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12 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2012

Nuclear Data Sheets for A = 92

Nuclear structure and decay data pertaining to all nuclides with mass number A = 92 (As, Se, Br, Kr, Rb, Sr, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd) have been compiled and evaluated, and incorporated into the ENSDF data file. All literature available by 15 September 2012 has been considered. This evaluation supersedes the previous publication for this mass chain (Coral M. Baglin, Nuclear Data Sheets 91, 423 (2000) (November 2000 cutoff date)), and subsequent unpublished reevaluations by C.M. Baglin for {sup 92}Kr (January 2004 literature cut-off) and {sup 92}Sr (August 2003 literature cut-off).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

High resolution gamma-ray spectroscopy at GANIL

Gamma-ray spectroscopy is intensively used at GANIL to measure low lying states in exotic nuclei on the neutron-rich as well as on the neutron-deficient side of the nuclear chart. On the neutron deficient border, gamma-rays have been observed for the first time in {sup 92}Pd. The level scheme which could be established points to the role of isoscalar pairing. On the neutron rich side, the lifetime of excited states in nuclei around {sup 68}Ni have been been measured using the plunger technique. This allows us to study the evolution of collectivity in a broad range of nuclei. In 2014 GANIL will host the AGATA array for a campaign of at least 2 years. This array is based on the gamma-ray tracking technique, which allows an impressive gain in resolving power.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

Periodic domain boundary ordering in a dense molecular adlayer: Sub-saturation carbon monoxide on Pd(111)

Here, we describe a previously unreported ordered phase of carbon monoxide adsorbed on the (111) facet of single crystal palladium at near-saturation coverage. The adlayer superstructure is identified from low energy electron diffraction to be c(16×2) with respect to the underlying Pd(111) surface net. The ideal coverage is determined to be 0.6875 ML, approximately 92% of the 0.75–ML saturation coverage. Density functional theory calculations support a model for the molecular packing characterized by strips of locally-saturated (2×2) regions, with the CO bound near high-symmetry surface sites, separated by antiphase domain boundaries. The structure exists in a narrow coverage range and is prepared by heating the saturated adlayer to desorb a small fraction of the CO. Comparison of the c(16×2) domain-boundary structure with structural motifs at lower coverages suggests that between 0.6 and 0.6875 ML the adlayer order may be more strongly influenced by interadsorbate repulsion than by adsorption-site-specific interactions. The system is an example of the structural complexity that results from the compromise between adsorbate–substrate and adsorbate–adsorbate interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

A Pd(II)-Functionalized Covalent Organic Framework for Catalytic Conjugate Additions of Arylboronic Acids to β,β-Disubstituted Enones

A palladium(II)-functionalized covalent organic framework (Pd@TpBpy COF) built from 1,3,5-triformylphloroglucinol (Tp) and [2,2'-bipyridine]-5,5'-diamine (Bpy) is reported as a recyclable catalyst for conjugate additions in aqueous media. Additions of an array of stereoelectronically diverse arylboronic acid nucleophiles to β,β-disubstituted enones form a variety of ketones containing benzylic all-carbon quaternary centers in up to 92 % isolated yield. Research on the recyclability of Pd@TpBpy COF demonstrate this catalyst remains active through at least 7 cycles and shows superior stability to related MOF catalysts with bipyridine linker units.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Direct internal recycling fractions approaching unity

Direct internal recycling (DIR) refers to the process of recovering pure hydrogen isotopes (D/T) from helium and other impurities in the fusion plasma exhaust and directing them back to the fuel injection system. Increasing the exhaust fraction purified through DIR significantly reduces the size and cost of the tritium plant and provides additional benefits including reduced requirements for both the tritium startup inventory and tritium breeding ratio. Metal foil pumps (MFPs) are the dominant technology for this separation, relying on the concept of superpermeation. We recently demonstrated that PdCu foils operated at low temperature provide both exceptional flux and resilience to helium absorption as the DIR fraction is increased. Herein we design and demonstrate continuous and semi-batch DIR processes using PdCu MFPs. Under continuous processing, stable performance was observed for DIR fractions up to 92 %. In addition, we demonstrate a semi-batch process capable of extending the DIR fraction to unity (> 99.8 %). Under the experimental conditions described within a PdCu MFP area of ~22 m 2 would be sufficient to process the fusion exhaust with 92 % DIR fraction at expected flowrates of 100 Pa·m 3 ·s -1 for a future fusion power plant.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

In Situ Dispersion of Palladium on TiO 2 During Reverse Water–Gas Shift Reaction: Formation of Atomically Dispersed Palladium

The application of single-atom catalysts (SACs) to high-temperature hydrogenation requires materials that thermodynamically favor metal atom isolation over cluster formation. Here, we show that Pd can be predominantly dispersed as isolated atoms onto TiO 2 during the reverse water-gas shift (rWGS) reaction at 400 °C. Achieving atomic dispersion requires an artificial increase of the absolute TiO 2 surface area by an order of magnitude and can be accomplished by physically mixing a precatalyst (Pd/TiO 2 ) with neat TiO 2 prior to the rWGS reaction. Furthermore, the in situ dispersion of Pd was reflected through a continuous increase of rWGS activity over 92 h and supported by kinetic analysis, infrared and X-ray absorption spectroscopies and scanning transmission electron microscopy. The thermodynamic stability of Pd under high-temperature rWGS conditions is associated with Pd-Ti coordination, which manifests upon O-vacancy formation and the artificial increase in TiO 2 surface area.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Catalytic Hydrogenation of Alkylphenols for Renewable Caprolactone

Selective hydrogenation of lignin-derived alkyl-phenol to alkyl-cyclohexanone is a key step in the synthesis of renewable caprolactone from lignin-derived monomers. Selective hydrogenation of p-cresol, a model compound for lignin-derived monomers, to 4-methyl-cyclohexanone was conducted using Pd/γ-Al 2 O 3 in a continuous three-phase flow reactor with side products of 4-methyl cyclohexanol. High conversion (85%) and selectivity (>93%) were demonstrated at ambient reaction pressure. Evaluation of the hydrogenation at different reaction parameters showed that the reaction selectivity was determined by the surface coverage of p-cresol and 4-methyl cyclohexanone. Furthermore, high selectivity to 4-methyl cyclohexanone was also attributed to the lower apparent activation barrier of p-cresol hydrogenation (67 ± 2 kJ mol –1 ) compared to that of hydrogenation 4-methyl cyclohexanone (92 ± 11 kJ mol –1 ), with a faster rate of initial hydrogenation of p-cresol relative to carbonyl hydrogenation of 4-methyl-cyclohexanone.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Nuclear matrix elements from direct lifetime or cross-section measurements

The method of simultaneous lifetime and g factor measurements using a plunger device and the RDDS and TDRIV techniques is introduced. Results on lifetimes and hyperfine-interaction parameters for 2{sup +}{sub 1} states in {sup 104-108}Pd, {sup 96,98,104}Ru, and {sup 92,94}Zr, using a plunger device. Another method to obtain electromagnetic matrix elements is direct cross section measurements using NRF. The method is outlined, and some recent results on {sup 76}Se are shown.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

SU-F-T-49: Dosimetry Parameters and TPS Commissioning for the CivaSheet Directional Pd-103 Brachytherapy Source

Purpose: The CivaSheet is a new LDR Pd-103 brachytherapy device offering directional-radiation for preferentially irradiating malignancies with healthy-tissue sparing. Observations are presented on dosimetric characterization, TPS commissioning, and evaluation of the dosesuperposition- principle for summing individual elements comprising a planar CivaSheet Methods: The CivaSheet comprises individual sources (CivaDots, 0.05cm thick and 0.25cm diam.) inside a flexible bioabsorbable substrate with a 0.8cm center-to-center rectangular array. All non-radioactive components were measured to ensure accuracy of manufacturer-provided dimensional information. The Pd spatial distribution was gleaned from radioactive and inert samples, then modeled with the MCNP6 radiation-transport-code. A 6×6 array CivaSheet was modeled to evaluate the dose superposition principle for treatment planning. Air-kerma-strength was estimated using the NIST WAFAC geometry. Absorbed dose was estimated in water with polar sampling covering 0.05≤r≤15cm in 0.05cm increments and 0°≤θ≤180° in 1° increments. These data were entered into VariSeed9.0 and tested for the dose-superposition-principle. Results: The dose-rate-constant was 0.579 cGy/h/U with g(r) determined along the rotational-axis of symmetry (0°) instead of 90°. gP(r) values at 0.1, 0.5, 2, 5, and 10cm were 1.884, 1.344, 0.558, 0.088, and 0.0046. F(r,θ) decreased between 0° and 180° by factors of 270, 23, and 5.1 at 0.1, 1, and 10cm. The highest dose-gradient was at 92°, changing by a factor of 3 within 1° due to Au-foil shielding. TPS commissioning from 0.1≤r≤11cm and 0°≤θ≤180° demonstrated 2% reproducibility of input data except at the high-dose-gradient where interpolations caused 3% differences. Dose superposition of CivaDots replicated a multi-source CivaSheet array within 2% except where another CivaDot was present. Following implantation, the device is not perfectly planar. TPS accuracy utilizing the dose-superposition-principle through geometric repositioning of CivaDots supersedes TPS limitations of intersource shielding effects Conclusion: Dosimetric characterization, source commissioning, and evaluation of the dose-superposition-principle with VariSeed9.0 permits treatment planning for the CivaSheet brachytherapy device. Research supported in part by CivaTech Oncology, Inc.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2020

Development of an autothermal formate-based hydrogen generator: From optimization of formate dehydrogenation conditions to thermal integration with Fuel Cells

Formate received significant attention for storing H2 in chemical bonds using the concept of H2 carriers. In this report, hydrogen generation from formate was optimized systematically by varying reaction variables. Initial mass activity with a turnover frequency of 3200 molH2 molPd–1 h–1 and 92% H2 yield were obtained in sodium formate (7 M 2.0 mL) dehydrogenation over Pd(3 wt %)/C at 80 °C. Influence of formate cations (Na, K, and NH4) on dehydrogenation was also elucidated, presenting that the fastest initial reaction kinetics was achieved with ammonium formate, whereas the highest H2 yield was obtained with potassium formate (PF) in multiple catalyst recycle tests. Finally, an on-site power generation system was integrated, where a proton exchange membrane fuel cell (PEMFC) was operated in conjunction with H2 produced from the custom developed semibatch dehydrogenation reactors. The system operation was demonstrated with continuous feeding of PF to generate H2 and power on demand without an external heat source by utilizing waste heat produced from the PEMFC in a highly efficient manner.

formate dehydrogenation, optimization of reaction ↗
DOE OSTI2014

On the feasibility of polyurethane based 3D dosimeters with optical CT for dosimetric verification of low energy photon brachytherapy seeds

Purpose: To investigate the feasibility of and challenges yet to be addressed to measure dose from low energy (effective energy <50 keV) brachytherapy sources (Pd-103, Cs-131, and I-125) using polyurethane based 3D dosimeters with optical CT. Methods: The authors' evaluation used the following sources: models 200 (Pd-103), CS-1 Rev2 (Cs-131), and 6711 (I-125). The authors used the Monte Carlo radiation transport code MCNP5, simulations with the ScanSim optical tomography simulation software, and experimental measurements with PRESAGE{sup ®} dosimeters/optical CT to investigate the following: (1) the water equivalency of conventional (density = 1.065 g/cm{sup 3}) and deformable (density = 1.02 g/cm{sup 3}) formulations of polyurethane dosimeters, (2) the scatter conditions necessary to achieve accurate dosimetry for low energy photon seeds, (3) the change in photon energy spectrum within the dosimeter as a function of distance from the source in order to determine potential energy sensitivity effects, (4) the optimal delivered dose to balance optical transmission (per projection) with signal to noise ratio in the reconstructed dose distribution, and (5) the magnitude and characteristics of artifacts due to the presence of a channel in the dosimeter. Monte Carlo simulations were performed using both conventional and deformable dosimeter formulations. For verification, 2.8 Gy at 1 cm was delivered in 92 h using an I-125 source to a PRESAGE{sup ®} dosimeter with conventional formulation and a central channel with 0.0425 cm radius for source placement. The dose distribution was reconstructed with 0.02 and 0.04 cm{sup 3} voxel size using the Duke midsized optical CT scanner (DMOS). Results: While the conventional formulation overattenuates dose from all three sources compared to water, the current deformable formulation has nearly water equivalent attenuation properties for Cs-131 and I-125, while underattenuating for Pd-103. The energy spectrum of each source is relatively stable within the first 5 cm especially for I-125. The inherent assumption of radial symmetry in the TG43 geometry leads to a linear increase in sample points within the 3D dosimeter as a function of distance away from the source, which partially offsets the decreasing signal. Simulations of dose reconstruction using optical CT showed the feasibility of reconstructing dose out to a radius of 10 cm without saturating projection images using an optimal dose and high dynamic range scanning; the simulations also predicted that reconstruction artifacts at the channel surface due to a small discrepancy in refractive index should be negligible. Agreement of the measured with calculated radial dose function for I-125 was within 5% between 0.3 and 2.5 cm from the source, and the median difference of measured from calculated anisotropy function was within 5% between 0.3 and 2.0 cm from the source. Conclusions: 3D dosimetry using polyurethane dosimeters with optical CT looks to be a promising application to verify dosimetric distributions surrounding low energy brachytherapy sources.

07 ISOTOPE AND RADIATION SOURCES↗