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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Copper Causes Regiospecific Formation of C4F8-Containing Six-Membered Rings and their Defluorination/Aromatization to C4F4-Containing Rings in Triphenylene/1,4-C4F8I2 Reactions

The presence of Cu in reactions of triphenylene (TRPH) and 1,4-C4F8I2 at 360 °C led to regiospecific substitution of TRPH ortho C(β) atoms to form C4F8-containing rings, completely suppressing substitution on C(α) atoms. In addition, Cu caused selective reductive-defluorination/aromatization (RD/A) to form C4F4- containing aromatic rings. Without Cu, the reactions of TRPH and 1,4- C4F8I2 were not regiospecific and no RD/A was observed. These results, supported by DFT calculations, are the first examples of Cupromoted (i) regiospecific perfluoroannulation, (ii) preparative C–F activation, and (iii) RD/A. HPLC-purified products were characterized by X-ray diffraction, low-temperature PES, and 1H/19F NMR.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2014

A Ni(II) Bis(diphosphine)-Hydride Complex Containing Proton Relays - Structural Characterization and Electrocatalytic Studies

The syntheses of the new 1,5-diphenyl-3,7-di(isopropyl)-1,5-diaza-3,7-diphosphacyclooctane ligand, PiPr2NPh2, is reported. The two equivalents of the ligand react with [Ni(CH3CN)6](BF4)2 to form the bis-diphosphine Ni(II)-complex [Ni(PiPr2NPh2)2](BF4)2, which acts as a proton reduction electrocatalyst. In addition to [Ni(PiPr2NPh2)2]2+, we report the syntheses and structural characterization of the Ni(0)-complex Ni(PiPr2NPh2)2, and the Ni(II)-hydride complex [HNi(PiPr2NPh2)2]BF4. The [HNi(PiPr2NPh2)2]BF4 complex represents the first Ni(II)-hydride in the [Ni(PR2NR'2)2]2+ family of compounds to be isolated and structurally characterized. In addition to the experimental data, the mechanism of electrocatalysis facilitated by [Ni(PiPr2NPh2)2]2+ is analyzed using linear free energy relationships recently established for the [Ni(PR2NR'2)2]2+ family. We thank Dr. Aaron Appel, Dr. Simone Raugei and Dr. Eric Wiedner for helpful discussions. This research was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Mass spectrometry was provided at W. R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the Department of Energy’s office of Biological and Environmental Research located at Pacific Northwest National Laboratory. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy.

diphosphine↗
DOE OSTI2016

Structure and thermodynamics of uranium-containing iron garnets

Use of crystalline garnet as a waste form phase appears to be advantageous for accommodating actinides from nuclear waste. Previous studies show that large amounts of uranium (U) and its analogues such as cerium (Ce) and thorium (Th) can be incorporated into the garnet structure. In this study, we synthesized U loaded garnet phases, Ca 3 U x Zr 2–x Fe 3 O 12 (x = 0.5–0.7), along with the endmember phase, Ca 3 (Zr 2 )SiFe 3+ 2 O 12 , for comparison. The oxidation states of U were determined by X-ray photoelectron and absorption spectroscopies, revealing the presence of mixed pentavalent and hexavalent uranium in the phases with x = 0.6 and 0.7. The oxidation states and coordination environments of Fe were measured using transmission 57 Fe-Mössbauer spectroscopy, which shows that all iron is tetrahedrally coordinated Fe 3+ . U substitution had a significant effect on local environments, the extent of U substitution within this range had a minimal effect on the structure, and unlike in the x = 0 sample, Fe exists in two different environments in the substituted garnets. The enthalpies of formation of garnet phases from constituent oxides and elements were first time determined by high temperature oxide melt solution calorimetry. The results indicate that these substituted garnets are thermodynamically stable under reducing conditions. Furthermore, our structural and thermodynamic analysis further provides explanation for the formation of natural uranium garnet, elbrusite-(Zr), and supports the potential use of Ca 3 U x Zr 2–x Fe 3 O 12 as viable waste form phases for U and other actinides.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Cobalt Complexes Containing Pendant Amines in the Second Coordination Sphere as Electrocatalysts for H2 Production

A series of heteroleptic 17e- cobalt complexes, [CpCoII(PtBu2NPh2)](BF4), [CpC6F5CoII(PtBu2NPh2)](BF4), [CpC5F4NCoII(PtBu2NPh2)](BF4), [where P2tBuN2Ph = 1,5-diphenyl-3,7-di(tert-butyl)-1,5-diaza-3,7-diphosphacyclooctane, CpC6F5 = C5H4(C6F5), and CpC5F4N = C5H4(C5F4N)] were synthesized, and structures of all three were determined by X-ray crystallography. Electrochemical studies showed that the CoIII/II couple of [CpC5F4NCoII(PtBu2NPh2)]+ appears 250 mV positive of the CoIII/II couple of [CpCoII(PtBu2NPh2)] as a result of the strongly electron-withdrawing perfluorpyridyl substituent on the Cp ring. Reduction of these paramagnetic CoII complexes by KC8 led to the diamagnetic 18e- complexes CpICo(PtBu2NPh2), CpC6F5CoI(PtBu2NPh2), CpC5F4NCoI(PtBu2NPh2), which were also characterized by crystallography. Protonation of these neutral CoI complexes led to the cobalt hydrides [CpCoIII(PtBu2NPh2)H](BF4), [CpC6F5CoIII(PtBu2NPh2)H](BF4), and [CpC5F4NCoIII(PtBu2NPh2)H](BF4). The cobalt hydride with the most electron-withdrawing Cp ligand, [CpC5F4NCoIII(PtBu2NPh2)H]+ is an electrocatalyst for production of H2 using 4-MeOC6H4NH3BF4 (pKaMeCN = 11.86) with a turnover frequency of 350 s-1 and an overpotential of 0.75 V. Experimental measurement of thermochemical data provided further insights into the thermodynamics of H2 elimination. This research was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy.

hydrogen, catalysis, electrocatalysis, proton rela↗
DOE OSTI2022

Container Evaluation: Analysis of the Swagelok Knuckle with Viewport as an Approved Hermetically Sealed Inner Container

This report outlines the results from the water ingress test, helium leak test and additional atmosphere testing for the Swagelok knuckle with viewport container further referred to as the SKV. This container is constructed from a standard union vacuum fitting, 1.33” conflat to 0.5” male VCR, a 1.33” conflat fused silica lensed viewport fitting, and a 0.5 inch VCR cap. The primary intended use of this container is to store Pu metal samples in the vault for a time interval exceeding 40 years. The samples need to be contained in an air free environment to ensure that the material does not oxidize over time. The container viewport is a critical design feature that will help the operators visually inspect and evaluate the state of the metal samples prior to opening the container. These containers are advertised as leak tight, but experimental tests were performed to test the water resistant criteria and the gas leaking criteria set forth by the TA-55 Criticality Safety Program. The results of the water ingress test show that the container is water-tight, with no signs of water penetrating the container within the required guidelines outlined in TA55-AP-522. The preliminary He leak test performed demonstrate that the conflat window port and VCR cap are able to maintain a hermetic seal. Additionally, all containers will be He leak tested independently by the manufacturer prior to shipping to LANL. A third voluntary test was added to assess the container’s ability to hold atmosphere, with successful results indicating the container is able to hold inert atmosphere to prevent lanthanum metal oxidation. It is the conclusion of the authorsthat there is enough evidence through the test conducted and outlined within this document that the proposed container meets the definition of a water-tight container, and it is able to provide a hermetic seal.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Performance Analyses of Passive Containment Cooling System for a Concrete Type Containment

The containment of nuclear power plants is the final barrier to keep the radioactive materials from uncontrolled release to the environment. To keep the containment integrity, pressure and temperature must be controlled by the spray system which relies on active components for PWRs with a concrete containment. To achieve a passive means to keep the containment integrity, therefore, cooling should be achieved by forming a natural circulation loop between internal cooling devices connected to an external heat sink. A system like this is often called Passive Containment Cooling System (PCCS). In the early phase of APR-1400 development, this concept was studied and VVER-1200 is also known to adopt the PCCS. The PCCS consists of a cooling device installed at the inside of the containment which is a tube-bank type heat exchanger where cooling occurs at the exterior of the tubes and a heat sink which is called Passive Containment Cooling Tank (PCCT) located at the outside of the containment on the top of the auxiliary building. In this paper, we introduce performance analysis results, utilizing the GOTHIC computer code. The PCCS performance analysis model was developed for APR-1400 which has a thermal power of 4000 MW and considers PCCS as an option to improve its safety characteristics. The PCCS which is considered in this paper is to cope with both Design Basis and Severe Accidents, considering SBO conditions. The pressure and temperature transients due to the Loss of Coolant Accident (LOCA) were analyzed with and without PCCS together with a normal case using the spray system. And, in particular, limitations of the PCCS in regard to mission time will be discussed. Through this study, it was found that the PCCS being considered as an option to improve the safety of APR-1400 can have almost same capability to control the containment pressure for LBLOCA as the containment spray system does. Although it would depends on the heat removal capacity of a given design such as the size of the heat transfer area, the PCCS could even replace the containment spray system. However, the PCCS may lose its capability after 24 hours as its temperature reaches that of the containment atmosphere. To extend the mission time of PCCS, either cooling or supplementary cold water needs to be provided to the external heat sink of PCCS. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2016

A Purple Cupredoxin from Nitrosopumilus maritimus Containing a Mononuclear Type 1 Copper Center with an Open Binding Site

Mononuclear cupredoxin proteins usually contain a coordinately saturated type 1 copper (T1Cu) center and function exclusively as electron carriers. Here we report a cupredoxin isolated from the nitrifying archaeon Nitrosopumilus maritimus SCM1, called Nmar1307, that contains a T1Cu center with an open binding site containing water. It displays a deep purple color due to strong absorptions around 413 nm (1880 M –1 cm –1 ) and 558 nm (2290 M –1 cm –1 ) in the UV–vis electronic spectrum. EPR studies suggest the protein contains two Cu(II) species of nearly equal population, one nearly axial, with hyperfine constant A∥ = 98 × 10 –4 cm –1 , and another more rhombic, with a smaller A∥ value of 69 × 10 –4 cm –1 . The X-ray crystal structure at 1.6 Å resolution confirms that it contains a Cu atom coordinated by two His and one Cys in a trigonal plane, with an axial H2O at 2.25 Å. Both UV–vis absorption and EPR spectroscopic studies suggest that the Nmar1307 can oxidize NO to nitrite, an activity that is attributable to the high reduction potential (354 mV vs SHE) of the copper site. These results suggest that mononuclear cupredoxins can have a wide range of structural features, including an open binding site containing water, making this class of proteins even more versatile.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Lift-based up-ender and methods using same to manipulate a shipping container containing unirradiated nuclear fuel

A shipping container containing an unirradiated nuclear fuel assembly is lifted off the ground by operating a crane to raise a lifting tool comprising a winch. The lifting tool is connected with the shipping container by a rigging line connecting with the shipping container at a lifting point located on the shipping container between the top and bottom of the shipping container, and by winch cabling connecting with the shipping container at the top of the shipping container. The shipping container is reoriented by operating the winch to adjust the length of the winch cabling so as to rotate the shipping container about the lifting point. Shortening the winch cabling rotates the shipping container about the lifting point from a horizontal orientation to a vertical orientation, while lengthening the winch cabling rotates the shipping container about the lifting point from the vertical orientation to the horizontal orientation.

42 ENGINEERING↗
DOE OSTI2015

Container inspection in the port container terminal by using 14 MeV neutrons

A proposal for an autonomous and flexible ship container inspection system is presented. This could be accomplished by the incorporation of inspection system on the container transportation devices (straddle carriers, yard gentry cranes automated guided vehicles, trailers). This configuration is terminal specific and it will be decided by container terminal operator. In such a way no part of port operational area will be used for inspection. The inspection scenario will include container transfer from ship to transportation device with inspection unit mounted on it, inspection during container movement to the container location. A neutron generator without associated alpha particle detection will be used. This will allow the use of higher neutron intensity (5x10{sup 9} - 10{sup 10} n/s in 4π). The inspected container will be stationary in the 'inspection position' on the transportation device while the 'inspection unit' will move along its side. Following analytical methods will be used simultaneously: neutron radiography, X-ray radiography, neutron activation analysis, (n,γ) and (n,n'γ) reactions, neutron absorption, and scattering, X-ray backscattering, Neutron techniques will take the advantage of using 'smart collimators' for neutrons and gammas, both emitted and detected. The inspected voxel will be defined by intersections/union of neutron generator and detectors solid angles. The container inspection protocol will be based on identification of discrepancies between its cargo manifest and its elemental 'fingerprint' and radiography profiles. In addition, the information on container weight will be obtained during the container transport and foreseen screening from the measurement of density of material in the container. (authors)

42 ENGINEERING↗
DOE OSTI2023

Water-Resistant Container Testing: A426-1000 Container Design

The purpose of this report is to detail the results of water ingress testing conducted on the A426-1000 container design and discuss these results against the water-resistant container requirements of TA55-AP- 522 and PA-RD-01009. The A426-1000 is a proposed commercially off the shelf inner container option for material storage inside of a glovebox and/or as an approved non-hermetically sealed inner of an approved packaging configuration inside of an approved outer container as listed in PA-RD-01022. The A426-1000 is shaped like a slip lid container, made of 316L stainless steel, and utilizes a smooth, threaded lid with a silicone O-ring for closure and containment. This container both lid and body is machined out of one billet piece of 316L stainless steel with no welds. See Figure 1 and Table 1 for a summary of the container specifications. For more details on the container design, see Section 1.4.

42 ENGINEERING↗
DOE OSTI2026

Water-Resistant Container Testing: A426-7, A426-25, and A426-50 Container Designs

The purpose of this report is to detail the results of water ingress testing conducted on the A426-7, A426-25, and A426-50 Mini-Pot container designs and discuss these results against the water-resistant container requirements of TA55-AP-522 and PA-RD-01009. The A426 design series is a proposed commercially off the shelf inner container option for material storage inside of a glovebox and/or as an approved nonhermetically sealed inner of an approved packaging configuration inside of an approved outer container as listed in PA-RD-01022. The A426-25 and A426-50 are shaped similar to an ointment jar, made of 316L stainless steel, and utilize a threaded lid for closure and containment. The A426-7 container is shaped similar to a vial, made of 316L stainless steel, and utilizes a threaded lid for closure and containment. See Figure 1 and Table 1-3 for a summary of the container specifications. For more details on the container design, see Section 1.4.

42 ENGINEERING↗
DOE OSTI2021

Evaluating Probability of Containment Effectiveness at a GCS Sites using integrated assessment modeling approach with Bayesian decision Networks

Improved scientific and engineering understanding of the behavior of geologic CO2 storage together with established regulatory framework and incentive structures raise the prospects for accelerated, large-scale deployment of this greenhouse gas emissions reduction approach. Incentive structures call for the establishment of appropriate verification and accounting approaches to support claims of the integrity of a geologic storage complex and to justify taking credit for long-term storage. In this study, we present a framework for assessing the probability of containment effectiveness over the lifetime of a geologic carbon storage site (e.g., after 70 years of injection and post-injection site performance) using forward stochastic model realizations based on site characterization data and using a monitoring-informed Bayesian network based on hypothetical detectability from surface seismic surveys over the site injection and post-injection phases. The National Risk Assessment Partnership’s open-source Integrated Assessment Model (NRAP-Open-IAM) was utilized to develop an ensemble of 10,000 a priori stochastic forecasts of CO2 containment. Those simulations were used to train the Bayesian network model to estimate the prior probabilities of the CO2 leakage mass into overlying, monitorable aquifers considering the uncertainties in the reservoir properties, permeability of potentially leaky wells and the overlying aquifers. The conditional probabilities in the Bayesian network were either learned from the NRAP-Open-IAM simulations or derived from the predefined detection thresholds for the monitoring method. Observations obtained from monitoring, over time during the site operation phases were then used to generate updated posterior probabilities of containment (and any loss from containment) in the Bayesian network by propagating the prior probabilities through the conditional probabilities. We demonstrate how to construct and use the Bayesian network for verifying the long-term storage complex effectiveness informed by monitoring based on the NRAP-Open-IAM simulations previously developed for the FutureGen 2.0 site. This approach may have relevance for stake holders to demonstrate secure geologic storage, provide a defensible, probabilistic approach to claim credit for geologic storage, and to estimate the likelihood that any fraction of the claimed credit may need to be refunded to the creditor based on available monitoring information.

Bayesian network, Risk assessment, Monitoring, car↗
DOE OSTI2014

Evaluating the Effects of Aluminum-Containing and Non-Aluminum Containing Deodorants on Axillary Skin Toxicity During Radiation Therapy for Breast Cancer: A 3-Armed Randomized Controlled Trial

Purpose: Deodorant use during radiation therapy for breast cancer has been controversial as there are concerns deodorant use may exacerbate axillary skin toxicity. The present study prospectively determined the use of both aluminum-containing and non aluminum containing deodorants on axillary skin toxicity during conventionally fractionated postoperative radiation therapy for breast cancer. Methods and Materials: This 3-arm randomized controlled study was conducted at a single center, tertiary cancer hospital between March 2011 and April 2013. Participants were randomized to 1 of 2 experimental groups (aluminum-containing deodorant and soap or non–aluminum containing deodorant and soap) or a control group (soap). A total of 333 participants were randomized. Generalized estimating equations were used to estimate and compare the odds of experiencing high levels of sweating and skin toxicity in each of the deodorant groups to the odds in the control group. The study evaluated a range of endpoints including objective measurements of axilla sweating, skin toxicity, pain, itch and burning. Quality of life was assessed with a validated questionnaire. Results: Radiation characteristics were similar across all groups. Patients in the deodorant groups did not report significantly different ratings for axillary pain, itch, or burning compared with the control group. Patients in the aluminum-containing deodorant group experienced significantly less sweating than the control; the odds of their sweating being barely tolerable and frequently or always interfering with their daily activities was decreased by 85% (odds ratio, 0.15; 95% confidence interval, 0.03-0.91). Conclusions: We found no evidence that the use of either aluminum-containing or non–aluminum containing deodorant adversely effects axillary skin reaction during conventionally fractionated radiation therapy for breast cancer. Our analysis also suggests patients in the aluminum-containing deodorant arm had significantly less sweating without increased symptoms of axillary radiation skin toxicity. These results add to the evidence that the prescription of deodorants during radiation therapy for breast cancer is now questionable.

62 RADIOLOGY AND NUCLEAR MEDICINE↗