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This presentation talks on the Critical experiments performed on the NCERC machines. Plutonium ( 239 Pu and 240 Pu), Highly Enriched Uranium, Low-Temperature (-40°C). This is all based on a simple design useful for modeling and validation. The design is made to incorporate materials of interest such as Tantalum, hafnium, lithium & more.
ENDF-6 formatted files were processed into A Compact ENDF (ACE) files using NJOY2016. Several validation tests were performed: (1) LANL Legacy Benchmark Suite (2) “Modern” Benchmark Suite (3) HEU Benchmark Suite (4) LEU Benchmark Suite (5) Mixed (U+Pu) Benchmark Suite (6) Pu Benchmark Suite (7) 233 U Benchmark Suite.
The Savannah River Site (SRS) plans to dissolve non-irradiated stainless steel (SS)-clad bundles of Fast Critical Assembly (FCA) materials in eighteen batches.1 FCA dissolution is currently underway in the 6.3D dissolver by simultaneous chemical and electrolytic dissolution, which is required to generate the harsh conditions necessary for dissolution of metal-oxide (MOX) and non-aluminum spent nuclear fuels (NASNFs).2 Nitric acid and potassium fluoride are used to promote chemical dissolution.2 Gadolinium will be added during processing as a thermal neutron poison for criticality control. There are no plans for recovering plutonium from this waste stream. After FCA dissolution, the acidic (HNO3/KF) “discards” containing the dissolved metals will be neutralized by addition of 50 wt% sodium hydroxide to a final free hydroxide concentration of 1.2 M.1 Neutralization will precipitate a slurry of insoluble solids, predominantly metal oxides/hydroxides of plutonium, uranium, and SS components. Small fractions of the SS components, Pu, U, and Gd will remain dissolved in the supernate. The neutralized slurry will be composited to existing radioactive waste storage tanks within the SRS Concentration, Storage, and Transfer Facilities (CSTF) containing other similar sludge batch (SB) materials.1 The fate of soluble plutonium and freshly-precipitated, colloidal plutonium from this process are of concern since the total Pu can challenge the waste acceptance criteria (WAC) at the downstream SRS Liquid Waste (LW) facility. Supernate decants including the neutralized FCA discards (nFCAd) within the CSTF will be composited with salt batch (StB) materials and transferred to the SRS Salt Waste Processing Facility (SWPF), where total plutonium is also of concern.
Over the the last 70 years plutonium (Pu) has been integral in the development of several technologies that have changed the world, yet our fundamental understanding of its chemistry is still far from complete. This is a testament to this element?s unique and complex properties, such as its ability to coexist as multiple oxidation states in aqueous solution. Careful manipulation of plutonium oxidation states is essential in the study and utilization of its rich chemistry. To achieve this level of control, a comprehensive mechanistic understanding of radiation-induced plutonium redox chemistry is critical due to the unavoidable exposure of plutonium to ionizing radiation fields, both inherent and from in-process applications. For this reason, we have developed an experimentally evaluated multi-scale computer model for the prediction of gamma radiation-induced Pu(IV) redox chemistry in concentrated nitric acid solutions (1.0, 3.0, and 6.0 M).
• Neutralization and solidification is the last step in the Aqueous Recovery Process • All waste streams are acidic and must be neutralized before being combined with grout in a solidification drum • The neutralization tank is a 250 L, 24” diameter, 45” high tank • The batch tank is a 125 L tank • The solidification drum is a 55-gallon drum, pre-filled with grout & a sacrificial mixing paddle • Normal mass in neutralization tank: 50 g Pu • Normal mass in batch tank or drum: 25 g Pu
New reactor designs, such as pebble-bed reactors, present challenges for the safeguarding of fissile material. Due to the multi-pass fuel circulation design and the non-uniform path a pebble may traverse through a pebble-bed reactor, there will be variations in the irradiation history of spent fuel pebbles. The standard approach of estimating actinide quantities based on fission gamma spectra or neutron emission paired with depletion modeling may yield uncertainties too large for safeguards and material accountancy. This project investigated, through modeling and experimentation, the potential of neutron self-interrogation of spent fuel pebbles as an innovative method to implement materials accountability. As an example, our feasibility studies indicate that the mass of U-235, U-238, Pu-239 and Pu-241 can be predicted to 4.1, 0.86, 13 and 13 % accuracy, respectively, when measuring 100 closely packed end-of-life spent fuel pebbles over approximately 12 days using a 4π counting geometry.
Based on the rationale presented, post-closure nuclear criticality is improbable when room closure compacts containers disposing transuranic (TRU) waste emplaced at the Waste Isolation Pilot Plant (WIPP), an operating repository in bedded salt in southeastern New Mexico. As described in the original WIPP certification, a qualitative estimate of the probability of post-closure criticality in TRU waste produced from atomic energy defense activities has been low either because remote-handled TRU waste canisters are neutronically isolated by the bedded salt or because the low fissile mass in an array of contact-handled TRU waste drums cannot be compacted sufficiently by room closure from salt creep. These situations are still valid for the majority of TRU waste that is disposed at WIPP without any disposal constraints, as updated herein. This report also qualitatively evaluates the probability of criticality after disposal of TRU waste in pipe overpack containers (POC) where every POC in a shipment may have the maximum 200 fissile gram equivalent of 239Pu content. The probability of criticality for a disposal room filled with POCs is estimated during four representative phases of repository evolution: (1) a large salt block falls onto POCs in the first 20 years, (2) salt creep closes a disposal room in the first 1000 years without brine seepage and subsequent gas generation, which permits maximum compaction, (3) some brine seepage occurs into the closed room, which initiates consumption of the fiberboard (cellulose) impact absorber in the POC in the second 1000 years, and (4) full brine inundation of a room and consumption of all fiberboard thereafter. Salt-block fall in the first phase does not greatly disrupt three tiers of POCs. The compacted spacing of POCs in the later three repository conditions is calculated through high-fidelity, geomechanical modeling. Criticality evaluation of compacted 200-g 239 Pu spheres at the compacted spacing shows that neither 12-inch nor 6-inch POCs are critical after the first 1000 years, the second 1000 years, or thereafter as the sea of reflector material changes to represent the three repository conditions. Specifically, fiberboard and iron isolates 239 Pu while dry, and brine reduces the reactivity when a room is partially and fully inundated. Because POC behavior bounds behavior of other standard TRU waste containers, post-closure criticality caused by room closure compacting containers is omitted in the performance assessments for the 2019 and 2026 WIPP compliance re-certification applications to the US Environmental Protection Agency.
Gamma and neutron measurements on various types of plutonium sources are presented in order to show the effects of O-17, O-18 F-19, Pu-236, age of the fuel, and size of the source on the gamma and neutron spectra. Analysis of the radiation measurements shows that fluorine is the main contributor to the neutron yields from present plutonium-molybdenum cermet fuel, while both fluorine and Pu-236 daughters contribute significantly to the gamma ray intensities.
The three Apollo 14 breccias 14301, 14313, and 14318 all show fission xenon due to the decay of Pu-244. To investigate possible in situ production of the fission gas, an analysis was made of the U-distribution in these three breccias. The major amount of the U lies in glass clasts and in matrix material and no more than 25% occurs in distinct high-U minerals. The U-distribution of each breccia is discussed in detail. Whitlockite grains in breccias 14301 and 14318 found with the U-mapping were etched and analyzed for fission tracks. The excess track densities are much smaller than indicated by the Xe-excess. Because of a preirradiation history documented by very high track densities in feldspar grains, however, it is impossible to attribute the excess tracks to the decay of Pu-244. A modified track method has been developed for measuring average U-concentrations in samples containing a heterogeneous distribution of U in the form of small high-U minerals. The method is briefly discussed, and results for the rocks 14301, 14313, 14318, 68815, 15595, and the soil 64421 are given.
The lunar breccia 14318 is one of three Apollo-14 breccias containing substantial amounts of parentless xenon from the spontaneous fission of extinct Pu-244. The argon and xenon contained in this breccia were studied by stepwise heating of pristine and neutron-irradiated samples. The isotopic composition of xenon from fission, determined by an improved method, is shown to be from Pu-244. Concentrations of this fissiogenic xenon are in substantial excess (15-fold) of what could be produced by spontaneous fission of U-238. The breccia is found to contain abundant trapped argon with an Ar-40/Ar-36 ratio of roughly 14. Otherwise, the argon is radiogenic and gives a convincing K-Ar age of 3.69 plus or minus 0.09 b.y. by the stepwise Ar-40/Ar-39 method, nearly in agreement with ages for other Apollo-14 breccias.
The times at which phyllosilicate matrix and euhedral olivines became associated have been determined for five C2 meteorites. The ages, calculated from fission track densities on crystal surfaces, are based on an initial Pu-244/U-238 ratio in the matrix material of 0.0154 at 4.6 b.y., and range from 4.22 b.y. for Nogoya to 4.42 b.y. for Murray. Unless the initial Pu-244/U-238 ratio was less than 0.004, the meteorites cannot have existed in their present form for 4.6 billion years. The measured ages place limits on the time when pre-compaction effects such as micrometeorite craters and solar flare tracks were produced, and they may approximately date the formation of the olivine crystals themselves.
Whitlockite grains in two Apennine Front KREEP soil fragments contain extremely high densities of fission tracks. A new method is described in which particle tracks are examined in an actinide-poor phase bordering an actinide-rich whitlockite phase. This method clearly distinguishes the fission track contributions from other track sources; e.g., Fe-group cosmic rays, spallation recoils, and dislocations. Observed track excesses, when corrected for U- and Th-related fission sources, are 4-20 times greater than the contribution from spontaneous fission of U-238 (based on an age of 4 b.y.), and probably represent a large and variable contribution from the fission of Pu-244. These fragments may have pre-Imbrium ages, underscoring the importance of KREEP as a constituent of the pre-mare lunar crust. Track excesses are not correlated with the U or Th contents of the whitlockite grains. This behavior suggests that Pu fractionates differently from U and Th in lunar igneous KREEP.
An analysis was carried out of the observed data with Nagoya (surface). Misato (34mwe) and Sakashita (80mwe) multidirectional muon telescope, for the solar activity maximum period of 1978-1983. These data respond to primaries extending over the median rigidity range 60GV to 600GV. The observed amplitude at Sakashita station in 1981-1983 increased, especially in 1982; the amplitude is twice as large as that in 1978-1980, when those at Nagoya and Misato stations are nearly the same as those in 1978-1980. Uni-directional anisotropy is derived by the best fit method by assuming the flat rigidity spectrum with the upper cutoff rigidity Pu. The value of Pu obtained is 270GV in 1981-1983 and 150GV in 1978-1980.
The I-Xe systems of six Allende inclusions (five Eggs and the Pink Angel) appear to have been altered by nonnebular secondary processes. Evidence for this includes temperature-ordered variations in the initial I isotopic composition within several objects (with older apparent I-Xe ages associated with higher extraction temperatures) and the absence of primitive I-Xe ages. The span of apparent ages seen in Allende objects (10 Myr or more) is probably too long to reflect any nebular process, so at least some alteration probably occurred ont the parent body. The range in initial (Pu-244)/(U-238) ratios for the Eggs (0.003-0.014) includes the current best estimates of the bulk solar system value (0.004-0.007). For Egg 3, the Pu/U ratio varies by a factor of two between extractions, probably the result of fractionation of Pu from U among different phases.
Analyses of noble gases in whole rock samples of the howardites Bholghati and Kapoeta and grain-size separates of Kapoeta yield evidence for excesses of the Xe isotopes Xe-129 , Xe-131, Xe-132, Xe-134, and Xe-136 in a low-temperture component, similar to lunar excess fission Xe. Such a component may be able to provide chronometric information if the relative abundances of radioactive progenitors (I-129, Pu-244, and U-238) can be determined, but the isotopic spectra obtained are not sufficiently precise to do so. Eucritic clast BH-5 in Bholghati contains Xe produced in situ by the decay of Pu-244. Calculated fission Xe retention ages are 30-70 Ma after the formation of the solar system, consistent with the apparent presence of Sm-146 decay products. Both the clast and the matrix of Bholghati have K-Ar ages of about 2 Ga, suggesting a common thermal event at least that recently.
Measurements of actinide and light REE (LREE) abundances and of phosphate abundances in equilibrated ordinary chondrites were obtained and were used to define the Pu abundance in the solar system and to determine the degree of variation of actinide and LREE abundances. The results were also used to compare directly the Pu/U ratio with the earlier obtained ratio determined indirectly, as (Pu/Nd)x(Nd/U), assuming that Pu behaves chemically as a LREE. The data, combined with high-accuracy isotope-dilution data from the literature, show that the degree of gram-scale variability of the Th, U, and LREE abundances for equilibrated ordinary chondrites is a factor of 2-3 for absolute abundances and up to 50 percent for relative abundances. The observed variations are interpreted as reflecting the differences in the compositions and/or proportions of solar nebula components accreted to ordinary chondrite parent bodies.
Some physical features of several unsteady separating turbulent boundary layers are presented for practical Reynolds numbers and reduced frequencies such as for helicopter and turbomachinery flows. The effects of unsteadiness amplitude and waveform are examined for flows along the floor of a converging and diverging wind tunnel test section. At the end of the converging portion, the mean skin friction coefficient normalized on the mean dynamic pressure is independent of the waveform and amplitude within low experimental uncertainties. In the detaching and detached portions of the flow, wall values of the fraction of time that the flow moves downstream of gamma sub pu, which is a separated flow state variable, shows that oscillation waveform and amplitude strongly influence the detached flow behavior. Distributions of gamma sub pu during a cycle indicate hysteresis within the detached flow and the effects of the higher harmonics of pressure gradient and velocity.
Possible evidence for the presence of Cm-248 in the early solar system was reported from fission gas studies (Rao and Gopalan, 1973) and recently from studies of very high nuclear track densities (not less than 5 x 10 exp 8/sq cm) in the merrillite of the H4 chondrite Forest Vale (F.V.) (Pellas et al., 1987). We report here an analysis of the isotopic abundances of xenon in F.V. phosphates and results of track studies in phosphate/pyroxene contacts. The fission xenon isotopic signature clearly identifies Pu-244 as the extinct progenitor. We calculate an upper limit Cm-248/Pu-244 to be less than 0.0015 at the beginning of Xe retention in F.V. phosphates. This corresponds to an upper limit of the ratio Cm-248/U-235 of not greater than 5 x 10 exp -5 further constraining the evidence for any late addition of freshly synthesized actinide elements just prior to solar system formation. The fission track density observed after annealing the phosphates at 290C (1 hr, which essentially erases spallation recoil tracks) is also in agreement with the Pu-244 abundance inferred from fission Xe. The spallation recoil tracks produced during the 76 Ma cosmic-ray exposure account for the very high track density in merrillites.