul Andrew; Riesterer, Jessica Lori

2012-12-01

The electron microscopic examination of selected irradiated TRISO coated particles of the AGR-1 experiment of fuel compact 6-3-2 are presented in this report. Compact 6-3-2 refers to the compact in Capsule 6 at level 3 of Stack 2. The fuel used in capsule 6 compacts, are called the “baseline” fuel as it is fabricated with refined coating process conditions used to fabricate historic German fuel, because of its excellent irradiation performance with UO2 kernels. The AGR-1 fuel is however made of low-enriched uranium oxycarbide (UCO). Kernel diameters are approximately 350 µm with a U-235 enrichment of approximately 19.7%. Compact 6-3-2more » has been irradiated to 11.3% FIMA compact average burn-up with a time average, volume average temperature of 1070.2°C and with a compact average fast fluence of 2.38E21 n/cm« less

Electron Microscopic Examination of Irradiated TRISO Coated Particles of Compact 6-3-2 of AGR-1 Experiment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Van Rooyen, Isabella Johanna; Demkowicz, Paul Andrew; Riesterer, Jessica Lori

2012-12-01

The electron microscopic examination of selected irradiated TRISO coated particles of the AGR-1 experiment of fuel compact 6-3-2 are presented in this report. Compact 6-3-2 refers to the compact in Capsule 6 at level 3 of Stack 2. The fuel used in capsule 6 compacts, are called the “baseline” fuel as it is fabricated with refined coating process conditions used to fabricate historic German fuel, because of its excellent irradiation performance with UO 2 kernels. The AGR-1 fuel is however made of low-enriched uranium oxycarbide (UCO). Kernel diameters are approximately 350 µm with a U-235 enrichment of approximately 19.7%. Compactmore » 6-3-2 has been irradiated to 11.3% FIMA compact average burn-up with a time average, volume average temperature of 1070.2°C and with a compact average fast fluence of 2.38E21 n/cm« less

Critical experiments at Sandia National Laboratories : technical meeting on low-power critical facilities and small reactors.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harms, Gary A.; Ford, John T.; Barber, Allison Delo

2010-11-01

Sandia National Laboratories (SNL) has conducted radiation effects testing for the Department of Energy (DOE) and other contractors supporting the DOE since the 1960's. Over this period, the research reactor facilities at Sandia have had a primary mission to provide appropriate nuclear radiation environments for radiation testing and qualification of electronic components and other devices. The current generation of reactors includes the Annular Core Research Reactor (ACRR), a water-moderated pool-type reactor, fueled by elements constructed from UO2-BeO ceramic fuel pellets, and the Sandia Pulse Reactor III (SPR-III), a bare metal fast burst reactor utilizing a uranium-molybdenum alloy fuel. The SPR-IIImore » is currently defueled. The SPR Facility (SPRF) has hosted a series of critical experiments. A purpose-built critical experiment was first operated at the SPRF in the late 1980's. This experiment, called the Space Nuclear Thermal Propulsion Critical Experiment (CX), was designed to explore the reactor physics of a nuclear thermal rocket motor. This experiment was fueled with highly-enriched uranium carbide fuel in annular water-moderated fuel elements. The experiment program was completed and the fuel for the experiment was moved off-site. A second critical experiment, the Burnup Credit Critical Experiment (BUCCX) was operated at Sandia in 2002. The critical assembly for this experiment was based on the assembly used in the CX modified to accommodate low-enriched pin-type fuel in water moderator. This experiment was designed as a platform in which the reactivity effects of specific fission product poisons could be measured. Experiments were carried out on rhodium, an important fission product poison. The fuel and assembly hardware for the BUCCX remains at Sandia and is available for future experimentation. The critical experiment currently in operation at the SPRF is the Seven Percent Critical Experiment (7uPCX). This experiment is designed to provide benchmark reactor physics data to support validation of the reactor physics codes used to design commercial reactor fuel elements in an enrichment range above the current 5% enrichment cap. A first set of critical experiments in the 7uPCX has been completed. More experiments are planned in the 7uPCX series. The critical experiments at Sandia National Laboratories are currently funded by the US Department of Energy Nuclear Criticality Safety Program (NCSP). The NCSP has committed to maintain the critical experiment capability at Sandia and to support the development of a critical experiments training course at the facility. The training course is intended to provide hands-on experiment experience for the training of new and re-training of practicing Nuclear Criticality Safety Engineers. The current plans are for the development of the course to continue through the first part of fiscal year 2011 with the development culminating is the delivery of a prototype of the course in the latter part of the fiscal year. The course will be available in fiscal year 2012.« less

The structure of liquid UO2-x in reducing gas atmospheres

NASA Astrophysics Data System (ADS)

Alderman, O. L. G.; Benmore, C. J.; Weber, J. K. R.; Skinner, L. B.; Tamalonis, A. J.; Sendelbach, S.; Hebden, A.; Williamson, M. A.

2017-02-01

High energy X-ray diffraction experiments performed on hypostoichiometric UO2-x liquids in reducing gas mixtures of 95%Ar:5%CO and 95%Ar:5%H2 are compared to that conducted in a pure Ar atmosphere [Skinner et al., Science 346, 984 (2014)]. The measurements are pertinent to severe accident scenarios at nuclear reactors, where core melts can encounter reducing conditions and further shed light on the oxide chemistry of the low valence states of uranium, particularly U(III), which become stable only at very high temperatures and low oxygen potentials. The radioactive samples were melted by floating small spheres of material using an aerodynamic levitator and heating with a laser beam. In the more reducing environments, a 1.7% shift to lower Q-values is observed in the position of the principal peak of the measured X-ray structure factors, compared to the more oxidizing Ar environment. This corresponds to an equivalent elongation in the U-U nearest neighbor distances and the U-U periodicity. The U-O peak (modal) bond-length, as measured from the real-space total correlation functions, is also observed to expand by 0.9-1.6% under reducing conditions, consistent with the presence of 15-27% U3+ cations, assuming constant U-O coordination number. The slightly larger U-U elongation, as compared to the U-O elongation, is interpreted as a slight increase in U-O-U bond angles. Difficulties concerning the determination of the hypostoichiometry, x, are discussed, along with the future directions for related research.

The structure of liquid UO 2-x in reducing gas atmospheres

DOE PAGES

Alderman, O. L. G.; Benmore, C. J.; Weber, J. K. R.; ...

2017-02-22

High energy X-ray diffraction experiments performed on hypostoichiometric UO 2-x liquids in reducing gas mixtures of 95%Ar:5%CO and 95%Ar:5%H 2 are compared to that conducted in a pure Ar atmosphere [Skinner et al., Science 346, 984 (2014)]. The measurements are pertinent to severe accident scenarios at nuclear reactors, where core melts can encounter reducing conditions and further shed light on the oxide chemistry of the low valence states of uranium, particularly U(III), which become stable only at very high temperatures and low oxygen potentials. The radioactive samples were melted by floating small spheres of material using an aerodynamic levitator andmore » heating with a laser beam. In the more reducing environments, a 1.7% shift to lower Q-values is observed in the position of the principal peak of the measured X-ray structure factors, compared to the more oxidizing Ar environment. This corresponds to an equivalent elongation in the U-U nearest neighbor distances and the U-U periodicity. The U-O peak (modal) bond-length, as measured from the real-space total correlation functions, is also observed to expand by 0.9–1.6% under reducing conditions, consistent with the presence of 15–27% U 3+ cations, assuming constant U-O coordination number. The slightly larger U-U elongation, as compared to the U-O elongation, is interpreted as a slight increase in U-O-U bond angles. Difficulties concerning the determination of the hypostoichiometry, x, are discussed, along with the future directions for related research.« less

Subcritical unity for the Argonaut reactor (in Portuguese)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mongiovi, G.; Aghina, L.O.B.

1971-04-01

tubetype fuel elements aiming at the construction of a subcritical unit employing the internal thermal column of an Argonaut reactor as a source. The results confirmed the feasibility of the use of natural UO/sub 2/ for the proposed arrangement as long as one has a strong source or a subcritical unit diameter greater than 100 cm. (INIS)

Fully Ceramic Microencapsulated Fuel Development for LWR Applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Snead, Lance Lewis; Besmann, Theodore M; Terrani, Kurt A

2012-01-01

The concept, fabrication, and key feasibility issues of a new fuel form based on the microencapsulated (TRISO-type) fuel which has been specifically engineered for LWR application and compacted within a SiC matrix will be presented. This fuel, the so-called fully ceramic microencapsulated fuel is currently undergoing development as an accident tolerant fuel for potential UO2 replacement in commercial LWRs. While the ability of this fuel to facilitate normal LWR cycle performance is an ongoing effort within the program, this will not be a focus of this paper. Rather, key feasibility and performance aspects of the fuel will be presented includingmore » the ability to fabricate a LWR-specific TRISO, the need for and route to a high thermal conductivity and fully dense matrix that contains neutron poisons, and the performance of that matrix under irradiation and the interaction of the fuel with commercial zircaloy clad.« less

Precisely Determining Ultralow level UO22+ in Natural Water with Plasmonic Nanowire Interstice Sensor

NASA Astrophysics Data System (ADS)

Gwak, Raekeun; Kim, Hongki; Yoo, Seung Min; Lee, Sang Yup; Lee, Gyoung-Ja; Lee, Min-Ku; Rhee, Chang-Kyu; Kang, Taejoon; Kim, Bongsoo

2016-01-01

Uranium is an essential raw material in nuclear energy generation; however, its use raises concerns about the possibility of severe damage to human health and the natural environment. In this work, we report an ultrasensitive uranyl ion (UO22+) detection method in natural water that uses a plasmonic nanowire interstice (PNI) sensor combined with a DNAzyme-cleaved reaction. UO22+ induces the cleavage of DNAzymes into enzyme strands and released strands, which include Raman-active molecules. A PNI sensor can capture the released strands, providing strong surface-enhanced Raman scattering signal. The combination of a PNI sensor and a DNAzyme-cleaved reaction significantly improves the UO22+ detection performance, resulting in a detection limit of 1 pM and high selectivity. More importantly, the PNI sensor operates perfectly, even in UO22+-contaminated natural water samples. This suggests the potential usefulness of a PNI sensor in practical UO22+-sensing applications. We anticipate that diverse toxic metal ions can be detected by applying various ion-specific DNA-based ligands to PNI sensors.

Phase separation of metal-added corium and its effect on a steam explosion

NASA Astrophysics Data System (ADS)

Min, B. T.; Kim, J. H.; Hong, S. W.; Hong, S. H.; Park, I. K.; Song, J. H.; Kim, H. D.

2008-07-01

To simulate a relocation of molten core material and its interaction phenomenon with water during a severe accident in a nuclear reactor, a typical corium of UO 2/ZrO 2/Zr/Stainless steel mixed at a 62 wt%, 15 wt%, 12 wt% and 11 wt%, respectively, was melted and then cooled down to become a solidified ingot. It was shown that the molten corium was separated into two layers, of which the upper layer was oxide mixtures and the lower layer was metal alloys. The upper layer was UO 2 and ZrO 2 and the lower layer mostly consisted of metal mixtures such as uranium, zirconium and stainless steel. Iron content varied with the positions and about a half of it existed as an alloy such as Fe 2U. Uranium metal was produced by reduction of UO 2 by zirconium metal. The average densities of the upper oxide layer and the lower metal layer were 8.802 and 9.411 g/cm 3, respectively. In another test, metal-added molten corium was poured into water and it showed that a steam explosion could occur by applying an external trigger.

NEUTRONIC REACTOR

DOEpatents

Daniels, F.

1962-12-18

A power plant is described comprising a turbine and employing round cylindrical fuel rods formed of BeO and UO/sub 2/ and stacks of hexagonal moderator blocks of BeO provided with passages that loosely receive the fuel rods so that coolant may flow through the passages over the fuels to remove heat. The coolant may be helium or steam and fiows through at least one more heat exchanger for producing vapor from a body of fluid separate from the coolant, which fluid is to drive the turbine for generating electricity. By this arrangement the turbine and directly associated parts are free of particles and radiations emanating from the reactor. (AEC)

Determination of irradiated reactor uranium in soil samples in Belarus using 236U as irradiated uranium tracer.

PubMed

Mironov, Vladislav P; Matusevich, Janna L; Kudrjashov, Vladimir P; Boulyga, Sergei F; Becker, J Sabine

2002-12-01

This work presents experimental results on the distribution of irradiated reactor uranium from fallout after the accident at Chernobyl Nuclear Power Plant (NPP) in comparison to natural uranium distribution in different soil types. Oxidation processes and vertical migration of irradiated uranium in soils typical of the 30 km relocation area around Chernobyl NPP were studied using 236U as the tracer for irradiated reactor uranium and inductively coupled plasma mass spectrometry as the analytical method for uranium isotope ratio measurements. Measurements of natural uranium yielded significant variations of its concentration in upper soil layers from 2 x 10(-7) g g(-1) to 3.4 x 10(-6) g g(-1). Concentrations of irradiated uranium in the upper 0-10 cm soil layers at the investigated sampling sites varied from 5 x 10(-12) g g(-1) to 2 x 10(-6) g g(-1) depending on the distance from Chernobyl NPP. In the majority of investigated soil profiles 78% to 97% of irradiated "Chernobyl" uranium is still contained in the upper 0-10 cm soil layers. The physical and chemical characteristics of the soil do not have any significant influence on processes of fuel particle destruction. Results obtained using carbonate leaching of 236U confirmed that more than 60% of irradiated "Chernobyl" uranium is still in a tetravalent form, ie. it is included in the fuel matrix (non-oxidized fuel UO2). The average value of the destruction rate of fuel particles determined for the Western radioactive trace (k = 0.030 +/- 0.005 yr(-1)) and for the Northern radioactive trace (k = 0.035 + 0.009 yr(-1)) coincide within experimental errors. Use of leaching of fission products in comparison to leaching of uranium for study of the destruction rate of fuel particles yielded poor coincidence due to the fact that use of fission products does not take into account differences in the chemical properties of fission products and fuel matrix (uranium).

Unusual ion UO(4)(-) formed upon collision induced dissociation of [UO(2)(NO(3))(3)](-), [UO(2)(ClO(4))(3)](-), [UO(2)(CH(3)COO)(3)](-) ions.

PubMed

Sokalska, Marzena; Prussakowska, Małgorzata; Hoffmann, Marcin; Gierczyk, Błazej; Frański, Rafał

2010-10-01

The following ions [UO(2)(NO(3))(3)](-), [UO(2)(ClO(4))(3)](-), [UO(2)(CH(3)COO)(3)](-) were generated from respective salts (UO(2)(NO(3))(2), UO(2)(ClO(4))(3), UO(2)(CH(3)COO)(2)) by laser desorption/ionization (LDI). Collision induced dissociation of the ions has led, among others, to the formation of UO(4)(-) ion (m/z 302). The undertaken quantum mechanical calculations showed this ion is most likely to possess square planar geometry as suggested by MP2 results or strongly deformed geometry in between tetrahedral and square planar as indicated by DFT results. Interestingly, geometrical parameters and analysis of electron density suggest it is an U(VI) compound, in which oxygen atoms bear unpaired electron and negative charge. Copyright © 2010 American Society for Mass Spectrometry. Published by Elsevier Inc. All rights reserved.

Ab-initio study of C and O impurities in uranium nitride

NASA Astrophysics Data System (ADS)

Lopes, Denise Adorno; Claisse, Antoine; Olsson, Pär

2016-09-01

Uranium nitride (UN) has been considered a potential fuel for Generation IV (GEN-IV) nuclear reactors as well as a possible new fuel for Light Water Reactors (LWR), which would permit an extension of the fuel residence time in the reactor. Carbon and oxygen impurities play a key role in the UN microstructure, influencing important parameters such as creep, swelling, gas release under irradiation, compatibility with structural steel and coolants, and thermal stability. In this work, a systematic study of the electronic structure of UN containing C and O impurities using first-principles calculations by the Density Functional Theory (DFT) method is presented. In order to describe accurately the localized U 5f electrons, the DFT + U formalism was adopted. Moreover, to avoid convergence toward metastable states, the Occupation Matrix Control (OMC) methodology was applied. The incorporation of C and O in the N-vacancy is found to be energetically favorable. In addition, only for O, the incorporation in the interstitial position is energetically possible, showing some degree of solubility for this element in this site. The binding energies show that the pairs (Csbnd Nvac) and (Osbnd Nvac) interact much further than the other defects, which indicate the possible occurrence of vacancy drag phenomena and clustering of these impurities in grain boundaries, dislocations and free surfaces. The migration energy of an impurity by single N-vacancy show that C and O employ different paths during diffusion. Oxygen migration requires significantly lower energy than carbon. This fact is due to flexibility in the Usbnd O chemical bonds, which bend during the diffusion forming a pseudo UO2 coordination. On the other hand, C and N have a directional and inflexible chemical bond with uranium; always requiring the octahedral coordination. These findings provide detailed insight into how these impurities behave in the UN matrix, and can be of great interest for assisting the development of this new nuclear fuel for next-generation reactors.

Alternative Anodes for the Electrolytic Reduction of Uranium Dioxide

NASA Astrophysics Data System (ADS)

Merwin, Augustus

Reprocessing of spent nuclear fuel is an essential step in closing the nuclear fuel cycle. In order to consume current stockpiles, ceramic uranium dioxide spent nuclear fuel will be subjected to an electrolytic reduction process. The current reduction process employs a platinum anode and a stainless steel alloy 316 cathode in a molten salt bath consisting of LiCl-2wt% Li 2O and occurs at 700°C. A major shortcoming of the existing process is the degradation of the platinum anode under the severely oxidizing conditions encountered during electrolytic reduction. This work investigates alternative anode materials for the electrolytic reduction of uranium oxide. The high temperature and extreme oxidizing conditions encountered in these studies necessitated a unique set of design constraints on the system. Thus, a customized experimental apparatus was designed and constructed. The electrochemical experiments were performed in an electrochemical reactor placed inside a furnace. This entire setup was housed inside a glove box, in order to maintain an inert atmosphere. This study investigates alternative anode materials through accelerated corrosion testing. Surface morphology was studied using scanning electron microscopy. Surface chemistry was characterized using energy dispersive spectroscopy and Raman spectroscopy. Electrochemical behavior of candidate materials was evaluated using potentiodynamic polarization characteristics. After narrowing the number of candidate electrode materials, ferrous stainless steel alloy 316, nickel based Inconel 718 and elemental tungsten were chosen for further investigation. Of these materials only tungsten was found to be sufficiently stable at the anodic potential required for electrolysis of uranium dioxide in molten salt. The tungsten anode and stainless steel alloy 316 cathode electrode system was studied at the required reduction potential for UO2 with varying lithium oxide concentrations. Electrochemical impedance spectroscopy showed mixed (kinetic and diffusion) control and an overall low impedance due to extreme corrosion. It was observed that tungsten is sufficiently stable in LiCl - 2wt% Li 2O at 700°C at the required anodic potential for the reduction of uranium oxide. This study identifies tungsten to be a superior anode material to platinum for the electrolytic reduction of uranium oxide, both in terms of superior corrosion behavior and reduced cost, and thus recommends that tungsten be further investigated as an alternative anode for the electrolytic reduction of uranium dioxide.

URANIUM OXIDE-CONTAINING FUEL ELEMENT COMPOSITION AND METHOD OF MAKING SAME

DOEpatents

Handwerk, J.H.; Noland, R.A.; Walker, D.E.

1957-09-10

In the past, bodies formed of a mixture of uranium dioxide and aluminum powder have been used in fuel elements; however, these mixtures were found not to be suitable when exposed to temperatures of about 600 deg C, because at such high temperatures the fuel elements were distorted. If uranosic oxide, U/sub 3/O/sub 8/, is substituted for UO/sub 2/, the mechanical properties are not impaired when these materials are used at about 600 deg C and no distortion takes place. The uranosic oxide and aluminum, both in powder form, are first mixed, and after a homogeneous mixture has been obtained, are shaped into fuel elements by extrusion at elevated temperature. Magnesium powder may be used in place of the aluminum.

Diffusion of radiogenic helium in natural uranium oxides

NASA Astrophysics Data System (ADS)

Roudil, Danièle; Bonhoure, Jessica; Pik, Raphaël; Cuney, Michel; Jégou, Christophe; Gauthier-Lafaye, F.

2008-08-01

The issue of nuclear waste management - and especially spent fuel disposal - demands further research on the long-term behavior of helium and its impact on physical changes in UO 2 and (U,Pu)O 2 matrices subjected to self-irradiation. Helium produced by radioactive decay of the actinides concentrates in the grains or is trapped at the grain boundaries. Various scenarios can be considered, and can have a significant effect on the radionuclide source terms that will be accessible to water after the canisters have been breached. Helium production and matrix damage is generally simulated by external irradiation or with actinide-doped materials. A natural uranium oxide sample was studied to acquire data on the behavior of radiogenic helium and its diffusion under self-irradiation in spent fuel. The sample from the Pen Ar Ran deposit in the Vendée region of France dated at 320 ± 9 million of years was selected for its simple geological history, making it a suitable natural analog of spent fuel under repository conditions during the initial period in a closed system not subject to mass transfer with the surrounding environment. Helium outgassing measured by mass spectrometry to determine the He diffusion coefficients through the ore shows that: (i) a maximum of 5% (2.1% on average) of the helium produced during the last 320 Ma in this natural analog was conserved, (ii) about 33% of the residual helium is occluded in the matrix and vacancy defects (about 10 -5 mol g -1) and 67% in bubbles that were analyzed by HRTEM. A similar distribution has been observed in spent fuel and in (U 0.9,Pu 0.1)O 2. The results obtained for the natural Pen Ar Ran sample can be applied by analogy to spent fuel, especially in terms of the apparent solubility limit and the formation, characteristics and behavior of the helium bubbles.

Overview of lower length scale model development for accident tolerant fuels regarding U3Si2 fuel and FeCrAl cladding

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Yongfeng

2016-09-01

U3Si2 and FeCrAl have been proposed as fuel and cladding concepts, respectively, for accident tolerance fuels with higher tolerance to accident scenarios compared to UO2. However, a lot of key physics and material properties regarding their in-pile performance are yet to be explored. To accelerate the understanding and reduce the cost of experimental studies, multiscale modeling and simulation are used to develop physics-based materials models to assist engineering scale fuel performance modeling. In this report, the lower-length-scale efforts in method and material model development supported by the Accident Tolerance Fuel (ATF) high-impact-problem (HIP) under the NEAMS program are summarized. Significantmore » progresses have been made regarding interatomic potential, phase field models for phase decomposition and gas bubble formation, and thermal conductivity for U3Si2 fuel, and precipitation in FeCrAl cladding. The accomplishments are very useful by providing atomistic and mesoscale tools, improving the current understanding, and delivering engineering scale models for these two ATF concepts.« less

Advances in the Development of a WCl6 CVD System for Coating UO2 Powders with Tungsten

NASA Technical Reports Server (NTRS)

Mireles, Omar R.; Tieman, Alyssa; Broadway, Jeramie; Hickman, Robert

2013-01-01

Demonstrated viability and utilization of: a) Fluidized powder bed. b) WCl6 CVD process. c) Coated spherical particles with tungsten. The highly corrosive nature of the WCl6 solid reagent limits material of construction. Indications that identifying optimized process variables with require substantial effort and will likely vary with changes in fuel requirements.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, Nicholas; Burns, Joseph R.

The aftermath of the Tōhoku earthquake and the Fukushima accident has led to a global push to improve the safety of existing light water reactors. A key component of this initiative is the development of nuclear fuel and cladding materials with potentially enhanced accident tolerance, also known as accident-tolerant fuels (ATF). These materials are intended to improve core fuel and cladding integrity under beyond design basis accident conditions while maintaining or enhancing reactor performance and safety characteristics during normal operation. To complement research that has already been carried out to characterize ATF neutronics, the present study provides an initial investigationmore » of the sensitivity and uncertainty of ATF systems responses to nuclear cross section data. ATF concepts incorporate novel materials, including SiC and FeCrAl cladding and high density uranium silicide composite fuels, in turn introducing new cross section sensitivities and uncertainties which may behave differently from traditional fuel and cladding materials. In this paper, we conducted sensitivity and uncertainty analysis using the TSUNAMI-2D sequence of SCALE with infinite lattice models of ATF assemblies. Of all the ATF materials considered, it is found that radiative capture in 56Fe in FeCrAl cladding is the most significant contributor to eigenvalue uncertainty. 56Fe yields significant potential eigenvalue uncertainty associated with its radiative capture cross section; this is by far the largest ATF-specific uncertainty found in these cases, exceeding even those of uranium. We found that while significant new sensitivities indeed arise, the general sensitivity behavior of ATF assemblies does not markedly differ from traditional UO2/zirconium-based fuel/cladding systems, especially with regard to uncertainties associated with uranium. We assessed the similarity of the IPEN/MB-01 reactor benchmark model to application models with FeCrAl cladding. We used TSUNAMI-IP to calculate similarity indices of the application model and IPEN/MB-01 reactor benchmark model. This benchmark was selected for its use of SS304 as a cladding and structural material, with significant 56Fe content. The similarity indices suggest that while many differences in reactor physics arise from differences in design, sensitivity to and behavior of 56Fe absorption is comparable between systems, thus indicating the potential for this benchmark to reduce uncertainties in 56Fe radiative capture cross sections.« less

A 100-kWt NaK-Cooled Space Reactor Concept for an Early-Flight Mission

NASA Astrophysics Data System (ADS)

Poston, David I.

2003-01-01

A stainless-steel (SS) sodium-potassium (NaK) cooled reactor could potentially be the first step in utilizing fission technology in space. The sum of all system-level experience for liquid-metal-cooled space reactors has been with NaK, including the SNAP-10a, the only reactor ever launched by the US. This paper describes a 100-kWt NaK reactor, the NaK-100, which is designed to be developed with minimal technical risk. In additional to NaK technology heritage, the NaK-100 uses a proven fuel-form (SS/UO2) and is designed for simplified system integration and testing. The pins are placed within a solid SS prism, and the NaK flows in an annulus between the pins and the prism. The nuclear and thermal-hydraulic performance of the NaK-100 is presented, as well as the major differences between the NaK-100 and SNAP-10a.

NEAMS Update. Quarterly Report for October - December 2011.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bradley, K.

2012-02-16

The Advanced Modeling and Simulation Office within the DOE Office of Nuclear Energy (NE) has been charged with revolutionizing the design tools used to build nuclear power plants during the next 10 years. To accomplish this, the DOE has brought together the national laboratories, U.S. universities, and the nuclear energy industry to establish the Nuclear Energy Advanced Modeling and Simulation (NEAMS) Program. The mission of NEAMS is to modernize computer modeling of nuclear energy systems and improve the fidelity and validity of modeling results using contemporary software environments and high-performance computers. NEAMS will create a set of engineering-level codes aimedmore » at designing and analyzing the performance and safety of nuclear power plants and reactor fuels. The truly predictive nature of these codes will be achieved by modeling the governing phenomena at the spatial and temporal scales that dominate the behavior. These codes will be executed within a simulation environment that orchestrates code integration with respect to spatial meshing, computational resources, and execution to give the user a common 'look and feel' for setting up problems and displaying results. NEAMS is building upon a suite of existing simulation tools, including those developed by the federal Scientific Discovery through Advanced Computing and Advanced Simulation and Computing programs. NEAMS also draws upon existing simulation tools for materials and nuclear systems, although many of these are limited in terms of scale, applicability, and portability (their ability to be integrated into contemporary software and hardware architectures). NEAMS investments have directly and indirectly supported additional NE research and development programs, including those devoted to waste repositories, safeguarded separations systems, and long-term storage of used nuclear fuel. NEAMS is organized into two broad efforts, each comprising four elements. The quarterly highlights October-December 2011 are: (1) Version 1.0 of AMP, the fuel assembly performance code, was tested on the JAGUAR supercomputer and released on November 1, 2011, a detailed discussion of this new simulation tool is given; (2) A coolant sub-channel model and a preliminary UO{sub 2} smeared-cracking model were implemented in BISON, the single-pin fuel code, more information on how these models were developed and benchmarked is given; (3) The Object Kinetic Monte Carlo model was implemented to account for nucleation events in meso-scale simulations and a discussion of the significance of this advance is given; (4) The SHARP neutronics module, PROTEUS, was expanded to be applicable to all types of reactors, and a discussion of the importance of PROTEUS is given; (5) A plan has been finalized for integrating the high-fidelity, three-dimensional reactor code SHARP with both the systems-level code RELAP7 and the fuel assembly code AMP. This is a new initiative; (6) Work began to evaluate the applicability of AMP to the problem of dry storage of used fuel and to define a relevant problem to test the applicability; (7) A code to obtain phonon spectra from the force-constant matrix for a crystalline lattice has been completed. This important bridge between subcontinuum and continuum phenomena is discussed; (8) Benchmarking was begun on the meso-scale, finite-element fuels code MARMOT to validate its new variable splitting algorithm; (9) A very computationally demanding simulation of diffusion-driven nucleation of new microstructural features has been completed. An explanation of the difficulty of this simulation is given; (10) Experiments were conducted with deformed steel to validate a crystal plasticity finite-element code for bodycentered cubic iron; (11) The Capability Transfer Roadmap was completed and published as an internal laboratory technical report; (12) The AMP fuel assembly code input generator was integrated into the NEAMS Integrated Computational Environment (NiCE). More details on the planned NEAMS computing environment is given; and (13) The NEAMS program website (neams.energy.gov) is nearly ready to launch.« less

Reactivity impact of {sup 16}O thermal elastic-scattering nuclear data for some numerical and critical benchmark systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kozier, K. S.; Roubtsov, D.; Plompen, A. J. M.

2012-07-01

The thermal neutron-elastic-scattering cross-section data for {sup 16}O used in various modern evaluated-nuclear-data libraries were reviewed and found to be generally too high compared with the best available experimental measurements. Some of the proposed revisions to the ENDF/B-VII.0 {sup 16}O data library and recent results from the TENDL system increase this discrepancy further. The reactivity impact of revising the {sup 16}O data downward to be consistent with the best measurements was tested using the JENDL-3.3 {sup 16}O cross-section values and was found to be very small in MCNP5 simulations of the UO{sub 2} and reactor-recycle MOX-fuel cases of the ANSmore » Doppler-defect numerical benchmark. However, large reactivity differences of up to about 14 mk (1400 pcm) were observed using {sup 16}O data files from several evaluated-nuclear-data libraries in MCNP5 simulations of the Los Alamos National Laboratory HEU heavy-water solution thermal critical experiments, which were performed in the 1950's. The latter result suggests that new measurements using HEU in a heavy-water-moderated critical facility, such as the ZED-2 zero-power reactor at the Chalk River Laboratories, might help to resolve the discrepancy between the {sup 16}O thermal elastic-scattering cross-section values and thereby reduce or better define its uncertainty, although additional assessment work would be needed to confirm this. (authors)« less

Joint tests at INL and CEA of a transient hot wire needle probe for in-pile thermal conductivity measurement

DOE Office of Scientific and Technical Information (OSTI.GOV)

Daw, J.E.; Knudson, D.L.; Villard, J.F.

2015-07-01

Thermal conductivity is a key property that must be known for proper design, testing, and deployment of new fuels and structural materials in nuclear reactors. Thermal conductivity is highly dependent on the physical structure, chemical composition, and the state of the material. Typically, thermal conductivity changes that occur during irradiation are currently measured out-of-pile using a 'cook and look' approach. But repeatedly removing samples from a test reactor to make measurements is expensive, has the potential to disturb phenomena of interest, and only provides understanding of the sample's end state when each measurement is made. There are also limited thermo-physicalmore » property data available for advanced fuels; and such data are needed for simulation codes, the development of next generation reactors, and advanced fuels for existing nuclear plants. Being able to quickly characterize fuel thermal conductivity during irradiation can improve the fidelity of data, reduce costs of post-irradiation examinations, increase understanding of how fuels behave under irradiation, and confirm or improve existing thermal conductivity measurement techniques. This paper discusses efforts to develop and evaluate an innovative in-pile thermal conductivity sensor based on the transient hot wire thermal conductivity method (THWM), using a single needle probe (NP) containing a line heat source and thermocouple embedded in the fuel. The sensor that has been designed and manufactured by the Idaho National Laboratory (INL) includes a unique combination of materials, geometry, and fabrication techniques that make the hot wire method suitable for in-pile applications. In particular, efforts were made to minimize the influence of the sensor and maximize fuel hot-wire heating. The probe has a thermocouple-like construction with high temperature resistant materials that remain ductile while resisting transmutation and materials interactions. THWM-NP prototypes were fabricated for both room temperature proof-of-concept evaluations and high temperature testing. Evaluations have been performed jointly by the INL and the French Alternative Energies and Atomic Energy Commission (CEA), both in Idaho Falls (USA) and in Cadarache (France), in the framework of a collaborative program for instrumentation of Material Testing Reactors. Initial tests were conducted on samples with a large range of thermal conductivities and temperatures ranging from 20 deg. C to 600 deg. C. Particularly, tests were recently performed on a sample having thermal conductivity and dimensions similar to UO{sub 2} and MOX nuclear fuels, in order to validate the ability of this sensor to operate for in-pile characterization of Light Water Reactors fuels. The results of the tests already completed at INL and CEA indicate that the Transient Hot Wire Needle Probe offers an enhanced method for in-pile detection of thermal conductivity. (authors)« less

UO(2) 2+ speciation determines uranium toxicity and bioaccumulation in an environmental Pseudomonas sp. isolate.

PubMed

Vanengelen, Michael R; Field, Erin K; Gerlach, Robin; Lee, Brady D; Apel, William A; Peyton, Brent M

2010-04-01

In the present study, experiments were performed to investigate how representative cellulosic breakdown products, when serving as growth substrates under aerobic conditions, affect hexavalent uranyl cation (UO(2) (2+)) toxicity and bioaccumulation within a Pseudomonas sp. isolate (designated isolate A). Isolate A taken from the Cold Test Pit South (CTPS) region of the Idaho National Laboratory (INL), Idaho Falls, ID, USA. The INL houses low-level uranium-contaminated cellulosic material and understanding how this material, and specifically its breakdown products, affect U-bacterial interactions is important for understanding UO(2) (2+) fate and mobility. Toxicity was modeled using a generalized Monod expression. Butyrate, dextrose, ethanol, and lactate served as growth substrates. The potential contribution of bicarbonate species present in high concentrations was also investigated and compared with toxicity and bioaccumulation patterns seen in low-bicarbonate conditions. Isolate A was significantly more sensitive to UO(2) (2+) and accumulated significantly more UO(2) (2+) in low-bicarbonate concentrations. In addition, UO(2) (2+) growth inhibition and bioaccumulation varied depending on the growth substrate. In the presence of high bicarbonate concentrations, sensitivity to UO(2) (2+) inhibition was greatly mitigated, and did not vary between the four substrates tested. The extent of UO(2) (2+) accumulation was also diminished. The observed patterns were related to UO(2) (2+) aqueous complexation, as predicted by MINTEQ (ver. 2.52) (Easton, PA, USA). In the low- bicarbonate medium, the presence of positively charged and unstable UO(2) (2+)-hydroxide complexes explained both the greater sensitivity of isolate A to UO(2) (2+), and the ability of isolate A to accumulate significant amounts of UO(2) (2+). The exclusive presence of negatively charged and stable UO(2) (2+)-carbonate complexes in the high bi-carbonate medium explained the diminished sensitivity of isolate A to UO(2) (2+) toxicity, and limited ability of isolate A to accumulate UO(2) (2+). (c) 2010 SETAC.

NEAMS update quarterly report for January - March 2012.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bradley, K.S.; Hayes, S.; Pointer, D.

Quarterly highlights are: (1) The integration of Denovo and AMP was demonstrated in an AMP simulation of the thermo-mechanics of a complete fuel assembly; (2) Bison was enhanced with a mechanistic fuel cracking model; (3) Mechanistic algorithms were incorporated into various lower-length-scale models to represent fission gases and dislocations in UO2 fuels; (4) Marmot was improved to allow faster testing of mesoscale models using larger problem domains; (5) Component models of reactor piping were developed for use in Relap-7; (6) The mesh generator of Proteus was updated to accept a mesh specification from Moose and equations were formulated for themore » intermediate-fidelity Proteus-2D1D module; (7) A new pressure solver was implemented in Nek5000 and demonstrated to work 2.5 times faster than the previous solver; (8) Work continued on volume-holdup models for two fuel reprocessing operations: voloxidation and dissolution; (9) Progress was made on a pyroprocessing model and the characterization of pyroprocessing emission signatures; (10) A new 1D groundwater waste transport code was delivered to the used fuel disposition (UFD) campaign; (11) Efforts on waste form modeling included empirical simulation of sodium-borosilicate glass compositions; (12) The Waste team developed three prototypes for modeling hydride reorientation in fuel cladding during very long-term fuel storage; (13) A benchmark demonstration problem (fission gas bubble growth) was modeled to evaluate the capabilities of different meso-scale numerical methods; (14) Work continued on a hierarchical up-scaling framework to model structural materials by directly coupling dislocation dynamics and crystal plasticity; (15) New 'importance sampling' methods were developed and demonstrated to reduce the computational cost of rare-event inference; (16) The survey and evaluation of existing data and knowledge bases was updated for NE-KAMS; (17) The NEAMS Early User Program was launched; (18) The Nuclear Regulatory Commission (NRC) Office of Regulatory Research was introduced to the NEAMS program; (19) The NEAMS overall software quality assurance plan (SQAP) was revised to version 1.5; and (20) Work continued on NiCE and its plug-ins and other utilities, such as Cubit and VisIt.« less

Molybdenum-UO2 cermet irradiation at 1145 K.

NASA Technical Reports Server (NTRS)

Mcdonald, G.

1971-01-01

Two molybdenum-uranium dioxide cermet fuel pins with molybdenum clad were fission-heated in a forced-convection helium coolant for sufficient time to achieve 5.3% burnup. The cermet core contained 20 wt % of 93.2% enriched uranium dioxide. The results were as follows: there was no visible change in the appearance of the molybdenum clad during irradiation; the maximum increase in diameter of the fuel pins was 0.8%; there was no migration of uranium dioxide along grain boundaries and no evident interaction between molybdenum and uranium dioxide; and, finally, approximately 12% of the fission gas formed was released from the cermet core into the gas plenum.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yamashita, T.; Fujino, T.; Masaki, N.

The structural parameters of ..cap alpha..- and ..beta..-CdUO/sub 4/ crystals are determined by x-ray powder diffraction technique. ..cap alpha..-CdUO/sub 4/ is rhombohedral and cell parameters are a = 6.233(3) A and ..cap alpha.. = 36.12(5)/sup 0/. ..beta..-CdUO/sub 4/ crystallizes in a C-centered orthorhombic cell with a = 7.023(4), b = 6.849(3), c = 3.514(2) A. The space groups are R3m for ..cap alpha..-CdUO/sub 4/ and Cmmm for ..beta..-CdUO/sub 4/. ..cap alpha..-CdUO/sub 4/: 1U in (000), 1Cd in (1/2 1/2 1/2), 2O(1) in +-(uuu), 2O(2) in +-(vvv); u = 0.113, v= 0.350, Z = 1. ..beta..-CdUO/sub 4/: 2U in (000; 1/2more » 1/2 0), 2Cd in (1/2 0 1/2; 0 1/2 1/2), 40(1) in (0, +-y, 0; 1/2, 1/2 +-y, 0), 4O(2) in (+-x, 0, 1/2; 1/2 +-x, 1/2, 1/2); x = 0.159, y = 0.278, Z = 2. ..beta..-CdUO/sub 4/ contains collinear uranyl UO/sub 2//sup 2 +/ groups with a U-O(1) distance of 1.91 A, located either along or parallel to the c axis whereas the U-O(1) bond length in ..cap alpha..-CdUO/sub 4/ is 1.98 A which is longer than the usual uranyl bond length.« less

High resolution photoelectron imaging of UO(-) and UO2(-) and the low-lying electronic states and vibrational frequencies of UO and UO2.

PubMed

Czekner, Joseph; Lopez, Gary V; Wang, Lai-Sheng

2014-12-28

We report a study of the electronic and vibrational structures of the gaseous uranium monoxide and dioxide molecules using high-resolution photoelectron imaging. Vibrationally resolved photoelectron spectra are obtained for both UO(-) and UO2(-). The spectra for UO2(-) are consistent with, but much better resolved than a recent study using a magnetic-bottle photoelectron analyzer [W. L. Li et al., J. Chem. Phys. 140, 094306 (2014)]. The electron affinity (EA) of UO is reported for the first time as 1.1407(7) eV, whereas a much more accurate EA is obtained for UO2 as 1.1688(6) eV. The symmetric stretching modes for the neutral and anionic ground states, and two neutral excited states for UO2 are observed, as well as the bending mode for the neutral ground state. These vibrational frequencies are consistent with previous experimental and theoretical results. The stretching vibrational modes for the ground state and one excited state are observed for UO. The current results for UO and UO2 are compared with previous theoretical calculations including relativistic effects and spin-orbit coupling. The accurate experimental data reported here provide more stringent tests for future theoretical methods for actinide-containing species.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jolly, Brian C.; Lindemer, Terrence; Terrani, Kurt A.

In support of fully ceramic matrix (FCM) fuel development, coating development work has begun at the Oak Ridge National Laboratory (ORNL) to produce tri-isotropic (TRISO) coated fuel particles with UN kernels. The nitride kernels are used to increase heavy metal density in these SiC-matrix fuel pellets with details described elsewhere. The advanced gas reactor (AGR) program at ORNL used fluidized bed chemical vapor deposition (FBCVD) techniques for TRISO coating of UCO (two phase mixture of UO 2 and UC x) kernels. Similar techniques were employed for coating of the UN kernels, however significant changes in processing conditions were required tomore » maintain acceptable coating properties due to physical property and dimensional differences between the UCO and UN kernels.« less

Enhancing the ABAQUS thermomechanics code to simulate multipellet steady and transient LWR fuel rod behavior

DOE Office of Scientific and Technical Information (OSTI.GOV)

R. L. Williamson

A powerful multidimensional fuels performance analysis capability, applicable to both steady and transient fuel behavior, is developed based on enhancements to the commercially available ABAQUS general-purpose thermomechanics code. Enhanced capabilities are described, including: UO2 temperature and burnup dependent thermal properties, solid and gaseous fission product swelling, fuel densification, fission gas release, cladding thermal and irradiation creep, cladding irradiation growth, gap heat transfer, and gap/plenum gas behavior during irradiation. This new capability is demonstrated using a 2D axisymmetric analysis of the upper section of a simplified multipellet fuel rod, during both steady and transient operation. Comparisons are made between discrete andmore » smeared-pellet simulations. Computational results demonstrate the importance of a multidimensional, multipellet, fully-coupled thermomechanical approach. Interestingly, many of the inherent deficiencies in existing fuel performance codes (e.g., 1D thermomechanics, loose thermomechanical coupling, separate steady and transient analysis, cumbersome pre- and post-processing) are, in fact, ABAQUS strengths.« less

Uranium(IV) adsorption by natural organic matter in anoxic sediments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bone, Sharon E.; Dynes, James J.; Cliff, John

2017-01-09

Uranium is an important fuel source and a global environmental contaminant. It accumulates in the tetravalent state, U(IV), in anoxic sediments, including ore deposits, marine basins, and contaminated aquifers. However, very little is known about the speciation of U(IV) in low temperature geochemical environments, inhibiting the development of a conceptual model of U behavior. Until recently, U(IV) was assumed to exist predominantly as the sparingly soluble mineral uraninite (UO 2) in anoxic sediments; yet studies now show that UO 2 is not often dominant in these environments. However, a model of U(IV) speciation under environmentally relevant conditions has not yetmore » been developed. Here we show that complexes of U(IV) adsorb on organic carbon and organic carbon-coated clays in an organic-rich natural substrate under field-relevant conditions. Whereas previous research assumed that the U(IV) product depended on the reduction pathway, our results demonstrate that UO 2 formation can be inhibited simply by decreasing the U:solid ratio. Thus, it is the number and type of surface ligands that controls U(IV) speciation subsequent to U(VI) reduction. Projections of U transport and bioavailability, and thus its threat to human and ecosystem health, must consider retention of U(IV) ions within the local sediment environment.« less

Structure, equilibrium and ligand exchange dynamics in the binary and ternary dioxouranium(VI)-ethylenediamine-N,N'-diacetic acid-fluoride system: A potentiometric, NMR and X-ray crystallographic study.

PubMed

Palladino, Giuseppe; Szabó, Zoltán; Fischer, Andreas; Grenthe, Ingmar

2006-11-21

The structure, thermodynamics and kinetics of the binary and ternary uranium(VI)-ethylenediamine-N,N'-diacetate (in the following denoted EDDA) fluoride systems have been studied using potentiometry, 1H, 19F NMR spectroscopy and X-ray diffraction. The UO2(2+)-EDDA system could be studied up to -log[H3O+] = 3.4 where the formation of two binary complexes UO2(EDDA)(aq) and UO2(H3EDDA)3+ were identified, with equilibrium constants logbeta(UO2EDDA) = 11.63 +/- 0.02 and logbeta(UO2H3EDDA3+) = 1.77 +/- 0.04, respectively. In the ternary system the complexes UO2(EDDA)F-, UO2(EDDA)(OH)- and (UO2)2(mu-OH)2(HEDDA)2F2(aq) were identified; the latter through 19F NMR. 1H NMR spectra indicate that the EDDA ligand is chelate bonded in UO2(EDDA)(aq), UO2(EDDA)F- and UO2(EDDA)(OH)- while only one carboxylate group is coordinated in UO2(H3EDDA)3+. The rate and mechanism of the fluoride exchange between UO2(EDDA)F- and free fluoride was studied by 19F NMR spectroscopy. Three reactions contribute to the exchange; (i) site exchange between UO2(EDDA)F- and free fluoride without any net chemical exchange, (ii) replacement of the coordinated fluoride with OH- and (iii) the self dissociation of the coordinated fluoride forming UO2(EDDA)(aq); these reactions seem to follow associative mechanisms. (1)H NMR spectra show that the exchange between the free and chelate bonded EDDA is slow and consists of several steps, protonation/deprotonation and chelate ring opening/ring closure, the mechanism cannot be elucidated from the available data. The structure (UO2)2(EDDA)2(mu-H2EDDA) was determined by single crystal X-ray diffraction and contains two UO2(EDDA) units with tetracoordinated EDDA linked by H2EDDA in the "zwitterion" form, coordinated through a single carboxylate oxygen from each end to the two uranium atoms. The geometry of the complexes indicates that there is no geometric constraint for an associative ligand substitution mechanism.

Dissolution of Biogenic and Synthetic UO2 under Varied Reducing Conditions

PubMed Central

ULRICH, KAI – UWE; SINGH, ABHAS; SCHOFIELD, ELEANOR J.; BARGAR, JOHN R.; VEERAMANI, HARISH; SHARP, JONATHAN O.; LATMANI, RIZLAN BERNIER -; GIAMMAR, DANIEL E.

2008-01-01

The chemical stability of biogenic UO2, a nanoparticulate product of environmental bioremediation, may be impacted by the particles’ surface free energy, structural defects, and compositional variability in analogy to abiotic UO2+x (0 ≤ x ≤ 0.25). This study quantifies and compares intrinsic solubility and dissolution rate constants of biogenic nano-UO2 and synthetic bulk UO2.00, taking molecular-scale structure into account. Rates were determined under anoxic conditions as a function of pH and dissolved inorganic carbon in continuous-flow experiments. The dissolution rates of biogenic and synthetic UO2 solids were lowest at near neutral pH and increased with decreasing pH. Similar surface area-normalized rates of biogenic and synthetic UO2 suggest comparable reactive surface site densities. This finding is consistent with the identified structural homology of biogenic UO2 and stoichiometric UO2.00. Compared to carbonate-free anoxic conditions, dissolved inorganic carbon accelerated the dissolution rate of biogenic UO2 by 3 orders of magnitude. This phenomenon suggests continuous surface oxidation of U(IV) to U(VI), with detachment of U(VI) as the rate-determining step in dissolution. Although reducing conditions were maintained throughout the experiments, the UO2 surface can be oxidized by water and radiogenic oxidants. Even in anoxic aquifers, UO2 dissolution may be controlled by surface U(VI) rather than U(IV) phases. PMID:18754482

Versatile Oxide Films Protect FeCrAl Alloys Under Normal Operation and Accident Conditions in Light Water Power Reactors

NASA Astrophysics Data System (ADS)

Rebak, Raul B.

2018-02-01

The US has currently a fleet of 99 nuclear power light water reactors which generate approximately 20% of the electricity consumed in the country. Near 90% of the reactors are at least 30 years old. There are incentives to make the existing reactors safer by using accident tolerant fuels (ATF). Compared to the standard UO2-zirconium-based system, ATF need to tolerate loss of active cooling in the core for a considerably longer time while maintaining or improving the fuel performance during normal operation conditions. Ferritic iron-chromium-aluminum (FeCrAl) alloys have been identified as an alternative to replace current zirconium alloys. They contain Fe (base) + 10-22 Cr + 4-6 Al and may contain smaller amounts of other elements such as molybdenum and traces of others. FeCrAl alloys offer outstanding resistance to attack by superheated steam by developing an alumina oxide on the surface in case of a loss of coolant accident like at Fukushima. FeCrAl alloys also perform well under normal operation conditions both in boiling water reactors and pressurized water reactors because they are protected by a thin oxide rich in chromium. Under normal operation condition, the key element is Cr and under accident conditions it is Al.

CRITICAL EXPERIMENT WITH BORAX-V. Internal Superheater

DOE Office of Scientific and Technical Information (OSTI.GOV)

Plumlee, K.E.; Baird, Q.L.; Stanford, G.S.

1963-11-01

A critical experiment was performed with 12 BORAX-V superheater subassemblies in a central voidable region plus 1228 to 1525 UO/sub 2/ fuel pins (3 wt% enriched) in a peripheral region. Removing water (28% of superheater volume) at room temperature decreased reactivity by 2.2%. The midplane (two- dimensional) peak-to-average power distribution in the voided superheater was approximately 1.24, mostly attributable to flux depressions within insulated fuel boxes. Cadmium ratios are also reported. The experiment was initiated to supplement computational information which might have affected plans for loading the superheater zone into the BORAX-V reactor. No changes were indicated by the experiment.more » (auth)« less

Dissolution experiments of commercial PWR (52 MWd/kgU) and BWR (53 MWd/kgU) spent nuclear fuel cladded segments in bicarbonate water under oxidizing conditions. Experimental determination of matrix and instant release fraction

NASA Astrophysics Data System (ADS)

González-Robles, E.; Serrano-Purroy, D.; Sureda, R.; Casas, I.; de Pablo, J.

2015-10-01

The denominated instant release fraction (IRF) is considered in performance assessment (PA) exercises to govern the dose that could arise from the repository. A conservative definition of IRF comprises the total inventory of radionuclides located in the gap, fractures, and the grain boundaries and, if present, in the high burn-up structure (HBS). The values calculated from this theoretical approach correspond to an upper limit that likely does not correspond to what it will be expected to be instantaneously released in the real system. Trying to ascertain this IRF from an experimental point of view, static leaching experiments have been carried out with two commercial UO2 spent nuclear fuels (SNF): one from a pressurized water reactor (PWR), labelled PWR, with an average burn-up (BU) of 52 MWd/kgU and fission gas release (FGR) of 23.1%, and one from a boiling water reactor (BWR), labelled BWR, with an average BU of and 53 MWd/kgU and FGR of 3.9%. One sample of each SNF, consisting of fuel and cladding, has been leached in bicarbonate water during one year under oxidizing conditions at room temperature (25 ± 5)°C. The behaviour of the concentration measured in solution can be divided in two according to the release rate. All radionuclides presented an initial release rate that after some days levels down to a slower second one, which remains constant until the end of the experiment. Cumulative fraction of inventory in aqueous phase (FIAPc) values has been calculated. Results show faster release in the case of the PWR SNF. In both cases Np, Pu, Am, Cm, Y, Tc, La and Nd dissolve congruently with U, while dissolution of Zr, Ru and Rh is slower. Rb, Sr, Cs and Mo, dissolve faster than U. The IRF of Cs at 10 and 200 days has been calculated, being (3.10 ± 0.62) and (3.66 ± 0.73) for PWR fuel, and (0.35 ± 0.07) and (0.51 ± 0.10) for BWR fuel.

Progress in understanding fission-product behaviour in coated uranium-dioxide fuel particles

NASA Astrophysics Data System (ADS)

Barrachin, M.; Dubourg, R.; Kissane, M. P.; Ozrin, V.

2009-03-01

Supported by results of calculations performed with two analytical tools (MFPR, which takes account of physical and chemical mechanisms in calculating the chemical forms and physical locations of fission products in UO2, and MEPHISTA, a thermodynamic database), this paper presents an investigation of some important aspects of the fuel microstructure and chemical evolutions of irradiated TRISO particles. The following main conclusions can be identified with respect to irradiated TRISO fuel: first, the relatively low oxygen potential within the fuel particles with respect to PWR fuel leads to chemical speciation that is not typical of PWR fuels, e.g., the relatively volatile behaviour of barium; secondly, the safety-critical fission-product caesium is released from the urania kernel but the buffer and pyrolytic-carbon coatings could form an important chemical barrier to further migration (i.e., formation of carbides). Finally, significant releases of fission gases from the urania kernel are expected even in nominal conditions.

Local structure and charge distribution in the UO(2)-U(4)O(9) system.

PubMed

Conradson, Steven D; Manara, Dario; Wastin, Franck; Clark, David L; Lander, Gerard H; Morales, Luis A; Rebizant, Jean; Rondinella, Vincenzo V

2004-11-01

Analysis of X-ray absorption fine structure spectra of UO(2+x) for x = 0-0.20 (UO(2)--U(4)O(9)) reveals that the adventitious O atoms are incorporated as oxo groups with U--O distances of 1.74 A, most likely associated with U(VI), that occur in clusters so that the UO(2) fraction of the material largely remains intact. In addition to the formation of some additional longer U--O bonds, the U sublattice consists of an ordered portion that displays the original U--U distance and a spectroscopically silent, glassy part. This is very different from previous models derived from neutron diffraction that maintained long U--O distances and high U--O coordination numbers. UO(2+x) also differs from PuO(2+x) in its substantially shorter An-oxo distances and no sign of stable coordination with H(2)O and its hydrolysis products.

Irradiation of TZM: Uranium dioxide fuel pin at 1700 K

NASA Technical Reports Server (NTRS)

Mcdonald, G. E.

1973-01-01

A fuel pin clad with TZM and containing solid pellets of uranium dioxide was fission heated in a static helium-cooled capsule at a maximum surface temperature of 1700 K for approximately 1000 hr and to a total burnup of 2.0 percent of the uranium-235. The results of the postirradiation examination indicated: (1) A transverse, intergranular failure of the fuel pin occurred when the fuel pin reached 2.0-percent burnup. This corresponds to 1330 kW-hr/cu cm, where the volume is the sum of the fuel, clad, and void volumes in the fuel region. (2) The maximum swelling of the fuel pin was less than 1.5 percent on the fuel-pin diameter. (3) There was no visible interaction between the TZM clad and the UO2. (4) Irradiation at 1700 K produced a course-grained structure, with an average grain diameter of 0.02 centimeter and with some of the grains extending one-half of the thickness of the clad. (5) Below approximately 1500 K, the irradiation of the clad produced a moderately fine-grained structure, with an average grain diameter of 0.004 centimeter.

Excision of uranium oxide chains and ribbons in the novel one-dimensional uranyl iodates K(2)[(UO(2))3(IO(3))(4)O(2)] and Ba[(UO(2)2(IO(3))(2)O(2)](H(2)O).

PubMed

Bean, A C; Ruf, M; Albrecht-Schmitt, T E

2001-07-30

The alkali metal and alkaline-earth metal uranyl iodates K(2)[(UO(2))(3)(IO(3))(4)O(2)] and Ba[(UO(2))(2)(IO(3))(2)O(2)](H(2)O) have been prepared from the hydrothermal reactions of KCl or BaCl(2) with UO(3) and I(2)O(5) at 425 and 180 degrees C, respectively. While K(2)[(UO(2))(3)(IO(3))(4)O(2)] can be synthesized under both mild and supercritical conditions, the yield increases from <5% to 73% as the temperature is raised from 180 to 425 degrees C. Ba[(UO(2))(2)(IO(3))(2)O(2)](H(2)O), however, has only been isolated from reactions performed in the mild temperature regime. Thermal measurements (DSC) indicate that K(2)[(UO(2))(3)(IO(3))(4)O(2)] is more stable than Ba[(UO(2))(2)(IO(3))(2)O(2)](H(2)O) and that both compounds decompose through thermal disproportionation at 579 and 575 degrees C, respectively. The difference in the thermal behavior of these compounds provides a basis for the divergence of their preparation temperatures. The structure of K(2)[(UO(2))(3)(IO(3))(4)O(2)] is composed of [(UO(2))(3)(IO(3))(4)O(2)](2)(-) chains built from the edge-sharing UO(7) pentagonal bipyramids and UO(6) octahedra. Ba[(UO(2))(2)(IO(3))(2)O(2)](H(2)O) consists of one-dimensional [(UO(2))(2)(IO(3))(2)O(2)](2)(-) ribbons formed from the edge sharing of distorted UO(7) pentagonal bipyramids. In both compounds the iodate groups occur in both bridging and monodentate binding modes and further serve to terminate the edges of the uranium oxide chains. The K(+) or Ba(2+) cations separate the chains or ribbons in these compounds forming bonds with terminal oxygen atoms from the iodate ligands. Crystallographic data: K(2)[(UO(2))(3)(IO(3))(4)O(2)], triclinic, space group P_1, a = 7.0372(5) A, b = 7.7727(5) A, c = 8.9851(6) A, alpha = 93.386(1) degrees, beta = 105.668(1) degrees, gamma = 91.339(1) degrees, Z = 1; Ba[(UO(2))(2)(IO(3))(2)O(2)](H(2)O), monoclinic, space group P2(1)/c, a = 8.062(4) A, b = 6.940(3) A, c = 21.67(1), beta= 98.05(1) degrees, Z = 4.

Topological analysis of void spaces in tungstate frameworks: Assessing storage properties for the environmentally important guest molecules and ions: CO 2, UO 2, PuO 2, U, Pu, Sr 2+, Cs +, CH 4, and H 2

DOE PAGES

Cole, Jacqueline M.; Cramer, Alisha J.; Zeidler, Anita

2015-07-15

The identification of inorganic materials, which are able to encapsulate environmentally important small molecules or ions via host-guest interactions, is crucial for the design and development of next-generation energy sources and for storing environmental waste. Especially sought after are molecular sponges with the ability to incorporate CO 2, gas pollutants, or nuclear waste materials such as UO 2 and PuO 2 oxides or U, Pu, Sr 2+ or Cs + ions. Porous framework structures promise very attractive prospects for applications in environmental technologies, if they are able to incorporate CH 4 for biogas energy applications, or to store H 2,more » which is important for fuel cells e.g. in the automotive industry. All of these applications should benefit from the host being resistant to extreme conditions such as heat, nuclear radiation, rapid gas expansion, or wear and tear from heavy gas cycling. As inorganic tungstates are well known for their thermal stability, and their rigid open-framework networks, the potential of Na 2O-Al 2O 3-WO 3 and Na 2O-WO 3 phases for such applications was evaluated. To this end, all known experimentally-determined crystal structures with the stoichiometric formula M aM’ bW cO d (M = any element) are surveyed together with all corresponding theoretically calculated Na aAl bW cO d and Na xW yO z structures that are statistically likely to form. Network descriptors that categorize these host structures are used to reveal topological patterns in the hosts, including the nature of porous cages which are able to accommodate a certain type of guest; this leads to the classification of preferential structure types for a given environmental storage application. Crystal structures of two new tungstates NaAlW 2O 8 (1) and NaAlW 3O 11 (2) and one updated structure determination of Na 2W 2O 7 (3) are also presented from in-house X-ray diffraction studies, and their potential merits for environmental applications are assessed against those of this larger data-sourced survey. Altogether, results show that tungstate structures with three-nodal topologies are most frequently able to accommodate CH 4 or H 2, while CO 2 appears to be captured by a wide range of nodal structure types. The computationally generated host structures appear systematically smaller than the experimentally determined structures. For the structures of 1 and 2, potential applications in nuclear waste storage seem feasible.« less

Comparisons of sodium void and Doppler reactivities in large oxide and carbide LMFBRs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Su, S F

Sodium void and Doppler reactivities in two full scale (3000 MWth) LMFBRs are analyzed; one is fueled with UO/sub 2/ - PuO/sub 2/ and the other is fueled with UC - PuC. These two reactors are analyzed for beginning of life as well as for beginning and end of equilibrium cycle conditions, and the variations of these two safety parameters with burnup are explained. A series of comperative analyses of these two and several hypothetical reactors are carried out to determine how differences in fuel type, sodium content, and heavy metal concentration between an oxide and a carbide reactor affectmore » their sodium void and Doppler reactivities. The effect of the presence of conrol poison on sodium void reactivity is also addressed.« less

Triso coating development progress for uranium nitride kernels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jolly, Brian C.; Lindemer, Terrence; Terrani, Kurt A.

2015-08-01

In support of fully ceramic matrix (FCM) fuel development [1-2], coating development work is ongoing at the Oak Ridge National Laboratory (ORNL) to produce tri-structural isotropic (TRISO) coated fuel particles with UN kernels [3]. The nitride kernels are used to increase fissile density in these SiC-matrix fuel pellets with details described elsewhere [4]. The advanced gas reactor (AGR) program at ORNL used fluidized bed chemical vapor deposition (FBCVD) techniques for TRISO coating of UCO (two phase mixture of UO2 and UCx) kernels [5]. Similar techniques were employed for coating of the UN kernels, however significant changes in processing conditions weremore » required to maintain acceptable coating properties due to physical property and dimensional differences between the UCO and UN kernels (Table 1).« less

A thermodynamic approach for advanced fuels of gas-cooled reactors

NASA Astrophysics Data System (ADS)

Guéneau, C.; Chatain, S.; Gossé, S.; Rado, C.; Rapaud, O.; Lechelle, J.; Dumas, J. C.; Chatillon, C.

2005-09-01

For both high temperature reactor (HTR) and gas cooled fast reactor (GFR) systems, the high operating temperature in normal and accidental conditions necessitates the assessment of the thermodynamic data and associated phase diagrams for the complex system constituted of the fuel kernel, the inert materials and the fission products. A classical CALPHAD approach, coupling experiments and thermodynamic calculations, is proposed. Some examples of studies are presented leading with the CO and CO 2 gas formation during the chemical interaction of [UO 2± x/C] in the HTR particle, and the chemical compatibility of the couples [UN/SiC], [(U, Pu)N/SiC], [(U, Pu)N/TiN] for the GFR system. A project of constitution of a thermodynamic database for advanced fuels of gas-cooled reactors is proposed.

Nuclear proliferomics: A new field of study to identify signatures of nuclear materials as demonstrated on alpha-UO3.

PubMed

Schwerdt, Ian J; Brenkmann, Alexandria; Martinson, Sean; Albrecht, Brent D; Heffernan, Sean; Klosterman, Michael R; Kirkham, Trenton; Tasdizen, Tolga; McDonald Iv, Luther W

2018-08-15

The use of a limited set of signatures in nuclear forensics and nuclear safeguards may reduce the discriminating power for identifying unknown nuclear materials, or for verifying processing at existing facilities. Nuclear proliferomics is a proposed new field of study that advocates for the acquisition of large databases of nuclear material properties from a variety of analytical techniques. As demonstrated on a common uranium trioxide polymorph, α-UO 3 , in this paper, nuclear proliferomics increases the ability to improve confidence in identifying the processing history of nuclear materials. Specifically, α-UO 3 was investigated from the calcination of unwashed uranyl peroxide at 350, 400, 450, 500, and 550 °C in air. Scanning electron microscopy (SEM) images were acquired of the surface morphology, and distinct qualitative differences are presented between unwashed and washed uranyl peroxide, as well as the calcination products from the unwashed uranyl peroxide at the investigated temperatures. Differential scanning calorimetry (DSC), UV-Vis spectrophotometry, powder X-ray diffraction (p-XRD), and thermogravimetric analysis-mass spectrometry (TGA-MS) were used to understand the source of these morphological differences as a function of calcination temperature. Additionally, the SEM images were manually segmented using Morphological Analysis for MAterials (MAMA) software to identify quantifiable differences in morphology for three different surface features present on the unwashed uranyl peroxide calcination products. No single quantifiable signature was sufficient to discern all calcination temperatures with a high degree of confidence; therefore, advanced statistical analysis was performed to allow the combination of a number of quantitative signatures, with their associated uncertainties, to allow for complete discernment by calcination history. Furthermore, machine learning was applied to the acquired SEM images to demonstrate automated discernment with at least 89% accuracy. Copyright © 2018 Elsevier B.V. All rights reserved.

10 CFR 2.1105 - Definitions.

Code of Federal Regulations, 2014 CFR

2014-01-01

... Nuclear Fuel Storage Capacity at Civilian Nuclear Power Reactors § 2.1105 Definitions. As used in this part: (a) Civilian nuclear power reactor means a civilian nuclear power plant required to be licensed... nuclear fuel means fuel that has been withdrawn from a nuclear reactor following irradiation, the...

10 CFR 2.1105 - Definitions.

Code of Federal Regulations, 2013 CFR

2013-01-01

... Nuclear Fuel Storage Capacity at Civilian Nuclear Power Reactors § 2.1105 Definitions. As used in this part: (a) Civilian nuclear power reactor means a civilian nuclear power plant required to be licensed... nuclear fuel means fuel that has been withdrawn from a nuclear reactor following irradiation, the...

High resolution photoelectron imaging of UO{sup −} and UO{sub 2}{sup −} and the low-lying electronic states and vibrational frequencies of UO and UO{sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Czekner, Joseph; Lopez, Gary V.; Wang, Lai-Sheng

2014-12-28

We report a study of the electronic and vibrational structures of the gaseous uranium monoxide and dioxide molecules using high-resolution photoelectron imaging. Vibrationally resolved photoelectron spectra are obtained for both UO{sup −} and UO{sub 2}{sup −}. The spectra for UO{sub 2}{sup −} are consistent with, but much better resolved than a recent study using a magnetic-bottle photoelectron analyzer [W. L. Li et al., J. Chem. Phys. 140, 094306 (2014)]. The electron affinity (EA) of UO is reported for the first time as 1.1407(7) eV, whereas a much more accurate EA is obtained for UO{sub 2} as 1.1688(6) eV. The symmetricmore » stretching modes for the neutral and anionic ground states, and two neutral excited states for UO{sub 2} are observed, as well as the bending mode for the neutral ground state. These vibrational frequencies are consistent with previous experimental and theoretical results. The stretching vibrational modes for the ground state and one excited state are observed for UO. The current results for UO and UO{sub 2} are compared with previous theoretical calculations including relativistic effects and spin-orbit coupling. The accurate experimental data reported here provide more stringent tests for future theoretical methods for actinide-containing species.« less

The crystal structures of α- and β-CdUO 4

NASA Astrophysics Data System (ADS)

Yamashita, Toshiyuki; Fujino, Takeo; Masaki, Norio; Tagawa, Hiroaki

1981-04-01

The structural parameters of α- and β-CdUO 4 crystals are determined by X-ray powder diffraction technique. α-CdUO 4 is rhombohedral and cell parameters are a = 6.233(3) Å and α = 36.12(5)°. β-CdUO 4 crystallizes in a C-centered orthorhombic cell with a = 7.023(4), b = 6.849(3), c = 3.514 (2) Å. The space groups are R overline3m for α-CdUO 4 and Cmmm for β-CdUO 4. α-CdUO 4: 1U in (000), 1Cd in ( {1}/{2}{1}/{2}{1}/{2}), 2O(1) in ±( uuu), 2O(2) in ±( vvv); u = 0.113, v = 0.350, Z = 1. β-CdUO 4: 2U in ( 000; {1}/{2}{1}/{2} 0 ), 2Cd in ( {1}/{2} 0 {1}/{2}; 0 {1}/{2}, {1}/{2}), 4O(1) in ( 0, ±y, 0; {1}/{2}, {1}/{2} ±y, 0 ), 4O(2) in ( ±x, 0, {1}/{2}; {1}/{2} ±x, {1}/{2}, {1}/{2}); x = 0.159, y = 0.278, Z = 2. β-CdUO 4 contains collinear uranyl UO 2+2 groups with a UO(1) distance of 1.91 Å, located either along or parallel to the c axis whereas the UO(1) bond length in α-CdUO 4 is 1.98 Å which is longer than the usual uranyl bond length.

Promises and Challenges of Thorium Implementation for Transuranic Transmutation - 13550

DOE Office of Scientific and Technical Information (OSTI.GOV)

Franceschini, F.; Lahoda, E.; Wenner, M.

2013-07-01

This paper focuses on the challenges of implementing a thorium fuel cycle for recycle and transmutation of long-lived actinide components from used nuclear fuel. A multi-stage reactor system is proposed; the first stage consists of current UO{sub 2} once-through LWRs supplying transuranic isotopes that are continuously recycled and burned in second stage reactors in either a uranium (U) or thorium (Th) carrier. The second stage reactors considered for the analysis are Reduced Moderation Pressurized Water Reactors (RMPWRs), reconfigured from current PWR core designs, and Fast Reactors (FRs) with a burner core design. While both RMPWRs and FRs can in principlemore » be employed, each reactor and associated technology has pros and cons. FRs have unmatched flexibility and transmutation efficiency. RMPWRs have higher fuel manufacturing and reprocessing requirements, but may represent a cheaper solution and the opportunity for a shorter time to licensing and deployment. All options require substantial developments in manufacturing, due to the high radiation field, and reprocessing, due to the very high actinide recovery ratio to elicit the claimed radiotoxicity reduction. Th reduces the number of transmutation reactors, and is required to enable a viable RMPWR design, but presents additional challenges on manufacturing and reprocessing. The tradeoff between the various options does not make the choice obvious. Moreover, without an overarching supporting policy in place, the costly and challenging technologies required inherently discourage industrialization of any transmutation scheme, regardless of the adoption of U or Th. (authors)« less

Affordable Development and Demonstration of a Small NTR Engine and Stage: A Preliminary NASA, DOE, and Industry Assessment

NASA Technical Reports Server (NTRS)

Borowski, Stanley K.; Sefcik, Robert J.; Fittje, James E.; McCurdy, David R.; Qualls, Arthur L.; Schnitzler, Bruce G.; Werner, James E.; Weitzberg, Abraham; Joyner, Claude R.

2015-01-01

The Nuclear Thermal Rocket (NTR) represents the next evolutionary step in cryogenic liquid rocket engines. Deriving its energy from fission of uranium-235 atoms contained within fuel elements that comprise the engine's reactor core, the NTR can generate high thrust at a specific impulse of approx. 900 seconds or more - twice that of today's best chemical rockets. In FY'11, as part of the AISP project, NASA proposed a Nuclear Thermal Propulsion (NTP) effort that envisioned two key activities - "Foundational Technology Development" followed by system-level "Technology Demonstrations". Five near-term NTP activities identified for Foundational Technology Development became the basis for the NCPS project started in FY'12 and funded by NASA's AES program. During Phase 1 (FY'12-14), the NCPS project was focused on (1) Recapturing fuel processing techniques and fabricating partial length "heritage" fuel elements for the two candidate fuel forms identified by NASA and the DOE - NERVA graphite "composite" and the uranium dioxide (UO2) in tungsten "cermet". The Phase 1 effort also included: (2) Engine Conceptual Design; (3) Mission Analysis and Requirements Definition; (4) Identification of Affordable Options for Ground Testing; and (5) Formulation of an Affordable and Sustainable NTP Development Strategy. During FY'14, a preliminary plan for DDT&E was outlined by GRC, the DOE and industry for NASA HQ that involved significant system-level demonstration projects that included GTD tests at the NNSS, followed by a FTD mission. To reduce development costs, the GTD and FTD tests use a small, low thrust (approx. 7.5 or 16.5 klbf) engine. Both engines use graphite composite fuel and a "common" fuel element design that is scalable to higher thrust (approx. 25 klbf) engines by increasing the number of elements in a larger diameter core that can produce greater thermal power output. To keep the FTD mission cost down, a simple "1-burn" lunar flyby mission was considered along with maximizing the use of existing and flight proven liquid rocket and stage hardware (e.g., from the RL10-B2 engine and Delta Cryogenic Second Stage) to further ensure affordability. This paper provides a preliminary NASA, DOE and industry assessment of what is required - the key DDT&E activities, development options, and the associated schedule - to affordably build, ground test and fly a small NTR engine and stage within a 10-year timeframe.

METHOD FOR PREPARATION OF UO$sub 2$ PARTICLES

DOEpatents

Johnson, J.R.; Taylor, A.J.

1959-09-22

A method is described for the preparation of highdensity UO/sub 2/ particles within the size range of 40 to 100 microns. In accordance with the invention UO/sub 2/ particles are autoclaved with an aqueous solution of uranyl ions. The resulting crystals are reduced to UO/sub 2/ and the UO/sub 2/ is heated to at least 1000 deg C to effect densification. The resulting UO/sub 2/ particles are screened, and oversize particles are crushed and screened to recover the particles within the desired size range.

Thermodynamics of formation of coffinite, USiO4

PubMed Central

Guo, Xiaofeng; Szenknect, Stéphanie; Mesbah, Adel; Labs, Sabrina; Clavier, Nicolas; Poinssot, Christophe; Ushakov, Sergey V.; Curtius, Hildegard; Bosbach, Dirk; Ewing, Rodney C.; Burns, Peter C.; Dacheux, Nicolas; Navrotsky, Alexandra

2015-01-01

Coffinite, USiO4, is an important U(IV) mineral, but its thermodynamic properties are not well-constrained. In this work, two different coffinite samples were synthesized under hydrothermal conditions and purified from a mixture of products. The enthalpy of formation was obtained by high-temperature oxide melt solution calorimetry. Coffinite is energetically metastable with respect to a mixture of UO2 (uraninite) and SiO2 (quartz) by 25.6 ± 3.9 kJ/mol. Its standard enthalpy of formation from the elements at 25 °C is −1,970.0 ± 4.2 kJ/mol. Decomposition of the two samples was characterized by X-ray diffraction and by thermogravimetry and differential scanning calorimetry coupled with mass spectrometric analysis of evolved gases. Coffinite slowly decomposes to U3O8 and SiO2 starting around 450 °C in air and thus has poor thermal stability in the ambient environment. The energetic metastability explains why coffinite cannot be synthesized directly from uraninite and quartz but can be made by low-temperature precipitation in aqueous and hydrothermal environments. These thermochemical constraints are in accord with observations of the occurrence of coffinite in nature and are relevant to spent nuclear fuel corrosion. PMID:25964321

Immobilization of uranium in biofilm microorganisms exposed to groundwater seeps over granitic rock tunnel walls in Olkiluoto, Finland

NASA Astrophysics Data System (ADS)

Krawczyk-Bärsch, Evelyn; Lünsdorf, Heinrich; Pedersen, Karsten; Arnold, Thuro; Bok, Frank; Steudtner, Robin; Lehtinen, Anne; Brendler, Vinzenz

2012-11-01

In an underground rock characterization facility, the ONKALO tunnel in Finland, massive 5-10-mm thick biofilms were observed attached to tunnel walls where groundwater was seeping from bedrock fractures at a depth of 70 m. In laboratory experiments performed in a flow cell with detached biofilms to study the effect of uranium on the biofilm, uranium was added to the circulating groundwater (CGW) obtained from the fracture feeding the biofilm. The final uranium concentration in the CGW was adjusted to 4.25 × 10-5 M, in the range expected from a leaking spent nuclear fuel (SNF) canister in a future underground repository. The effects were investigated using microelectrodes to measure pH and Eh, time-resolved laser fluorescence spectroscopy (TRLFS), energy-filtered transmission electron microscopy (EF-TEM), and electron energy-loss spectroscopy (EELS) studies and thermodynamic calculations were utilized as well. The results indicated that the studied biofilms constituted their own microenvironments, which differed significantly from that of the CGW. A pH of 5.37 was recorded inside the biofilm, approximately 3.5 units lower than the pH observed in the CGW, due to sulfide oxidation to sulfuric acid in the biofilm. Similarly, the Eh of +73 mV inside the biofilm was approximately 420 mV lower than the Eh measured in the CGW. Adding uranium increased the pH in the biofilm to 7.27 and reduced the Eh to -164 mV. The changes of Eh and pH influenced the bioavailability of uranium, since microbial metabolic processes are sensitive to metals and their speciation. EF-TEM investigations indicated that uranium in the biofilm was immobilized intracellularly in microorganisms by the formation of metabolically mediated uranyl phosphate, similar to needle-shaped autunite (Ca[UO2]2[PO4]2·2-6H2O) or meta-autunite (Ca[UO2]2[PO4]2·10-12H2O). In contrast, TRLFS studies of the contaminated CGW identified aqueous uranium carbonate species, likely (Ca2UO2[CO3]3), formed due to the high concentration of carbonate in the CGW. The results agreed with thermodynamic calculations of the theoretically predominant field of uranium species, formed in the uranium-contaminated CGW at the measured geochemical parameters. This investigation clearly demonstrated that biological systems must be considered as a part of natural systems that can significantly influence radionuclide behavior. The results improve our understanding of the mechanisms of biofilm response to radionuclides in relation to safety assessments of SNF repositories.

Reanalysis of the gas-cooled fast reactor experiments at the zero power facility proteus - Spectral indices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Perret, G.; Pattupara, R. M.; Girardin, G.

2012-07-01

The gas-cooled fast reactor (GCFR) concept was investigated experimentally in the PROTEUS zero power facility at the Paul Scherrer Inst. during the 1970's. The experimental program was aimed at neutronics studies specific to the GCFR and at the validation of nuclear data in fast spectra. A significant part of the program used thorium oxide and thorium metal fuel either distributed quasi-homogeneously in the reference PuO{sub 2}/UO{sub 2} lattice or introduced in the form of radial and axial blanket zones. Experimental results obtained at the time are still of high relevance in view of the current consideration of the Gas-cooled Fastmore » Reactor (GFR) as a Generation-IV nuclear system, as also of the renewed interest in the thorium cycle. In this context, some of the experiments have been modeled with modern Monte Carlo codes to better account for the complex PROTEUS whole-reactor geometry and to allow validating recent continuous neutron cross-section libraries. As a first step, the MCNPX model was used to test the JEFF-3.1, JEFF-3.1.1, ENDF/B-VII.0 and JENDL-3.3 libraries against spectral indices, notably involving fission and capture of {sup 232}Th and {sup 237}Np, measured in GFR-like lattices. (authors)« less

A novel benzimidazole-functionalized 2-D COF material: synthesis and application as a selective solid-phase extractant for separation of uranium.

PubMed

Li, Juan; Yang, Xiaodan; Bai, Chiyao; Tian, Yin; Li, Bo; Zhang, Shuang; Yang, Xiaoyu; Ding, Songdong; Xia, Chuanqin; Tan, Xinyu; Ma, Lijian; Li, Shoujian

2015-01-01

A novel COF-based material (COF-COOH) containing large amounts of carboxylic groups was prepared for the first time by using a simple and effective one-step synthetic method, in which the cheap and commercially available raw materials, trimesoyl chloride and p-phenylenediamine, were used. The as-synthesized COF-COOH was modified with previously synthesized 2-(2,4-dihydroxyphenyl)-benzimidazole (HBI) by "grafting to" method, and a new solid-phase extractant (COF-HBI) with highly efficient sorption performance for uranium(VI) was consequently obtained. A series of characterizations demonstrated that COF-COOH and COF-HBI exhibited great thermostabilities and irradiation stabilities. Sorption behavior of the COF-based materials toward U(VI) was compared in simulated nuclear industrial effluent containing UO2(2+) and 11 undesired ions, and the UO2(2+) sorption amount of COF-HBI was 81 mg g(-1), accounting for approximately 58% of the total sorption amount, which was much higher than the sorption selectivity of COF-COOH to UO2(2+) (39%). Batch sorption experiment results indicated that the uranium(VI) sorption on COF-HBI was a pH dependent, rapid (sorption equilibrium was reached in 30 min), endothermic and spontaneous process. In the most favorable conditions, the equilibrium sorption capacity of the adsorbent for uranium could reach 211 mg g(-1). Copyright © 2014 Elsevier Inc. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pritam Chakraborty; Michael R. Tonks; Giovanni Pastore

Grain boundary (GB) separation as a mechanism for fission gas release (FGR), complementary to gas bubble interlinkage, has been experimentally observed in irradiated light water reactor fuel. However there has been limited effort to develop physics-based models incorporating this mechanism for the analysis of FGR. In this work, a computational study is carried out to investigate GB separation in UO2 fuel under the effect of gas bubble pressure and hydrostatic stress. A non-dimensional stress intensity factor formula is obtained through 2D axisymmetric analyses considering lenticular bubbles and Mode-I crack growth. The obtained functional form can be used in higher length-scalemore » models to estimate the contribution of GB separation to FGR.« less

Development of LWR Fuels with Enhanced Accident Tolerance

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lahoda, Edward J.; Boylan, Frank A.

2015-10-30

Significant progress was made on the technical, licensing, and business aspects of the Westinghouse Electric Company’s Enhanced Accident Tolerant Fuel (ATF) by the Westinghouse ATF team. The fuel pellet options included waterproofed U 15N and U 3Si 2 and the cladding options SiC composites and zirconium alloys with surface treatments. Technology was developed that resulted in U 3Si 2 pellets with densities of >94% being achieved at the Idaho National Laboratory (INL). The use of U 3Si 2 will represent a 15% increase in U235 loadings over those in UO₂ fuel pellets. This technology was then applied to manufacture pelletsmore » for 6 test rodlets which were inserted in the Advanced Test Reactor (ATR) in early 2015 in zirconium alloy cladding. The first of these rodlets are expected to be removed in about 2017. Key characteristics to be determined include verification of the centerline temperature calculations, thermal conductivity, fission gas release, swelling and degree of amorphization. Waterproofed UN pellets have achieved >94% density for a 32% U 3Si 2/68% UN composite pellet at Texas A&M University. This represents a U235 increase of about 31% over current UO 2 pellets. Pellets and powders of UO 2, UN, and U 3Si 2the were tested by Westinghouse and Los Alamos National Laboratory (LANL) using differential scanning calorimetry to determine what their steam and 20% oxygen corrosion temperatures were as compared to UO 2. Cold spray application of either the amorphous steel or the Ti 2AlC was successful in forming an adherent ~20 micron coating that remained after testing at 420°C in a steam autoclave. Tests at 1200°C in 100% steam on coatings for Zr alloy have not been successful, possibly due to the low density of the coatings which allowed steam transport to the base zirconium metal. Significant modeling and testing has been carried out for the SiC/SiC composite/SiC monolith structures. A structure with the monolith on the outside and composite on the inside was developed which is the current baseline structure and a SiC to SiC tube closure approach. Permeability tests and mechanical tests were developed to verify the operation of the SiC cladding. Steam autoclave (420°C), high temperature (1200°C) flowing steam tests and quench tests were carried out with minimal corrosion, mechanical or hermeticity degradation effect on the SiC cladding or end plug closure. However, in-reactor loop tests carried out in the MIT reactor indicated an unacceptable degree of corrosion, likely due to the corrosive effect of radiolysis products which attacked the SiC.« less

Structure of complexes of uranyl succinate with carbamide and dimethylurea

NASA Astrophysics Data System (ADS)

Serezhkina, L. B.; Grigor'ev, M. S.; Seliverstova, N. V.; Serezhkin, V. N.

2017-09-01

Three new succinate-containing complexes of uranyl with carbamide ( Urea) and N,N'-dimethylurea ( s-Dmur) are synthesized and studied by IR spectroscopy and X-ray diffraction. Structures of the same type, [UO2( Urea)4(H2O)][(UO2)2(C4H4O4)3] · 3H2O and [UO2( Urea)4(H2O)][(UO2)2(C4H4O4)3] · 2 Urea contain two sorts of uranium-containing complex groups, namely, mononuclear [UO2( Urea)4(H2O)]2+ cations and two-dimensional [(UO2)2(C4H4O4)3]2- anions described by crystal-chemical formulas AM 5 1 and A 2 Q 3 02, respectively ( A = UO2 2+, M 1 = Urea or H2O, Q 02 = C4H4O4 2-), and differ only in the nature of noncoordinated molecules—water and carbamide. The main structural groups of the [(UO2)2(C4H4O4)2( s-Dmur)3] crystals are [(UO2)2(C4H4O4)2( s-Dmur)3] chains belonging to the A 2 Q 2 02 M 3 1 ( A = UO2 2+, Q 02 = C4H4O4 2-, M 1 = s-Dmur) crystal-chemical group. Specific features of intermolecular interactions in the crystal structures are revealed using the Voronoi-Dirichlet method of molecular polyhedra.

Application of the DART Code for the Assessment of Advanced Fuel Behavior

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rest, J.; Totev, T.

2007-07-01

The Dispersion Analysis Research Tool (DART) code is a dispersion fuel analysis code that contains mechanistically-based fuel and reaction-product swelling models, a one dimensional heat transfer analysis, and mechanical deformation models. DART has been used to simulate the irradiation behavior of uranium oxide, uranium silicide, and uranium molybdenum aluminum dispersion fuels, as well as their monolithic counterparts. The thermal-mechanical DART code has been validated against RERTR tests performed in the ATR for irradiation data on interaction thickness, fuel, matrix, and reaction product volume fractions, and plate thickness changes. The DART fission gas behavior model has been validated against UO{sub 2}more » fission gas release data as well as measured fission gas-bubble size distributions. Here DART is utilized to analyze various aspects of the observed bubble growth in U-Mo/Al interaction product. (authors)« less

Synchrotron X-ray characterization of mackinawite and uraninite relevant to bio-remediation of groundwater contaminated with uranium

NASA Astrophysics Data System (ADS)

Carpenter, J.; Hyun, S.; Hayes, K. F.

2010-12-01

Uranium (U) originating from mining operations for weapon manufacturing and nuclear energy production is a significant radionuclide contaminant in groundwater local to uranium mining, uranium milling, and uranium mill tailing (UMT) storage sites. In the USA, the Department of Energy (DOE) is currently overseeing approximately 24 Uranium Mill Tailing Remediation Action (UMTRA) sites which have collectively processed over 27 million tons of uranium ore1,2. In-Situ microbial bio-reduction of the highly mobile U6+ ion into the dramatically less mobile U4+ ion has been demonstrated as an effective remedial process to inhibit uranium migration in the aqueous phase3. The resistance of this process to oxidization and possible remobilization of U when bioremediation stops (and oxidants such as oxygen from the air or nitrate in water diffuse into the formation) in the long term is not known. UMTRA site studies3 have shown that iron sulfide solids are produced by sulfate reducing bacteria (SRB) during U bioremediation, and some forms of these iron sulfide solids are known to be effective oxidant scavengers, potentially protecting against re-oxidation and thus remobilization of U. This work is investigating the role of iron sulfide solids in the long-term immobilization of reduced U compounds after bioremediation is completed in groundwater local to UMTRA sites. Re-oxidation tests are being performed in packed media columns loaded with both FeS and U solids. High quality mackinawite (FeS), and uraninite (UO2) have been synthesized in our laboratory via a wet chemistry approach. These synthetic materials are expected to mimic the naturally occurring and biogenic materials present in biologically stimulated UMTRA sites. In order to establish the initial conditions of the prepared experimental columns and to compare synthetic and biogenic FeS and UO2, these synthesized materials have been characterized with synchrotron radiation at the Stanford Synchrotron Radiation Lightsource using synchrotron x-ray powder diffraction (SXRD) and extended x-ray absorption fine structure (EXAFS). SXRD data were collected and analyzed with profile fitting to determine lattice parameters and crystallite size for comparison with published values for both biogenic and synthetic materials. This is particularly of interest for UO2, as there is very little information on particle size and lattice parameters for synthetic UO2 in the literature. Profile fitting of the SXRD data for FeS gives lattice parameters of a = b = 3.668 and a mean crystallite size of 5 to 8 nm. Both of these values are in good agreement with published values. For fresh UO2, lattice parameters were determined as a = b = c = 5.4 nm for both freshly synthesized and aged (3 months) UO2 and particle size was determined to be 3.5 nm for fresh UO2 and 5.83 nm for aged UO2. This suggests a growth mechanism for crystallites over time, and an inferred decrease in reactivity.

Expanding the Chemistry of Actinide Metallocene Bromides. Synthesis, Properties and Molecular Structures of the Tetravalent and Trivalent Uranium Bromide Complexes: (C 5Me 4R) 2UBr 2, (C 5Me 4R) 2U(O-2,6- iPr 2C 6H 3)(Br), and [K(THF)][(C 5Me 4R) 2UBr 2] (R = Me, Et)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lichtscheidl, Alejandro Gaston; Pagano, Justin K.; Scott, Brian Lindley

The organometallic uranium species (C 5Me 4R) 2UBr 2 (R = Me, Et) were obtained by treating their chloride analogues (C 5Me 4R) 2UCl 2 (R = Me, Et) with Me 3SiBr. Treatment of (C 5Me 4R) 2UCl 2 and (C 5Me 4R) 2UBr 2 (R = Me, Et) with K(O-2,6- iPr 2C 6H 3) afforded the halide aryloxide mixed-ligand complexes (C 5Me 4R) 2U(O-2,6- iPr 2C 6H 3)(X) (R = Me, Et; X = Cl, Br). Complexes (C 5Me 4R) 2U(O-2,6- iPr 2C 6H 3)(Br) (R = Me, Et) can also be synthesized by treating (C 5Me 4R) 2U(O-2,6-more » iPr 2C 6H 3)(Cl) (R = Me, Et) with Me 3SiBr, respectively. Reduction of (C 5Me 4R) 2UCl 2 and (C 5Me 4R) 2UBr 2 (R = Me, Et) with KC 8 led to isolation of uranium(III) “ate” species [K(THF)][(C 5Me 5) 2UX 2] (X = Cl, Br) and [K(THF) 0.5][(C 5Me 4Et) 2UX 2] (X = Cl, Br), which can be converted to the neutral complexes (C 5Me 4R) 2U[N(SiMe 3) 2] (R = Me, Et). Analyses by nuclear magnetic resonance spectroscopy, X-ray crystallography, and elemental analysis are also presented.« less

Expanding the Chemistry of Actinide Metallocene Bromides. Synthesis, Properties and Molecular Structures of the Tetravalent and Trivalent Uranium Bromide Complexes: (C 5Me 4R) 2UBr 2, (C 5Me 4R) 2U(O-2,6- iPr 2C 6H 3)(Br), and [K(THF)][(C 5Me 4R) 2UBr 2] (R = Me, Et)

DOE PAGES

Lichtscheidl, Alejandro Gaston; Pagano, Justin K.; Scott, Brian Lindley; ...

2016-01-06

The organometallic uranium species (C 5Me 4R) 2UBr 2 (R = Me, Et) were obtained by treating their chloride analogues (C 5Me 4R) 2UCl 2 (R = Me, Et) with Me 3SiBr. Treatment of (C 5Me 4R) 2UCl 2 and (C 5Me 4R) 2UBr 2 (R = Me, Et) with K(O-2,6- iPr 2C 6H 3) afforded the halide aryloxide mixed-ligand complexes (C 5Me 4R) 2U(O-2,6- iPr 2C 6H 3)(X) (R = Me, Et; X = Cl, Br). Complexes (C 5Me 4R) 2U(O-2,6- iPr 2C 6H 3)(Br) (R = Me, Et) can also be synthesized by treating (C 5Me 4R) 2U(O-2,6-more » iPr 2C 6H 3)(Cl) (R = Me, Et) with Me 3SiBr, respectively. Reduction of (C 5Me 4R) 2UCl 2 and (C 5Me 4R) 2UBr 2 (R = Me, Et) with KC 8 led to isolation of uranium(III) “ate” species [K(THF)][(C 5Me 5) 2UX 2] (X = Cl, Br) and [K(THF) 0.5][(C 5Me 4Et) 2UX 2] (X = Cl, Br), which can be converted to the neutral complexes (C 5Me 4R) 2U[N(SiMe 3) 2] (R = Me, Et). Analyses by nuclear magnetic resonance spectroscopy, X-ray crystallography, and elemental analysis are also presented.« less

A charge-optimized many-body potential for the U-UO2-O2 system

NASA Astrophysics Data System (ADS)

Li, Yangzhong; Liang, Tao; Sinnott, Susan B.; Phillpot, Simon R.

2013-12-01

Building on previous charge-optimized many-body (COMB) potentials for metallic α-U and gaseous O2, we have developed a new potential for UO2, which also allows the simulation of U-UO2-O2 systems. The UO2 lattice parameter, elastic constants and formation energies of stoichiometric and non-stoichiometric intrinsic defects are well reproduced. Moreover, this is the first rigid-ion potential that produces the correct deviation of the Cauchy relation, as well as the first classical interatomic potential that is able to determine the defect energies of non-stoichiometric intrinsic point defects in UO2 with an appropriate reference state. The oxygen molecule interstitial in the α-U structure is shown to decompose, with some U-O bonds approaching the natural bond length of perfect UO2. Finally, we demonstrate the capability of this COMB potential to simulate a complex system by performing a simulation of the α-U + O2 → UO2 phase transformation. We also identify a possible mechanism for uranium oxidation and the orientation of the resulting fluorite UO2 structure relative to the coordinate system of orthorhombic α-U.

Surface reactions of ethanol over UO 2(100) thin film

DOE Office of Scientific and Technical Information (OSTI.GOV)

S. D. Senanayake; Mudiyanselage, K.; Burrell, A. K.

2015-10-08

The study of the reactions of oxygenates on well-defined oxide surfaces is important for the fundamental understanding of heterogeneous chemical pathways that are influenced by atomic geometry, electronic structure, and chemical composition. In this work, an ordered uranium oxide thin film surface terminated in the (100) orientation is prepared on a LaAlO 3 substrate and studied for its reactivity with a C-2 oxygenate, ethanol (CH 3CH 2OH). With the use of synchrotron X-ray photoelectron spectroscopy (XPS), we have probed the adsorption and desorption processes observed in the valence band, C 1s, O 1s, and U 4f to investigate the bondingmore » mode, surface composition, electronic structure, and probable chemical changes to the stoichiometric-UO 2(100) [smooth-UO 2(100)] and Ar +-sputtered UO 2(100) [rough-UO 2(100)] surfaces. Unlike UO 2(111) single crystal and UO 2 thin film, Ar-ion-sputtering of this UO 2(100) did not result in noticeable reduction of U cations. Upon ethanol adsorption (saturation occurred at 0.5 ML), only the ethoxy (CH 3CH 2O –) species is formed on smooth-UO 2(100) whereas initially formed ethoxy species are partially oxidized to surface acetate (CH3COO–) on the Ar +-sputtered UO 2(100) surface. Furthermore, all ethoxy and acetate species are removed from the surface between 600 and 700 K.« less

Status of French reactors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ballagny, A.

1997-08-01

The status of French reactors is reviewed. The ORPHEE and RHF reactors can not be operated with a LEU fuel which would be limited to 4.8 g U/cm{sup 3}. The OSIRIS reactor has already been converted to LEU. It will use U{sub 3}Si{sub 2} as soon as its present stock of UO{sub 2} fuel is used up, at the end of 1994. The decision to close down the SILOE reactor in the near future is not propitious for the start of a conversion process. The REX 2000 reactor, which is expected to be commissioned in 2005, will use LEU (exceptmore » if the fast neutrons core option is selected). Concerning the end of the HEU fuel cycle, the best option is reprocessing followed by conversion of the reprocessed uranium to LEU.« less

Selective Extraction of Uranium from Liquid or Supercritical Carbon Dioxide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farawila, Anne F.; O'Hara, Matthew J.; Wai, Chien M.

2012-07-31

Current liquid-liquid extraction processes used in recycling irradiated nuclear fuel rely on (1) strong nitric acid to dissolve uranium oxide fuel, and (2) the use of aliphatic hydrocarbons as a diluent in formulating the solvent used to extract uranium. The nitric acid dissolution process is not selective. It dissolves virtually the entire fuel meat which complicates the uranium extraction process. In addition, a solvent washing process is used to remove TBP degradation products, which adds complexity to the recycling plant and increases the overall plant footprint and cost. A liquid or supercritical carbon dioxide (l/sc -CO2) system was designed tomore » mitigate these problems. Indeed, TBP nitric acid complexes are highly soluble in l/sc -CO2 and are capable of extracting uranium directly from UO2, UO3 and U3O8 powders. This eliminates the need for total acid dissolution of the irradiated fuel. Furthermore, since CO2 is easily recycled by evaporation at room temperature and pressure, it eliminates the complex solvent washing process. In this report, we demonstrate: (1) A reprocessing scheme starting with the selective extraction of uranium from solid uranium oxides into a TBP-HNO3 loaded Sc-CO2 phase, (2) Back extraction of uranium into an aqueous phase, and (3) Conversion of recovered purified uranium into uranium oxide. The purified uranium product from step 3 can be disposed of as low level waste, or mixed with enriched uranium for use in a reactor for another fuel cycle. After an introduction on the concept and properties of supercritical fluids, we first report the characterization of the different oxides used for this project. Our extraction system and our online monitoring capability using UV-Vis absorbance spectroscopy directly in sc-CO2 is then presented. Next, the uranium extraction efficiencies and kinetics is demonstrated for different oxides and under different physical and chemical conditions: l/sc -CO2 pressure and temperature, TBP/HNO3 complex used, reductant or complexant used for selectivity, and ionic liquids used as supportive media. To complete the extraction and recovery cycle, we then demonstrate uranium back extraction from the TBP loaded sc-CO2 phase into an aqueous phase and the characterization of the uranium complex formed at the end of this process. Another aspect of this project was to limit proliferation risks by either co-extracting uranium and plutonium, or by leaving plutonium behind by selectively extracting uranium. We report that the former is easily achieved, since plutonium is in the tetravalent or hexavalent oxidation state in the oxidizing environment created by the TBP-nitric acid complex, and is therefore co-extracted. The latter is more challenging, as a reductant or complexant to plutonium has to be used to selectively extract uranium. After undertaking experiments on different reducing or complexing systems (e.g., AcetoHydroxamic Acid (AHA), Fe(II), ascorbic acid), oxalic acid was chosen as it can complex tetravalent actinides (Pu, Np, Th) in the aqueous phase while allowing the extraction of hexavalent uranium in the sc-CO2 phase. Finally, we show results using an alternative media to commonly used aqueous phases: ionic liquids. We show the dissolution of uranium in ionic liquids and its extraction using sc-CO2 with and without the presence of AHA. The possible separation of trivalent actinides from uranium is also demonstrated in ionic liquids using neodymium as a surrogate and diglycolamides as the extractant.« less

Hydrothermal syntheses, structures, and properties of the new uranyl selenites Ag(2)(UO(2))(SeO(3))(2), M[(UO(2))(HSeO(3))(SeO(3))] (M = K, Rb, Cs, Tl), and Pb(UO(2))(SeO(3))(2).

PubMed

Almond, Philip M; Albrecht-Schmitt, Thomas E

2002-03-11

The transition metal, alkali metal, and main group uranyl selenites, Ag(2)(UO(2))(SeO(3))(2) (1), K[(UO(2))(HSeO(3))(SeO(3))] (2), Rb[(UO(2))(HSeO(3))(SeO(3))] (3), Cs[(UO(2))(HSeO(3))(SeO(3))] (4), Tl[(UO(2))(HSeO(3))(SeO(3))] (5), and Pb(UO(2))(SeO(3))(2) (6), have been prepared from the hydrothermal reactions of AgNO(3), KCl, RbCl, CsCl, TlCl, or Pb(NO(3))(2) with UO(3) and SeO(2) at 180 degrees C for 3 d. The structures of 1-5 contain similar [(UO(2))(SeO(3))(2)](2-) sheets constructed from pentagonal bipyramidal UO(7) units that are joined by bridging SeO(3)(2-) anions. In 1, the selenite oxo ligands that are not utilized within the layers coordinate the Ag(+) cations to create a three-dimensional network structure. In 2-5, half of the selenite ligands are monoprotonated to yield a layer composition of [(UO(2))(HSeO(3))(SeO(3))](1-), and coordination of the K(+), Rb(+), Cs(+), and Tl(+) cations occurs through long ionic contacts. The structure of 6 contains a uranyl selenite layered substructure that differs substantially from those in 1-5 because the selenite anions adopt both bridging and chelating binding modes to the uranyl centers. Furthermore, the Pb(2+) cations form strong covalent bonds with these anions creating a three-dimensional framework. These cations occur as distorted square pyramidal PbO(5) units with stereochemically active lone pairs of electrons. These polyhedra align along the c-axis to create a polar structure. Second-harmonic generation (SHG) measurements revealed a response of 5x alpha-quartz for 6. The diffuse reflectance spectrum of 6 shows optical transitions at 330 and 440 nm. The trailing off of the 440 nm transition to longer wavelengths is responsible for the orange coloration of 6.

Coordination trends in alkali metal crown ether uranyl halide complexes: the series [A(crown)]2[UO(2)X(4)] where A=Li, Na, K and X=Cl, Br.

PubMed

Danis, J A; Lin, M R; Scott, B L; Eichhorn, B W; Runde, W H

2001-07-02

UO(2)(C(2)H(3)O(2))(2).2H(2)O reacts with AX or A(C(2)H(3)O(2) or ClO(4)) (where A = Li, Na, K; X = Cl, Br) and crown ethers in HCl or HBr aqueous solutions to give the sandwich-type compounds [K(18-crown-6)](2)[UO(2)Cl(4)] (1), [K(18-crown-6)](2)[UO(2)Br(4)] (2), [Na(15-crown-5)](2)[UO(2)Cl(4)] (3), [Na(15-crown-5)](2)[UO(2)Br(4)] (4), [Li(12-crown-4)](2)[UO(2)Cl(4)] (5), and [Li(12-crown-4)](2)[UO(2)Br(4)] (6). The compounds have been characterized by single-crystal X-ray diffraction, powder diffraction, elemental analysis, IR, and Raman spectroscopy. The [UO(2)X(4)](2-) ions coordinate to two [A(crown)](+) cations through the four halides only (2), through two halides only (3), through the two uranyl oxygens and two halides (3, 4), or through the two uranyl oxygen atoms only (5, 6). Raman spectra reveal nu(U-O) values that correlate with expected trends. The structural trends are discussed within the context of classical principles of hard-soft acid-base theory.

Syntheses and crystal structures of two topologically related modifications of Cs(2)[(UO(2))(2)(MoO(4))(3)].

PubMed

Krivovichev, S V; Cahill, C L; Burns, P C

2002-01-14

Two polymorphs of Cs(2)(UO(2))(2)(MoO(4))(3) have been synthesized by hydrothermal (alpha-phase) and high-temperature (beta-phase) routes. Both were characterized by single-crystal X-ray diffraction: alpha-Cs(2)(UO(2))(2)(MoO(4))(3), orthorhombic, Pna2(1), a = 20.4302(15) A, b = 8.5552(7) A, c = 9.8549(7) A, Z = 4; beta-Cs(2)(UO(2))(2)(MoO(4))(3), tetragonal, P4(2)/n, a = 10.1367(8) A, c = 16.2831(17) A, Z = 4. The structures of both phases consist of linked UO(7) pentagonal bipyramids and MoO(4) tetrahedra: alpha-Cs(2)(UO(2))(2)(MoO(4))(3) is a framework compound with large channels parallel to the c axis. Two cesium sites are located in these channels and are coordinated by 8 and 10 oxygen atoms. The structure of beta-Cs(2)(UO(2))(2)(MoO(4))(3) contains corrugated [(UO(2))(2)(MoO(4))(3)] sheets that are parallel to (001). The cesium cations are located between the sheets and are coordinated by eight oxygen atoms. The structures are topologically related; both can be described in terms of chains of 5-connected UO(7) pentagonal bipyramids and 3- and 4-connected MoO(4) tetrahedra.

Validation of the fission yield and decay data libraries with the 10 s-delayed 235 U fission γ-ray energy spectrum

NASA Astrophysics Data System (ADS)

Mendoza, E.; Álvarez-Velarde, F.; Bécares, V.; Cano-Ott, D.; González-Romero, E.; Martínez, T.; Villamarín, D.

2017-10-01

We have measured with a LaCl3 detector the γ-ray spectrum emitted by a 235 U enriched UO2 fuel rod 10 s after being irradiated with thermal neutrons. The experimental results are compared with simulations performed with the fission product yield and radioactive decay data libraries present in the most recent releases of ENDF/B, JEFF and JENDL.

Structure and cation ordering in La 2UO 6, Ce 2UO 6, LaUO 4, and CeUO 4 by first principles calculations

DOE PAGES

Casillas-Trujillo, Luis; Xu, H.; McMurray, Jake W.; ...

2016-07-06

In the present work, we have used density functional theory (DFT) and DFT+U to investigate the crystal structure and phase stability of four model compounds in the Ln 2O 3-UO 2-UO 3 ternary oxide system: La2UO 6, Ce 2UO 6, LaUO 4, CeUO 4, due to the highly-correlated nature of the f-electrons in uranium. We have considered both hypothetical ordered compounds and compounds in which the cations randomly occupy atomic sites in a fluorite-like lattice. We determined that ordered compounds are stable and are energetically favored compared to disordered configurations, though the ordering tendencies are weak. To model and analyzemore » the structures of these complex oxides, we have used supercells based on a layered atomic model. In the layer model, the supercell is composed of alternating planes of anions and cations. We have considered two different ordering motifs for the cations, namely single species (isoatomic) cation layers versus mixed species cation layers. Energy differences between various ordered cationic arrangements were found to be small. This may have implications regarding radiation stability, since cationic arrangements should be able to change under irradiation with little cost in energy.« less