The use of SIMS and SEM for the characterization of individual particles with a matrix originating from a nuclear weapon.

The application of scanning electron microscopy (SEM) and secondary ion mass spectrometry (SIMS) for characterization of mixed plutonium and uranium particles from nuclear weapons material is presented. The particles originated from the so-called Thule accident in Greenland in 1968. Morphological properties have been studied by SEM and two groups were identified: a "popcorn" structure and a spongy structure. The same technique, coupled with an energy-dispersive X-ray (EDX) spectrometer, showed a heterogeneous composition of Pu and U in the surface layers of the particles. The SIMS depth profiles revealed a varying isotopic composition indicating a heterogeneous mixture of Pu and U in the original nuclear weapons material itself. The depth distributions agree with synchrotron-radiation-based mu-XRF (X-ray fluorescence microprobe) measurements on the particle (Eriksson, M., Wegryzynek, D., Simon, R., & Chinea-Cano, E., in prep.) when a SIMS relative sensitivity factor for Pu to U of 6 is assumed. Different SIMS identified isotopic ratio groups are presented, and the influence of interferences in the Pu and U mass range are estimated. The study found that the materials are a mixture of highly enriched 235U (235U:238U ratio from 0.96 to 1.4) and so-called weapons grade Pu (240Pu:239Pu ratio from 0.028 to 0.059) and confirms earlier work reported in the literature.     

Variations of phthalate ester concentrations in sediments from the Chester River, Maryland

Phthalate esters discharged from a plasticizer-manufacturing plant were distinguished from those of other sources in the Chester River, Maryland by comparing the distinctive patterns of alkyl phthalate species of the plant to those of sediment samples from sites along the mid-river axis. The magnitude of the changes in individual phthalate species were placed in perspective by charting their concentrations with distance along the river. Short sediment cores were also analyzed to determine the profile of phthalate ester pollution in the Chester River during the previous decade in which the river experienced a significant oyster mortality. A significant level of phthalate ester pollution was found in the Chester River sediment but its source was not found to be the plasticizer plant.     

Natural and fallout radionuclide concentrations in the environment of Islamabad

A study on the concentration of natural and fallout radionuclides in environmental samples collected from different localities of Islamabad was performed. For the determination of gamma-emitters such as ²³⁸U, ²³²Th, ⁴⁰K and ¹³⁷Cs high purity germanium (HPGe) detector was used while for the analysis of ⁹⁰Sr, a beta-emitter, liquid scintillation counting system was used. The indoor absorbed dose rate was measured by a CaF₂ : Dy thermoluminescence detector. Other radiation parameters were also determined to evaluate the radiation hazard. All the results were well within the permissible limits showing that there is no radiation hazard in the environment of Islamabad.     

Synthesis of highly crosslinked monodisperse polymer particles: Effect of reaction parameters on the size and size distribution

Monodisperse polystyrene particles crosslinked with different concentrations of divinylbenzene were synthesized in the 3.2–9.1 μm size range by dispersion polymerization in an isopropyl alcohol/toluene mixed‐dispersion medium with poly(N‐vinylpyrrolidone) as a steric stabilizer and 2,2′‐azobisisobutyronitrile as a radical initiator. The effects of the reaction parameters such as the crosslinking agent concentration, media solvency (controlled by varying the amount of toluene addition), the initiator concentration, and the stabilizer concentration on the particle size and size distribution were investigated with reference particles with a monodisperse size distribution and crosslinked by 1.5 wt % divinylbenzene. The appropriate increase in media solvency was a prerequisite for preparing crosslinked particles without coagulated and/or odd‐shaped particles. The investigation of the effects of the polymerization parameters also shows that only specific sets of conditions produce particles with a monodisperse size distribution. The glass‐transition temperatures of the particles increased with increasing divinylbenzene concentration. © 2002 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 40: 4368–4377, 2002     

Determination of plutonium,americium and curium isotopes in radioactive metal wastes deriving from nuclear decommissioning

A radiochemical analytical method, coupling different measurements techniques (alpha spectrometry, liquid scintillation counting and mass-spectrometry) for quantifying the content of the most significant plutonium and americium/curium isotopes in metal waste samples, is presented. The method based on the sequential determination of all the analytes of interest has the great advantage to perform the sample pre-treatment only once, resulting fast and cheap while maintaining sufficient selectivity and sensitivity. The mean values of radiochemical yields and the minimum detectable activities have been evaluated. Significant activity ratios between transuranic isotopes have been revealed and used to investigate the origin of the waste samples.

     

Study of particle size distribution and formation mechanism of radioactive aerosols generated in high-energy neutron fields

The size distributions of ³⁸Cl, ³⁹Cl, ⁸²Br and ⁸⁴Br aerosols generated by irradiations of argon and krypton gases containing di-octyl phthalate (DOP) aerosols with 45 MeV and 65 MeV quasi-monoenergetic neutrons were measured in order to study the formation mechanism of radioactive particles in high energy radiation fields. The effects of the size distribution of the radioactive aerosols on the size of the added DOP aerosols, the energy of the neutrons and the kinds of nuclides were studied. The observed size distributions of the radioactive particles were explained by attachment of the radioactive atoms generated by the neutron-induced reactions to the DOP aerosols.     

On the evolution of the rate of polymerization,number and size distribution of particles in styrene emulsion polymerization above CMC

This work is an extension of a communication reported by two of the authors [Carro and Herrera‐Ordoñez, Macromol Rapid Commun 2006, 27, 274], where bimodal particle size distributions (PSD), obtained by asymmetric flow‐field flow fractionation (AFFF, AF⁴), were taken as evidence of certain degree of stability of primary particles. Now, emulsion polymerizations of styrene were performed under conditions employed before by other researchers, intending to examine if the behavior observed is general. The number of particles (N) and PSD were studied by means of dynamic light scattering and AF⁴. By the later, bimodal PSDs were detected in all cases, where the population corresponding to primary particles (diameter <20 nm) depends on reaction conditions. Regarding N, AF⁴ results show that it is constant during interval II, in contrast to DLS results. Primary particle coagulation was evidenced as minimums in N evolution and the rate of polymerization curves, monitored by calorimetry and gravimetry, which are enhanced when higher particle number is generated and/or the ionic strength is increased. These results suggest that particle coagulation is not as extensive as it would be expected according to the coagulative theory. © 2010 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 48: 3152–3160, 2010     

Comparison of radionuclide ratios in atmospheric nuclear explosions and nuclear releases from Chernobyl and Fukushima seen in gamma ray spectrometry

The Comprehensive Nuclear Test Ban Treaty has remote radionuclide monitoring followed by an On Site Inspection (OSI) to clarify the nature of a suspect event as part of its verification regime. An important aspect of radionuclide measurements on site is the discrimination of other potential sources of similar radionuclides such as reactor accidents or medical isotope production. The Chernobyl and Fukushima nuclear reactor disasters offer two different reactor source term environmental inputs that can be compared against historical measurements of nuclear explosions. The comparison of whole-sample gamma spectrometry measurements from these three events and the analysis of similarities and differences are presented. This analysis is a step toward confirming what is needed for measurements during an OSI under the auspices of the Comprehensive Test Ban Treaty.     

The distribution of particles characterized by size and free mobility within polydisperse populations of protein-polysaccharide conjugates, determined from two-dimensional agarose electropherograms

New approaches for the characterization of polydisperse particle populations are presented*. The investigated samples contain virus-sized protein-polysaccharide conjugates which had previously been prepared as immunogens against bacterial meningitis (Hib). The analysis is based on two-dimensional agarose electrophoresis (Serwer-type). This method, like the one of O'Farrell, achieves a separation according to size and charge. It relies on a different principle, however, and is applicable to nondenatured particles which are 100 to more than 1000 times larger in mass than regular uncrosslinked proteins. Data from stained gel patterns are evaluated by the computer program ELPHOFIT, which makes it possible to standardize the gel and to construct a nomogram which defines every position on the gel in terms of particle size and free mobility (related to surface net charge density). The output of ELPHOFIT, consisting of nomogram parameters, is transferred to the image processing program GELFIT. This software is used to evaluate the computer images obtained by digitizing the stained gel patterns: (i) The nomogram is electronically superimposed on the computer image. (ii) The gel pattern is transformed from a curvilinear to a rectangular coordinate system of particle size and free mobility. The center of gravity as well as density maxima are given in coordinates of particle size and free mobility. Ranges of grey levels can be accentuated by adding 16 pseudocolors. (iii) Using surface-stripping techniques, GELFIT provides an estimate for the number of major subpopulations within each preparation. (iv) Numerical values for the distribution of particle size and free mobility are determined. Using program IMAGE, the quantitative physical assessment of a given conjugate preparation is presented in the form of a computer-generated three-dimensional plot, the shape of which serves to identify and characterize the preparation visually. The data analysis based on digitized two-dimensional gel patterns is automated to an extent that a technician can perform routine evaluations. It uses the Macintosh II personal computer.     

Synthetic process to control the total size and component distribution of multilayer magnetic composite particles

A new synthetic process to prepare composite particles with multilayers, comprised of usual polymer latices, ultra-fine magnetic particles, and a polystyrene layer was examined under various solution conditions.First, the synthetic conditions of heterocoagulates, consisted of polystyrene latices (2a=180900 nm) and NiO·ZnO·Fe₂O₃ particles (2a=20 nm), were investigated as a function of medium pH, particle concentration, and particle size ratio, based on the concept of the heterocoagulation theory as applied by Harding et al. Regular heterocoagulates were generated under suitable medium and mixing conditions, and that their total size can be controlled by selecting the size of the original polymer latices used as the core.Second, the best encapsulation condition of the heterocoagulates via emulsion polymerization with polystyrene monomer was surveyed. The encapsulation of the heterocoagulates was greatly promoted by pretreatment with oleate molecules, although there is no tendency for the encapsulation when the surfactant-free bare heterocoagulates are used as the core.     

Measurements of radioxenon in ground level air in South Korea following the claimed nuclear test in North Korea on October 9, 2006

Following the claimed nuclear test in the Democratic People’s Republic of Korea (DPRK) on October 9, 2006, and a reported seismic event, a mobile system for sampling of atmospheric xenon was transported to the Republic of South Korea (ROK) in an attempt to detect possible emissions of radioxenon in the region from a presumed test. Five samples were collected in the ROK during October 11–14, 2006 near the ROK–DPRK border, and thereafter transported to the Swedish Defense Research Agency (FOI) in Stockholm, Sweden, for analysis. Following the initial measurements, an automatic radioxenon sampling and analysis system was installed at the same location in the ROK, and measurements on the ambient atmospheric radioxenon background in the region were performed during November 2006 to February 2007. The measured radioxenon concentrations strongly indicate that the explosion in October 9, 2006 was a nuclear test. The conclusion is further strengthened by atmospheric transport models. Radioactive xenon measurement was the only independent confirmation that the supposed test was in fact a nuclear explosion and not a conventional (chemical) explosive.     

Determination of the pore connectivity and pore size distribution and pore spatial distribution of porous chromatographic particles from nitrogen sorption measurements and pore network modelling theory

The pore connectivity, pore size distribution and pore spatial distribution of the porous structure of native and silanized silica particles were determined by matching the experimental nitrogen sorption data with the theoretical results obtained from pore network model simulations. The agreement between theory and experiment is found to be good. The results clearly indicate that the deposition of the silane layer to the pore surfaces of the native silica particles produces a silanized silica particle with a mean pore diameter and pore connectivity smaller than that of the native silica particle. Furthermore, the evaluation of the pore diffusivity of ribonuclease under unretained conditions shows that the lower values of the pore connectivity found in the samples of silanized silica particles, when compared with the values of the pore connectivity obtained for the native silica particles, increase the diffusional mass transfer resistance within the porous structure of the silanized silica particles.     

Determination of long-lived radionuclides in radioactive wastes from the IEA-R1 nuclear research reactor

Ion-exchange resins and activated charcoal beds are employed for purification of the cooling water that is pumped through the core of pool type nuclear research reactors. Once expended, these media are replaced and become radioactive wastes that contain low concentrations of long-lived fission and activation products, uranium isotopes and transuranium elements. Determination of the radioactive inventory is of paramount importance in the management of such radioactive wastes, which, besides high-energy photon emitters that can be identified and quantified directly by gamma-ray spectrometry, also contain pure alpha, pure beta and low-energy photon emitters whose quantitative determination require radiochemical separation. These later are collectively known as difficult to measure (DTM) radionuclides. A characterization program embracing the DTM radionuclides is currently in progress for spent ion-exchange resins and activated charcoal beds that were definitively withdrawn from the water cleanup system of the IEA-R1 nuclear research reactor. Radiochemical methods used in the characterization program include separations with specific anionic resins, chromatographic extractions and co-precipitation, which enabled the measurement of the activity concentrations of ⁹⁰Sr, ²³⁴U, ²³⁵U, ²³⁸U, ²³⁸Pu, ^239+240Pu, ²⁴¹Pu, ²⁴¹Am and ²⁴⁴Cm. An enhanced retention of uranium and transuranium elements was observed in the activated charcoal compared to the ion-exchange resins as a result of the tendency of actinides to undergo hydrolysis in aqueous solutions.     

Histograms of the size distribution of kraft lignin particles in aqueous solutions at various pH values

The size distribution of kraft lignin particles in aqueous solutions in a wide pH range (9.5−2.0) was studied by filtration through track membranes.     

Natural radionuclide concentrations in drinking water (well and spring mineral waters) samples from Bordj-Bouarreridj region,east Algeria

Journal of Radioanalytical and Nuclear Chemistry - Using gamma ray spectroscopy with high purity germanium detector, the activity concentrations of 238U, 232Th and 40K radionuclides in drinking...     

Elastic light scattering from nonspherical and polydisperse particles in the size range from 100 to 2000 NM

In the case of monodisperse dilute systems it is possible to calculate the distance distribution function for homogeneous and inhomogeneous particles of arbitrary shape. The distance distribution function enables one to find a rough classification of the shape and to determine the size of the particle. This function can be deconvoluted to the radial polarization density profile for particles with spherical symmetry. A number, mass or intensity distribution can be calculated from the light scattering data from polydisperse systems if the distribution can be described by a single parameter and if it is possible to calculate the shape factor of the particles, as it is the case for spheres and spheroids. The range of applicability of the method depends on the experimental set-up, but is in most cases in the size range from 100 nm to several micrometers.     

Compressibility, the measurement of surface tension, and particle size in molecular or nuclear matter

It is shown that the interface shrinkage resulting from the capillary pressure difference between both sides of a curved interface is the product of a "standard shrinkage"kappagamma (kappa is the isothermal compressibility, gamma the interfacial tension) by a dimensionless factor that depends only on the shape of the sample of matter under study. The behaviour of the standard shrinkage in the critical domain shows that it cannot be a measure of the thickness of the liquid-vapour interface in that domain. The standard shrinkage of classical liquids somewhat above triple point is usually near to 0.048 v(c)(1/3) (v(c) is the critical molecular volume); exceptions to this rule are discussed. The variation of the standard shrinkage along the liquid-vapour coexistence curves of water and argon is presented; the effect of the interface shrinkage on the measured surface tension of liquids can become important within about 15% of the critical temperature. The standard shrinkage of solids is less than that of the corresponding liquids, and is of no consequence when measuring the surface tension of solids. The standard shrinkage of the nuclear fluid is 0.23 fm=0.09 v(c)(1/3). The saturation density of infinite nuclear matter is about 9% less than its value in atomic nuclei, and a term proportional to A(1/3) (A is the mass number) must be added to the nuclear binding energy formula.