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At least 469 records · Page 26

In Vitro Dissolution Tests of Plutonium and Americium Containing Contamination Originating From ZPPR Fuel Plates

Assessing the extent of internal dose is of concern whenever workers are exposed to airborne radionuclides or other contaminants. Internal dose determinations depend upon a reasonable estimate of the expected biological half-life of the contaminants in the respiratory tract. One issue with refractory elements is determining the dissolution rate of the element. Actinides such as plutonium (Pu) and Americium (Am) tend to be very refractory and can have biological half-lives of tens of years. In the event of an exposure, the dissolution rates of the radionuclides of interest needs to be assessed in order to assign the proper internal dose estimates. During the November 2011 incident at the Idaho National Laboratory (INL) involving a ZPPR fuel plate, air filters in a constant air monitor (CAM) and a giraffe filter apparatus captured airborne particulate matter. These filters were used in dissolution rate experiments to determine the apparent dissolution half-life of Pu and Am in simulated biological fluids. This report describes these experiments and the results. The dissolution rates were found to follow a three term exponential decay equation. Differences were noted depending upon the nature of the biological fluid simulant. Overall, greater than 95% of the Pu and 93% of the Am were in a very slow dissolving component with dissolution half-lives of over 10 years.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Predicted Radiation Output from Several Kilograms of Plutonium Oxide

Neutron and gamma signatures from 3.44 kg of plutonium oxide were predicted with MCNP6 in anticipation of a passive diagnostic measurement campaign. Calculated radiation fields are visualized through use of “FMESH” type tallies. This work is effectively an extension of previous efforts and application of MISC for the photon source term is the main advancement. Large sources of modeling uncertainty include physical can dimensions and thus internal volume and density estimates. Material age is unknown and will also affect the passive gamma signature. The measurement campaign will provide information for model refinement and subsequent simulations. The authors have requested passive data collection on the pair of cans with the largest and smallest mass and such data will be valuable for benchmarking purposes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Plutonium Oxide Containment and the Potential for Water-Borne Transport as a Consequence of ARIES Oxide Processing Operations

The question of oxide containment during processing and storage has become a primary concern when considering the continued operability of the Plutonium Facility (PF-4) at Los Alamos National Laboratory (LANL). An Evaluation of the Safety of the Situation (ESS), “Potential for Criticality in a Glovebox Due to a Fire” (TA55-ESS-14-002-R2, since revised to R3) first issued in May, 2014 summarizes these concerns: “The safety issue of fire water potentially entering a glovebox is: the potential for the water to accumulate in the bottom of a glovebox and result in an inadvertent criticality due to the presence of fissionable materials in the glovebox locations and the increased reflection and moderation of neutrons from the fire water accumulation.” As a result, the existing documented safety analysis (DSA) was judged inadequate and, while it explicitly considered the potential for criticality resulting from water intrusion into gloveboxes, criticality safety evaluation documents (CSEDs) for the affected locations did not evaluate the potential for fire water intrusion into a glovebox.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Streamlined Approach for Environmental Restoration (SAFER) Plan for Corrective Action Unit 411: Double Tracks Plutonium Dispersion (Nellis), Nevada Test and Training Range, Nevada (Rev. 0)

This Streamlined Approach for Environmental Restoration (SAFER) Plan addresses the actions needed to achieve closure for Corrective Action Unit (CAU) 411, Double Tracks Plutonium Dispersion (Nellis). CAU 411 is located on the Nevada Test and Training Range and consists of a single corrective action site (CAS), NAFR-23-01, Pu Contaminated Soil. There is sufficient information and historical documentation from previous investigations and the 1996 interim corrective action to recommend closure of CAU 411 using the SAFER process. Based on existing data, the presumed corrective action for CAU 411 is clean closure. However, additional data will be obtained during a field investigation to document and verify the adequacy of existing information, and to determine whether the CAU 411 closure objectives have been achieved. This SAFER Plan provides the methodology to gather the necessary information for closing the CAU. The results of the field investigation will be presented in a closure report that will be prepared and submitted to the Nevada Division of Environmental Protection (NDEP) for review and approval. The site will be investigated based on the data quality objectives (DQOs) developed on November 20, 2014, by representatives of NDEP, the U.S. Air Force (USAF), and the U.S. Department of Energy (DOE), National Nuclear Security Administration Nevada Field Office. The DQO process was used to identify and define the type, amount, and quality of data needed to determine whether CAU 411 closure objectives have been achieved. The following text summarizes the SAFER activities that will support the closure of CAU 411; Collect environmental samples from designated target populations to confirm or disprove the presence of contaminants of concern (COCs) as necessary to supplement existing information; If COCs are no longer present, establish clean closure as the corrective action; If COCs are present, the extent of contamination will be defined and further corrective actions will be evaluated with the stakeholders (NDEP, USAF); and Confirm the preferred closure option is sufficient to protect human health and the environment.

54 ENVIRONMENTAL SCIENCES↗

Corrective Action Decision Document for Corrective Action Unit 568. Area 3 Plutonium Dispersion Sites, Nevada National Security Site, Nevada Revision 0

The purpose of this Corrective Action Decision Document is to identify and provide the rationale for the recommendation of corrective action alternatives (CAAs) for the 14 CASs within CAU 568. Corrective action investigation (CAI) activities were performed from April 2014 through May 2015, as set forth in the Corrective Action Investigation Plan for Corrective Action Unit 568: Area 3 Plutonium Dispersion Sites, Nevada National Security Site, Nevada; and in accordance with the Soils Activity Quality Assurance Plan, which establishes requirements, technical planning, and general quality practices. The purpose of the CAI was to fulfill data needs as defined during the DQO process. The CAU 568 dataset of investigation results was evaluated based on a data quality assessment. This assessment demonstrated that the dataset is complete and acceptable for use in fulfilling the DQO data needs. Based on the evaluation of analytical data from the CAI, review of future and current operations at the 14 CASs, and the detailed and comparative analysis of the potential CAAs, the following corrective actions are recommended for CAU 568: • No further action is the preferred corrective action for CASs 03-23-17, 03-23-22, 03-23-26. • Closure in place is the preferred corrective action for CAS 03-23-19; 03-45-01; the SE DCBs at CASs 03-23-20, 03-23-23, 03-23-31, 03-23-32, 03-23-33, and 03-23-34; and the Pascal-BHCA at CAS 03-23-31. • Clean closure is the preferred corrective action for CASs 03-08-04, 03-23-30, and 03-26-04; and the four well head covers at CASs 03-23-20, 03-23-23, 03-23-31, and 03-23-33.

54 ENVIRONMENTAL SCIENCES↗

Corrective Action Investigation Plan for Corrective Action Unit 413: Clean Slate II Plutonium Dispersion (TTR) Tonopah Test Range, Nevada (Rev. 1)

Corrective Action Unit (CAU) 413 is located on the Tonopah Test Range, which is approximately 130 miles northwest of Las Vegas, Nevada, and approximately 40 miles southeast of Tonopah, Nevada. The CAU 413 site consists of the release of radionuclides to the surface and shallow subsurface from the conduct of the Clean Slate II (CSII) storage–transportation test conducted on May 31, 1963. CAU 413 includes one corrective action site (CAS), TA-23-02CS (Pu Contaminated Soil). The known releases at CAU 413 are the result of the atmospheric deposition of contamination from the 1963 CSII test. The CSII test was a non-nuclear detonation of a nuclear device located inside a reinforced concrete bunker covered with 2 feet of soil. This test dispersed radionuclides, primarily plutonium, on the ground surface. The presence and nature of contamination at CAU 413 will be evaluated based on information collected from a corrective action investigation (CAI). The investigation is based on the data quality objectives (DQOs) developed on June 17, 2015, by representatives of the Nevada Division of Environmental Protection; the U.S. Air Force; and the U.S. Department of Energy (DOE), National Nuclear Security Administration Nevada Field Office. The DQO process was used to identify and define the type, amount, and quality of data needed to develop and evaluate appropriate corrective actions for CAU 413. The CAI will include radiological surveys, geophysical surveys, collection and analyses of soil samples, and assessment of investigation results. The collection of soil samples will be accomplished using both probabilistic and judgmental sampling approaches. To facilitate site investigation and the evaluation of DQO decisions, the releases at CAU 413 have been divided into seven study groups.

54 ENVIRONMENTAL SCIENCES↗

NaI Measurements of Plutonium & Other Sources with the INL Coin

This report is a presentation for the NEOD training course at SNL. Its purpose is to summarize the effects of the INL coin on gamma ray spectra for 60 Co, 137 Cs, and plutonium. Spectra recorded with and without the INL Coin illustrate how transmission plays a role in the dose-ratio factors written on the coin.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Generalized Rate Theory for Void and Bubble Swelling and its Application to Plutonium Metal Alloys

In the classical rate theory for void swelling, vacancies and self-interstitials are produced by radiation in equal numbers, and in addition, thermal vacancies are also generated at the sinks, primarily at edge dislocations, at voids, and at grain boundaries. In contrast, due to the high formation energy of self-interstitials for normal metals and alloys, their thermal generation is negligible, as pointed out by Bullough and Perrin. However, recent DFT calculations of the formation energy of self-interstitial atoms in bcc metals have revealed that the sum of formation and migration energies for self-interstitials atoms (SIA) is of the same order of magnitude as for vacancies. The ratio of the activation energies for thermal generation of SIA and vacancies is presented. For fcc metals, this ratio is around three, but for bcc metals it is around 1.5. Reviewing theoretical predictions of point defect properties in δ-Pu, this ratio could possibly be less than one. As a result, thermal generation of SIA in bcc metals and in plutonium must be taken into considerations when modeling the growth of voids and of helium bubbles, and the classical rate theory (CRT) for void and bubble swelling must be extended to a generalized rate theory (GRT).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Aerosol Physics Considerations for Using Cerium Oxide CeO 2 as a Surrogate for Plutonium Oxide PuO 2 in Airborne Release Fraction Measurements for Storage Container Investigations

Cerium oxide (CeO2) dust is recommended as a surrogate for plutonium oxide (PuO2) in airborne release fraction experiments. The total range of applicable particle sizes for PuO2 extends from 0.0032 μm (the diameter of a single PuO2 molecule) to 10 μm (the defined upper boundary for respirable particles). For particulates with a physical particle diameter of 1.0 μm, the corresponding aerodynamic diameters for CeO2 and PuO2 are 2.7 μm and 3.4 μm, respectively. Cascade impactor air samplers are capable of measuring the size distributions of CeO2 or PuO2 particulates. In this document, the aerodynamic diameters for CeO2 and PuO2 were calculated for seven different physical diameters (0.0032, 0.02, 0.11, 0.27, 1.0, 3.2, and 10 μm). For cascade impactor measurements, CeO2 and PuO2 particulates with the same physical diameter would be collected onto the same or adjacent collection substrates. The difference between the aerodynamic diameter of CeO2 and PuO2 particles (that have the same physical diameter) is 39% of the resolution of a twelve-stage MSP Inc. 125 cascade impactor, and 34% for an eight-stage Andersen impactor. An approach is given to calculate the committed effective dose (CED) coefficient for PuO2 aerosol particles, compared to a corresponding aerodynamic diameter of CeO2 particles. With this approach, use of CeO2 as a surrogate for PuO2 material would follow a direct conversion based on a molar equivalent. In addition to the analytical information developed for this document, several US national labs have published articles about the use of CeO2 as a PuO2 surrogate. Different physical and chemical aspects were considered by these investigators, including thermal properties, ceramic formulations, cold pressing, sintering, molecular reactions, and mass loss in high temperature gas flows. All of those US national lab studies recommended the use of CeO2 as a surrogate material for PuO2.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Corrective Action Decision Document/Corrective Action Plan for Corrective Action Unit 413: Clean Slate II Plutonium Dispersion (TTR) Tonopah Test Range, Nevada. Revision 0

This Corrective Action Decision Document/Corrective Action Plan provides the rationale and supporting information for the selection and implementation of corrective actions at Corrective Action Unit (CAU) 413, Clean Slate II Plutonium Dispersion (TTR). CAU 413 is located on the Tonopah Test Range and includes one corrective action site, TA-23-02CS. CAU 413 consists of the release of radionuclides to the surface and shallow subsurface from the Clean Slate II (CSII) storage–transportation test conducted on May 31, 1963. The CSII test was a non-nuclear detonation of a nuclear device located inside a concrete bunker covered with 2 feet of soil. To facilitate site investigation and the evaluation of data quality objectives decisions, the releases at CAU 413 were divided into seven study groups: 1 Undisturbed Areas 2 Disturbed Areas 3 Sedimentation Areas 4 Former Staging Area 5 Buried Debris 6 Potential Source Material 7 Soil Mounds Corrective action investigation (CAI) activities, as set forth in the CAU 413 Corrective Action Investigation Plan, were performed from June 2015 through May 2016. Radionuclides detected in samples collected during the CAI were used to estimate total effective dose using the Construction Worker exposure scenario. Corrective action was required for areas where total effective dose exceeded, or was assumed to exceed, the radiological final action level (FAL) of 25 millirem per year. The results of the CAI and the assumptions made in the data quality objectives resulted in the following conclusions: The FAL is exceeded in surface soil in SG1, Undisturbed Areas; The FAL is assumed to be exceeded in SG5, Buried Debris, where contaminated debris and soil were buried after the CSII test; The FAL is not exceeded at SG2, SG3, SG4, SG6, or SG7. Because the FAL is exceeded at CAU 413, corrective action is required and corrective action alternatives (CAAs) must be evaluated. For CAU 413, three CAAs were evaluated: no further action, clean closure, and closure in place. The CAAs were evaluated on technical merit focusing on performance, reliability, feasibility, safety, and cost. Based on the evaluation of analytical data from the CAI, review of future and current operations at CAU 413, and the detailed and comparative analysis of CAAs, clean closure was selected as the preferred CAA for CAU 413 by the U.S. Air Force, Nevada Division of Environmental Protection, and U.S. Department of Energy at the CAA meeting held on August 24, 2016.

54 ENVIRONMENTAL SCIENCES↗

Corrective Action Decision Document/Corrective Action Plan for Corrective Action Unit 414: Clean Slate III Plutonium Dispersion (TTR) Tonopah Test Range, Nevada, Revision 1

This Corrective Action Decision Document/Corrective Action Plan provides the rationale and supporting information for the selection and implementation of corrective actions at Corrective Action Unit (CAU) 414, Clean Slate III Plutonium Dispersion (TTR). This document has been developed in accordance with the Federal Facility Agreement and Consent Order. CAU 414 is located on the Tonopah Test Range and includes one corrective action site, TA-23-03CS, Pu Contaminated Soil.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Closure Report for Corrective Action Unit 413: Clean Slate II Plutonium Dispersion (TTR) Tonopah Test Range, Nevada, Revision 0

This Closure Report (CR) presents information supporting the closure of Corrective Action Unit (CAU) 413: Clean Slate II Plutonium Dispersion (TTR), located on the Tonopah Test Range, Nevada. CAU 413 consists of the release of radionuclides to the surface and shallow subsurface from the conduct of the Clean Slate II storage-transportation test conducted on May 31, 1963. The purpose of this CR is to provide documentation and justification for the clean closure of CAU 413 under the FFACO without further corrective action. This justification is based on historical knowledge of the site, previous site investigations, closure activities conducted at the site, and the results of verification samples. Clean closure activities included excavating and disposing of radiologically contaminated soil and debris in the vicinity of ground zero, and collecting verification samples to support the corrective action of clean closure. Results confirmed that further corrective action is not required at CAU 413. Based on the corrective action activities conducted, clean closure of the site is complete; the closure objectives established in the CADD/CAP have been achieved; and no further corrective action at the site is required.

54 ENVIRONMENTAL SCIENCES↗

Surplus Plutonium Disposition Sphincter Seal Development & Testing

The Surplus Plutonium Disposition Project (SPD, Project Y744) requested the Savannah River National Laboratory (SRNL) to perform a series of leak and durability tests on sphincter seals that were designed to process blend cans and shield cans into an SPD glovebox. Each sphincter seal assembly consisted of a stainless-steel outer sleeve weldment that was bolted onto the test enclosure and an aluminum inner sleeve that housed seven to nine Neoprene seals. All tests were executed to determine long term effects from processing approximately a year’s worth of blend and shield cans through the sphincter seals.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Characterization of Impure Plutonium Oxide Neutron Calibration Standards through Evaluation by Neutron Multiplicity Equations

Plutonium oxide calibration standards STD4C, STD6C and STD8C have been historically used, and are currently the only MT52 standards in use, for calibration and measurement control program of Passive/Active Neutron Coincidence Counter known as PAN1 at PF-4. In this paper, previously measured high-statistics data are used in conjunction with neutron multiplicity equations to determine multiplication M and α parameter of these standards as the explicit knowledge of these parameters may allow quantification of precision and bias of accountability measurements of different material types and matrices of items.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Indications of flat bands driving the δ to α volume collapse of plutonium

On cooling from the melt, plutonium (Pu) undergoes a series of structural transformations accompanied by a ≈ 28% reduction in volume from its δ phase to its α phase at low temperatures. While Pu’s partially filled 5f -electron shells are known to be involved, their precise role in the transformations has remained unclear. By using calorimetry measurements on α-Pu and gallium-stabilized δ-Pu combined with resonant ultrasound and X-ray scattering data to account for the anomalously large softening of the lattice with temperature, we show here that the difference in electronic entropy between the α and δ phases dominates over the difference in phonon entropy. Rather than finding an electronic specific heat characteristic of broad $f$-electron bands in α-Pu, as might be expected to occur within a Kondo collapsed phase in analogy with cerium, we find it to be indicative of flatter subbands. An important role played by Pu’s 5$f$ electrons in the formation of its larger unit cell α phase comprising inequivalent lattice sites and varying bond lengths is therefore suggested.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗