Fabrication of 50-mg252Cf neutron sources for the FDA activation analysis facility

The Transuranium Processing Plant (TPP) at the Oak Ridge National Laboratory (ORNL) has been requested by the Food and Drug Administration (FDA) to furnish 200 mg of²⁵²Cf for use in their new activation analysis facility. This paper discusses the procedure to be employed in fabricating the californium into four neutron sources, each containing a nominal 50-mg of²⁵²Cf. The completed neutron sources will be assayed using a precision fast-neutron counter, decontaminated and loaded into a concreete-shielded shipping container weighing 10.7 Mg for shipment to the FDA facility located at Howard University in Washington, D. C.Research sponsored by the Office of Basic Energy Sciences, U. S. Department of Energy, under contract DE-AC05-840R21400 with Martin Marietta Energy Systems, Inc.     

Positronium formation at low temperatures: the role of trapped electrons

Measurements have been carried out of electron spin densities (by electron spin resonance technique) and positronium (Ps) formation probability as functions of Co-60 γ-irradiation dose in poly(methyl methacrylate) and linear poly(ethylene) at 77 K. We observe a linear relationship between the enhancement of the Ps formation and the density of trapped electrons in both polymers. This clear correlation strongly supports the previous suggestion by the authors that the increase in Ps formation with time (that has been observed at low temperatures for a number of polymers) can be explained as a reaction of free positrons with trapped electrons produced by the previously injected positrons.     

The design of a spin-polarized slow positron beam

Spin-polarized low-energy positrons were considered as useful probes for studying electron spin states of both surface and bulk materials. Due to the spin-dependent interactions between electrons and positrons, the formation of positronium (Ps), an electron-positron bound system, can be distinguished from different electron spin states. Recently, a positron source of ¹⁸F has been developed for a spin polarized slow positron beam at the institute of physical and chemical research (RIKEN). The design of an electrostatic positron beam will be discussed in conjunction with a spin rotator.     

Determination of cell asymmetry in temperature-modulated DSC

The quality of measurement of heat capacity by differential scanning calorimetry (DSC) is based on the symmetry of the twin calorimeters. This symmetry is of particular importance for the temperature-modulated DSC (TMDSC) since positive and negative deviations from symmetry cannot be distinguished in the most popular analysis methods. Three different DSC instruments capable of modulation have been calibrated for asymmetry using standard non-modulated measurements and a simple method is described that avoids potentially large errors when using the reversing heat capacity as the measured quantity. It consists of overcompensating the temperature-dependent asymmetry by increasing the mass of the sample pan.On leave from Toray Industries, Inc., Otsu, Shiga 520, JapanOn leave from Toray Research Center, Inc., Otsu, Shiga 520, JapanThis work was supported by the Division of Materials Research, National Science Foundation, Polymers Program, Grant # DMR 90-00520 and the Division of Materials Sciences, Office of Basic Energy Sciences, U. S. Department of Energy at Oak Ridge National Laboratory, managed by Lockheed Martin Energy Research Corp. for the U. S. Department of Energy, under contract number DE-AC0S-96OR22464. Support for instrumentation came from TA Instruments, Inc. and Mettler-Toledo, Research support was also given by ICI Painls, and Toray Industries, Inc.     

Application of positron annihilation induced Auger Electron Spectroscopy to the study of surface chemistry

Positron annihilation induced Auger Electron Spectroscopy (PAES), makes use a beam of low energy positrons to excite Auger transitions by annihilating core electrons. This novel mechanism provides PAES with a number of unique features which distinguishes it from other methods of surface analysis. In PAES the very large collisionally induced secondary electron background which is present under the low energy Auger peaks using conventional tecniques can be eliminated by using a positron beam whose energy is below the range of Auger electron energies. In addition, PAES is more surface selective than conventional Auger Spectroscopy because the PAES signal originates almost exclusively from the topmost atomic layer due to the fact that the positrons annihilating with the core electrons are trapped in an image correlation well just outside the surface. In this paper, recent applications of Positron Annihilation Induced Auger Electron Spectroscopy (PAES) to the study of surface structure and surface chemistry will be discussed including studies of the growth, alloying and inter-diffusion of ultrathin layers of metals, metals on semiconductors, and semiconductors on semiconductors. In addition, the possibilities for future application of PAES to the study of catalysis and surface chemistry will be outlined.     

Mercury speciation methods for utility flue gas

Accurate measurement of mercury speciation (Hg⁰ and Hg²⁺) in power plant flue gas is necessary to model the fate and transport of mercury in the atmosphere and understand and evaluate the effectiveness of mercury control technologies. Research work jointly sponsored by the Electric Power Research Institute (EPRI) and the U.S. Department of Energy (DOE) is currently under way at the University of North Dakota Energy & Environmental Research Center to determine whether U.S. Environmental Protection Agency (EPA) Method 29 or other methods can speciate mercury. Five different methods have been tested, and it has been found that EPA Method 29 does not speciate mercury properly in coal-generated flue gas. Two methods that show promise are the tris-buffer and the Ontario Hydro methods. Received: 2 December 1996 / Revised: 5 March 1997 / Accepted: 6 March 1997     

Photon-activation analysis of caesium

The corrosive behaviour of caesium has been attributed in part to the presence of a non-metallic impurity such as oxygen. A photon-activation method for determining oxygen and carbon in caesium is described. Scintillation coincidence-counting and pulseheight discrimination are used to count the gamma-ray activity resulting from annihilation of the positrons emitted. Variation of beam energy has been investigated in order to obtain optimum irradiation conditions. In the samples analysed and under the conditions used, less than 100 ppm of oxygen and carbon can be detected. Results are compared with those from other methods.     

Toxicologically important trace elements in Iranian diets

The intake of aluminum, arsenic, cadmium, lead and mercury via the daily diet by Iranian population groups was determined. The relevant daily diets were prepared through dietary recording and duplicate portion, and the trace elements were measured using analytical methods based on NAA, ICP and AAS. The results for the Iranian diets are discussed and compared with corresponding ones from other countries. The project has been performed in the frame of a co-ordinated research project of the International Atomic Energy Agency with participants from various countries. This revised version was published online in July 2006 with corrections to the Cover Date.     

Evaluation of elastic‐scattering cross sections for electrons and positrons over a wide energy range

Quantification of surface‐ and bulk‐analytical methods, e.g. Auger‐electron spectroscopy (AES), X‐ray photoelectron spectroscopy (XPS), electron‐probe microanalysis (EPMA), and analytical electron microscopy (AEM), requires knowledge of reliable elastic‐scattering cross sections for describing electron transport in solids. Cross sections for elastic scattering of electrons and positrons by atoms, ions, and molecules can be calculated with the recently developed code ELSEPA (Elastic Scattering of Electrons and Positrons by Atoms) for kinetic energies of the projectile from 10 eV to 50 eV. These calculations can be made after appropriate selection of the basic input parameters: electron‐density distribution, a model for the nuclear‐charge distribution, and a model for the electron‐exchange potential (the latter option applies only to scattering of electrons). Additionally, the correlation‐polarization potential and an imaginary absorption potential can be considered in the calculations. We report comparisons of calculated differential elastic‐scattering cross sections (DCSs) for silicon and gold at selected energies (500 eV, 5 keV, 30 keV) relevant to AES, XPS, EPMA, and AEM, and at 100 MeV as a limiting case. The DCSs for electrons and positrons differ considerably, particularly for medium‐ and high‐atomic‐number elements and for kinetic energies below about 5 keV. The DCSs for positrons are always monotonically decreasing functions of the scattering angle, while the DCSs for electrons have a diffraction‐like structure with several minima and maxima. A significant influence of the electron‐exchange correction is observed at 500 eV. The correlation‐polarization correction is significant for small scattering angles at 500 eV, while the absorption correction is important at energies below about 10 keV. Copyright © 2005 John Wiley & Sons, Ltd.     

Monte Carlo transport of electrons and positrons through thin foils

In measurements on electrons traversing matter it is important to know the transmission through that medium, their path-lengths and their angular distribution through matter. This allows one to seek improvement in techniques which employ electrons, including medical applications and materials irradiation. This work presents a simulation of the transport of beams of electrons and positrons through thin foils using an analog Monte Carlo code that simulates in a detailed way every electron movement or interaction in matter. As those particles penetrate thin absorbers, it has been assumed that they interact with matter only through elastic scattering, with negligible energy loss. This type of interaction has been described quite precisely because its angular form influences very much the angular distribution of electrons and positrons in matter. With this code it has been calculated that the number of particles, with energies between 100 and 3000 keV, which are transmitted through different media of various thicknesses as well as their angular distributions, show good agreement with the experimental data. The discrepancies are less than 5% for thicknesses lower than about 30% of the corresponding range in the tested material. As elastic scattering is very anisotropic, its angular distribution resembles a collimated incident beam for very thin foils, becoming slowly more isotropic when absorber thickness is increased.     

Static dipole polarizability and binding energy of sodium clusters Nan (n=1-10): A critical assessment of all-electron based post Hartree-Fock and density functional methods

A systematic all electron post Hartree-Fock as well as density functional theory (DFT) based calculations for the polarizability and binding energy of sodium metal clusters have been performed and an in-depth analysis of the discrepancy between the experimental and theoretical results is presented. A systematic investigation for the assessment of different DFT exchange-correlation functionals in predicting the polarizability values has also been reported. All the pure DFT functionals have been found to considerably underestimate the calculated polarizability values as compared to the MP2 results. DFT calculations using the full Hartree-Fock exchange along with one-parameter progressive correlation functional have, however, been shown to yield results in good agreement with the MP2 and experimental results. The possible sources of error present in the experimental measurements as well as in the different theoretical methods have also been analyzed. One of the most important conclusions of the present study is that the effect of electron correlation plays a significant role in determining the polarizability of the clusters and the MP2 method can be considered to be one of the most reliable methods for their prediction. It has also been noted that the polarizability value of the lower member clusters (Na2 and Na4) calculated by highly sophisticated methods such as, CCSD and CCSD(T) are found to be very close to the corresponding MP2 values. The polarizability and the binding energy of the clusters are found to be inversely related to each other and their correlation is rationalized by invoking the minimum polarizability principle. A good linear correlation between the polarizability and volume of the cluster has also been found to exist.     

Determination of polychlorinated biphenyl congeners and chlorinated pesticides in a fish tissue standard reference material

The concentrations of a wide range of polychlorinated biphenyl congeners (PCBs) and chlorinated pesticides in a fish tissue Standard Reference Material (SRM) have been determined using multiple methods of analysis. This material, SRM 1946, Lake Superior Fish Tissue, was recently issued by the National Institute of Standards and Technology (NIST) and complements a suite of marine environmental natural-matrix SRMs that are currently available from NIST for the determination of organic contaminants such as aliphatic hydrocarbons, polycyclic aromatic hydrocarbons (PAHs), PCBs, and chlorinated pesticides. SRM 1946 is a fresh tissue homogenate (frozen) prepared from filleted adult lake trout (Salvelinus namaycush namaycush) collected from the Apostle Islands region of Lake Superior. SRM 1946 has certified and reference concentrations for PCB congeners, including the three non- ortho PCB congeners, and chlorinated pesticides. Certified concentrations are available for 30 PCB congeners and 15 chlorinated pesticides. Reference concentrations are available for 12 PCB congeners and 2 chlorinated pesticides. In addition, SRM 1946 is characterized for additional chemical constituents and properties: fatty acids, extractable fat, methylmercury, total mercury, selected trace elements, proximates, and caloric content. The characterization of chlorinated compounds is described in this paper with an emphasis on the approach used for the certification of the concentrations of PCB congeners and chlorinated pesticides. The PCB congener and chlorinated pesticide data are also compared to concentrations in other marine natural-matrix reference materials available from NIST (fish oil, mussel tissue, whale blubber, and a second fresh frozen fish tissue homogenate prepared from filleted adult lake trout collected from Lake Michigan) and from other organizations such as the National Research Council Canada (ground whole carp), the International Atomic Energy Agency (fish homogenate), and the European Commission Joint Research Centre [fish oils (cod and mackerel) and mussel tissue].     

Positron annihilation spectroscopic studies of solvothermally synthesized ZnO nanobipyramids and nanoparticles

Zinc oxide (ZnO) samples in the form of hexagonal-based bipyramids and particles of nanometer dimensions were synthesized through solvothermal route and characterized by x-ray diffraction and transmission electron microscopy. Positron annihilation experiments were performed to study the structural defects such as vacancies and surfaces in these nanosystems. From coincidence Doppler broadening measurements, the positron trapping sites were identified as Zn vacancies or Zn-O-Zn trivacancy clusters. The positron lifetimes, their relative intensities, and the Doppler broadened lineshape parameter S all showed characteristic changes across the nanobipyramid size corresponding to the thermal diffusion length of positrons. In large nanobipyramids, vacancies within the crystallites also trapped positrons and the effects of agglomeration of such vacancies due to increased temperatures of synthesis were reflected in the variation of the annihilation parameters with their base diameters. The sizes of the nanoparticles used were all in the limit of thermal diffusion length of positrons and the annihilation characteristics were in accordance with the decreasing contribution from surfaces with increasing particle size.     

Development of anangiogenesis-focused cDNA chip and validation of its functionality

DNA chip has been used as a powerful tool to study the genetic reprogramming of cells and its link to cellular phenotype such as angiogenesis. To evaluate the angiogenesis related genetic reprogramming more efficiently, we here developed an angiogenesis-focused cDNA chip containing 153 angiogenesis related genes arrayed in duplicate on a slide glass. In order to validate the functionality of the angiogenesis-focused cDNA chip, we examined gene expression profiles in HT1080 cells treated with either fetal bovine serum, a well known pro-angiogenic factor, or trichostatin A, a known angiogenesis inhibitor, using the cDNA chip. All duplicate data from the analysis are well matched with each other and gene expression profiles are well consistent with previously reported data. These results demonstrate that the angiogenesis-focused cDNA chip developed here can be a useful tool towards angiogenesis- related researches.     

Cell asymmetry correction for temperature modulated differential scanning calorimetry

The quality of measurement of heat capacity by differential scanning calorimetry (DSC) is based on strict symmetry of the twin calorimeter. This symmetry is of particular importance for temperature-modulated DSC (TMDSC) since positive and negative deviations from symmetry cannot be distinguished in the most popular analysis methods. The heat capacities for sapphire-filled and empty aluminum calorimeters (pans) under designed cell imbalance caused by different pan-masses were measured. In addition, the positive and negative signs of asymmetry have been explored by analyzing the phase-shift between temperature and heat flow for sapphire and empty runs. The phase shifts change by more than 180° depending on the sign of the asymmetry. Once the sign of asymmetry is determined, the asymmetry correction for temperature-modulated DSC can be made.On leave from Toray Research Center, Inc., Otsu, Shiga 520, JapanThis work was supported by the Division of Materials Research, National Science Foundation, Polymers Program, Grant # DMR 90-00520 and the Division of Materials Sciences, Office of Basic Energy Sciences, U.S. Department of Energy at Oak Ridge National Laboratory, managed by Lockheed Martin Energy Research Corp. for the U.S. Department of Energy, under contract number DE-AC05-960R22464.     

Quantification of Nb and Zr in the irradiated pressure tubes from Wolsong CANDU Unit 1 by neutron activation analysis

When the Wolsong 1st CANDU reactor in Korea is reaching the end of its original lifespan, decommissioning has been one of the largest issues faced by the nuclear industry and the government for the estimation of expense. The radioactive sources in the construction stuffs and components of the reactor such as pressure tubes, steam generators must be evaluated for the estimation of the appropriate expense for the decommissioning. Unfortunately we do not have exact information about the initial composition of the pressure tubes. In this study the elemental contents of Nb and Zr in the activated zircaloy pressure tubes was investigated. Nb is one of the important elements that characterize the physical and mechanical properties of the pressure tube and a major source of high radioactivity. The prepared samples were strongly irradiated again in the vertical irradiation channel at the HANARO research reactor in the Korea Atomic Energy Research Institute (KAERI) and then measured by an HPGe detector.     

Preparation and characterization of multi-walled carbon nanotubes (MWCNTs), functionalized with phosphonic acid (MWCNTs–C–PO3H2) and its application as a novel,efficient, heterogeneous,highly selective and reusable catalyst for acetylation of alcohols,phenols, aromatic amines,and thiols

A novel, efficient, heterogeneous, and reusable multi-walled carbon nanotubes (MWCNTs), functionalized with phosphonic acid (MWCNTs–C–PO₃H₂) has been synthesized. The synthesized CNTs were characterized using some electron microscopic techniques such as scanning electron microscopy (SEM), atomic force microscopy (AFM), Energy dispersive X-ray spectroscopy (EDAX), and also some thermal and spectroscopic methods such as thermogravimetry (TG). The nitrogen adsorption behavior of the MWCNTs–C–PO₃H₂ catalyst was evaluated using the TG instrumentation system at 25 °C. The catalyst was applied successfully for highly efficient and selective acetylation of alcohols, phenols, thiols and aromatic amines with acetic anhydride at room temperature under solvent-free conditions. The reusability of the catalyst was checked and the recovered catalyst was reused for five runs without significant loss in activity.     

Scintillator-fiber flow-cell radioactivity detector for liquid chromatography

Summary A new type of flow-cell radiation detector for use in liquid chromatography which is packed with aligned scintillator fibers is described. A primary advantage of the fiber packed cell is that light generated by the scintillator is absorbed to a much less extent by the fibers than by the powder scintillator used in conventional flow cells. A detection efficiency of 55% has been obtained for carbon-14 using 0.1-mm diameter hand-pulled glass fibers. Computer modeling has shown that even better results can be obtained by using smaller and more uniform diameter fibers which will allow better packing. The fiber cell also demonstrates back pressures which are a factor of 50 less than the conventional cell and much less susceptibility to absorption of compounds because of its lower surface area. Research sponsored by the Office of Energy Research, U.S. Department of Energy, under contract DE-AC05-840R21400 with Martin Marietta Energy Systems, Inc.     

Biotransformation of coal substructure model compounds by microbial enzymes

Research with both coal substructure model compounds and macromolecular coal has shown that intermonomeric chemical bonds within coal are susceptible to cleavage by microbial enzymes from bacterial and fungal sources. This is particularly true when low rank lignite coals are used as substrates for enzymes after first being solubilized under alkaline conditions to form water-soluble coal polymers. When these soluble polymers are used as substrates, high-performance liquid chromatography (HPLC) methods are used to show that particular enzymes catalyze their depolymerization. By using chemical presolubilization followed by enzymatic depolymerization, it may be possible to develop commercial processes for the enzymatic depolymerization of coal into useful low-mol-wt chemicals, or into liquid or gaseous fuels. Evidence indicates that oxidative enzymes, such as peroxidases or etherases, and hydrolytic enzymes, such as esterases, have the best potential for effectively depolymerizing coal. Recent findings in our laboratory also suggest that certain hydrolases from saprophytic soil fungi may also work well.     

Validation of NAA data for a background soils characterization project

Background soils from areas around the United States Department of Energy facilities in Oak Ridge, Tennessee were characterized as part of an environmental restoration project. The data obtained in this project were validated using guidelines from the Environmental Protection Agency (EPA) Contract Laboratory Program (CLP), when EPA methods were used. However, there are no final EPA guidelines for validation of data obtained using radiochemical analytical methods, so procedures for validation had to be developed. This paper will describe the validation guidelines that were developed for neutron activation analysis (NAA) data and discuss the regulatory basis for them.Managed by Martin Marietta Energy Systems, Inc. for the U.S. DEPARTMENT OF ENERGY under contract DE-AC05-84OR21400