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As a result of nuclear weapons testing and accidents, plutonium has been distributed into the environment. The areas close to the sites of these tests and accidental dispersions contain plutonium deposition of such a magnitude that health authorities and responsible officials have mandated that the contaminated areas be protected, generally through isolation or removal of the contaminated areas. In recent years remedial actions have taken place at all these sites. For reasons not entirely clear, the public perceives radiation exposure risk to be much greater than the evidence would suggest [1]. This perception seems to be particularly true for plutonium, which has often been ''demonized'' in various publications as the ''most hazardous substance known to man'' [2]. As the position statement adapted by the Health Physics Society explains, ''Plutonium's demonization is an example of how the public has been misled about radiation's environmental and health threats generally, and in cases like plutonium, how it has developed a warped ''risk perception'' that does not reflect reality'' [3]. As a result of this risk perception and ongoing debate surrounding environmental plutonium contamination, remedial action criteria are difficult to establish. By examining the data available before and after remedial actions taken at the …

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A key uncertainty in models of the global carbonate-silicate cycle and long-term climate is the way that silicates weather under different climatologic conditions, and in the presence or absence of organic activity. Digital imaging of basalts in Hawaii resolves the coupling between temperature, rainfall, and weathering in the presence and absence of lichens. Activation energies for abiotic dissolution of plagioclase (23.1{+-} 2.5 kcal/mol) and olivine (21.3 {+-} 2.7 kcal/mol) are similar to those measured in the laboratory, and are roughly double those measured from samples taken underneath lichen. Abiotic weathering rates appear to be proportional to rainfall. Dissolution of plagioclase and olivine underneath lichen is far more sensitive to rainfall.

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To confirm conversion of soil Pb to pyromorphite [Pb{sub 5}(PO{sub 4}){sub 3}Cl], a Pb contaminated soil collected adjacent to a historical smelter was reacted with hydroxyapatite in slurries of soil and hydroxyapatite separated by a dialysis membrane and incubated. A crystalline precipitate formed on the dialysis membrane in the slurry systems was identified as chloropyromorphite. Soluble species measured in the soil slurry indicated that dissolution of solid-phase soil Pb was the rate-limiting step for pyromorphite formation. Additionally samples reacted with hydroxyapatite were incubated at field-capacity moisture content. The sequential chemical extraction used to identify species in the field-moist soil incubation experiment showed that hydroxyapatite treatment reduced the first four fractions of extractable Pb and correspondingly increased the recalcitrant extraction residue fraction by 35% of total Pb at 0 d incubation and by 45% after 240 d incubation. the increase in the extraction residue fraction in the 240 d incubation as compared to the 0 d incubation implies that the reaction occurs in the soil but the increase in the hydroxyapatite amended 0 d incubated soil as compared to the control soil illustrates the chemical extraction procedure caused changes in the extractability. Thus, the chemical extraction procedure cannot easily be utilized …

This paper describes the evolution of the process for assessing the hazards of a geologic disposal system for radioactive waste and, similarly, nuclear power reactors, and the relationship of this process with other assessments of risk, particularly assessments of hazards from manufactured carcinogenic chemicals during use and disposal. This perspective reviews the common history of scientific concepts for risk assessment developed to the 1950s. Computational tools and techniques developed in the late 1950s and early 1960s to analyze the reliability of nuclear weapon delivery systems were adopted in the early 1970s for probabilistic risk assessment of nuclear power reactors, a technology for which behavior was unknown. In turn, these analyses became an important foundation for performance assessment of nuclear waste disposal in the late 1970s. The evaluation of risk to human health and the environment from chemical hazards is built upon methods for assessing the dose response of radionuclides in the 1950s. Despite a shared background, however, societal events, often in the form of legislation, have affected the development path for risk assessment for human health, producing dissimilarities between these risk assessments and those for nuclear facilities. An important difference is the regulator's interest in accounting for uncertainty and the …

The last major development effort for nuclear power and propulsion systems ended in 1993. Currently, there is not an initiative at either the National Aeronautical and Space Administration (NASA) or the U.S. Department of Energy (DOE) that requires the development of new nuclear power and propulsion systems. Studies continue to show nuclear technology as a strong technical candidate to lead the way toward human exploration of adjacent planets or provide power for deep space missions, particularly a 15,000 lbf bimodal nuclear system with 115 kW power capability. The development of nuclear technology for space applications would require technology development in some areas and a major flight qualification program. The last major ground test facility considered for nuclear propulsion qualification was the U.S. Air Force/DOE Space Nuclear Thermal Propulsion Project. Seven years have passed since that effort, and the questions remain the same, how to qualify nuclear power and propulsion systems for future space flight. It can be reasonably assumed that much of the nuclear testing required to qualify a nuclear system for space application will be performed at DOE facilities as demonstrated by the Nuclear Rocket Engine Reactor Experiment (NERVA) and Space Nuclear Thermal Propulsion (SNTP) programs. The nuclear infrastructure …

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The Lawrence Livermore National Laboratory (LLNL) Ground-Based Nuclear Explosion Monitoring (GNEM) R and D program has made significant progress populating a comprehensive Seismic Research knowledge Base (SRKB) and deriving calibration parameters for the Middle East and North Africa (ME/NA) and Former Soviet Union (FSU) regions. The LLNL SRKB provides not only a coherent framework in which to store and organize very large volumes of collected seismic waveforms, associated event parameter information, and spatial contextual data, but also provides an efficient data processing/research environment for deriving location and discrimination correction surfaces. The SRKB is a flexible and extensible framework consisting of a relational database (RDB), Geographical Information System (GIS), and associated product/data visualization and data management tools. This SRKB framework is designed to accommodate large volumes of data (over 2 million waveforms from 20,000 events) in diverse formats from many sources in addition to maintaining detailed quality control and metadata. Using the SRKB framework, they are combining travel-time observations, event characterization studies, and regional tectonic models to assemble a library of ground truth information and phenomenology correction surfaces required for support of the ME/NA and FSU regionalization program. Corrections and parameters distilled from the LLNL SRKB provide needed contributions to the …

Accurate seismic event location is key to monitoring the Comprehensive Nuclear-Test-Ban Treaty (CTBT) and is largely dependent on our understanding of the crust and mantle velocity structure. This is particularly challenging in aseismic regions, devoid of calibration data, which leads us to rely on a priori constraints on the velocities. We investigate our ability to improve seismic event location in the Middle East, North Africa, and the Former Soviet Union (ME/NA/FSU) by using a priori three-dimensional (3-D) velocity models in lieu of more commonly used one dimensional (1-D) models. Event locations based on 1-D models are often biased, as they do not account for significant travel-time variations that result from heterogeneous crust and mantle; it follows that 3-D velocity models have the potential to reduce this bias. Here, we develop a composite 3-D model for the ME/NA/FSU regions. This fully 3-D model is an amalgamation of studies ranging from seismic reflection to geophysical analogy. Our a priori model specifies geographic boundaries and velocity structures based on geology, tectonics, and seismicity and information taken from published literature, namely a global sediment thickness map of 1{sup o} resolution (Laske and Masters, 1997), a regionalized crustal model based on geology and tectonics (Sweeney …

Long-range seismic profiles from Peaceful Nuclear Explosions (PNE) in the Former Soviet Union (FSU) provide a unique data set to investigate several important issues in regional Comprehensive Nuclear-Test-Ban Treaty (CTBT) monitoring. The recording station spacing ({approx}15 km) allows for extremely dense sampling of the propagation from the source to {approx} 3300 km. This allows us to analyze the waveforms at local, near- and far-regional and teleseismic distances. These data are used to: (1) study the evolution of regional phases and phase amplitude ratios along the profile; (2) infer one-dimensional velocity structure along the profile; and (3) evaluate the spatial correlation of regional and teleseismic travel times and regional phase amplitude ratios. We analyzed waveform data from four PNE's (m{sub b} = 5.1-5.6) recorded along profile KRATON, which is an east-west trending profile located in northern Sibertil. Short-period regional discriminants, such as P/S amplitude ratios, will be essential for seismic monitoring of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) at small magnitudes (m{sub b} < 4.0). However, P/S amplitude ratios in the short-period band, 0.5-5.0 Hz, show some scatter. This scatter is primarily due to propagation and site effects, which arise from variability in the elastic and anelastic structure of the crustal waveguide. …

The study of a homologous series of silsesquioxane monomers has uncovered striking discontinuities in gelation behavior. An investigation of the chemistry during the early stages of the polymerization has provided a molecular basis for these observations. Monomers containing from one to four carbon atoms exhibit a pronounced tendency to undergo inter or intramolecular cyclization. The cyclic intermediates have been characterized by {sup 29}Si NMR, chemical ionization mass spectrometry and isolation from the reaction solution. These carbosiloxanes are local thermodynamic sinks that produce kinetic bottlenecks in the production of high molecular weight silsesquioxanes. The formation of cyclics results in slowing down or in some cases completely shutting down gelation. An additional finding is that the cyclic structures are incorporated intact into the final xerogel. Since cyclization alters the structure of the building block that eventually makes up the xerogel network, it is expected that this will contribute importantly to the bulk properties of the xerogel as well.

The miscibility of polypropylene (PP) melts in which the chains differ only in stereochemical composition has been investigated by two different procedures. One approach used detailed local information from a Monte Carlo simulation of a single chain, and the other approach takes this information from a rotational isomeric state model devised decades ago, for another purpose. The first approach uses PRISM theory to deduce the intermolecular packing in the polymer blend, while the second approach uses a Monte Carlo simulation of a coarse-grained representation of independent chains, expressed on a high-coordination lattice. Both approaches find a positive energy change upon mixing isotactic PP (iPP) and syndiotactic polypropylene (sPP) chains in the melt. This conclusion is qualitatively consistent with observations published recently by Muelhaupt and coworkers. The size of the energy chain on mixing is smaller in the MC/PRISM approach than in the RIS/MC simulation, with the smaller energy change being in better agreement with the experiment. The RIS/MC simulation finds no demixing for iPP and atactic polypropylene (aPP) in the melt, consistent with several experimental observations in the literature. The demixing of the iPP/sPP blend may arise from attractive interactions in the sPP melt that are disrupted when the sPP …

The structure of Na{sub 16}Nb{sub 12.8}Ti{sub 3.2}O{sub 44.8}(OH){sub 3.2} {center_dot} 8H{sub 2}O, a member of a new family of Sandia Octahedral Molecular Sieves (SOMS) having a Nb/Na/M{sup IV} (M= Ti, Zr) oxide framework and exchangeable Na and water in open channels, was determined from Synchrotron X-ray data. The SOMS phases are isostructural with variable M{sup IV}:Nb(1:50--1:4) ratios. The SOMS are extremely selective for sorption of divalent cations, particularly Sr{sup 2+}. The ion-exchanged SOMS undergo direct thermal conversion to a perovskite-type phase, indicating this is a promising new method for removal and sequestration of radioactive Sr-90 from mixed nuclear wastes.

The syntheses, crystal structures and some properties of {alpha}- and {beta}-ZnHPO{sub 3}{center_dot}N{sub 4}C{sub 2}H{sub 4} are reported. These two polymorphs are the first organically-templated hydrogen phosphites. They are built up from vertex-sharing HPO{sub 3} pseudo pyramids and ZnO{sub 3}N tetrahedra, where the Zn-N bond represents a direct link between zinc and the neutral 2-cyanoguanidine template. {alpha}-ZnHPO{sub 3}{center_dot}N{sub 4}C{sub 2}H{sub 4} is built up from infinite layers of vertex-sharing ZnO{sub 3}N and HPO{sub 3} groups forming 4-rings and 8-rings. {beta}-ZnHPO{sub 3}{center_dot}N{sub 4}C{sub 2}H{sub 4} has strong one-dimensional character, with the polyhedral building units forming 4-ring ladders. Similarities and differences to related zinc phosphates are discussed. Crystal data: {alpha}-ZnHPO{sub 3}{center_dot}N{sub 4}C{sub 2}H{sub 4}, M{sub r} = 229.44, monoclinic, P2{sub 1}/c, a = 9.7718 (5) {angstrom}, b = 8.2503 (4) {angstrom}, c = 9.2491 (5) {angstrom}, {beta} = 104.146 (1){sup 0}, V = 723.1 (1) {angstrom}{sup 3}, R(F) = 2.33%, wR(F) = 2.52%. {beta}-ZnHPO{sub 3}{center_dot}N{sub 4}C{sub 2}H{sub 4}, M{sub r} = 229.44, monoclinic, C2/c, a = 14.5092 (9) {angstrom}, b = 10.5464 (6) {angstrom}, c = 10.3342 (6) {angstrom}, {beta} = 114.290 (1){sup 0}, V = 1441.4 (3) {angstrom}{sup 3}, R(F) = 3.01%, wR(F) = 3.40%.

Accurate seismic event location is integral to the effective monitoring of the Comprehensive Nuclear-Test-Ban Treaty (CTBT), as well as being a fundamental component of earthquake source characterization. To account for the effects of crustal and mantle structure on seismic travel times, and to improve seismic event location in the Middle East and North Africa (MENA), we are developing a set of radially heterogeneous and azimuthally invariant travel-time models of the crust and upper mantle for each MENA seismic station. We begin by developing an average one-dimensional velocity model that minimizes the P-phase travel-time residuals from regional through teleseismic distance at each station. To do this we (1) generate a suite of 1-D velocity models of the earth, (2) compute travel times through the 1-D models using a tau-p formulation to produce standard travel-time tables, and (3) minimize the root-mean-square (rms) residuals between the P-phase arrivals predicted by each model and a groomed set of ISC P-phase arrival times (Engdahl et al., 1991). Once we have an average one-dimensional velocity model that minimizes the P-phase travel-time residuals for all distances, we repeat steps 1 through 3, systematically perturbing the travel-time model and using a grid search procedure to optimize models within …

Trialkoxysilyl-containing monomers of the type (RO){sub 3}Si(CH{sub 2}){sub 3}C(O)OtBu (R = Me, Et) were prepared by hydrosilation of the corresponding vinylic tert-butyl esters CH{sub 3}CHCH{sub 2}C(O)OtBu. Acid- or base-catalyzed polymerization of the monomers leads to very high molecular weight polymers with relatively narrow polydispersities. The polymerization results in complete condensation of the alkoxy groups while the tert-butyl ester functionality remains fully intact. Partial or full deprotection of the tert-butyl group can easily be achieved to yield the corresponding carboxylic acid polymers. The ester and carboxylic acid functionalities of these new materials allow for their potential use in a variety of applications such as scavenging of heavy metals.

Magnesium aryloxides were prepared in a variety of solvents through the reaction of dibutyl magnesium with sterically varied aryl alcohols: 2,6-dimethylphenol (H-DMP), 2,6-diisopropylphenol (H-DIP), and 2,4,6-trichlorophenol (H-TCP). Upon using a sufficiently strong Lewis-basic solvent, the monomeric species Mg(DMP){sub 2}(py){sub 3} (1, py = pyridine), Mg(DIP){sub 2}(THF){sub 3}, (2a, THF = tetrahydrofuran) Mg(TCP){sub 2}(THF){sub 3} (3) were isolated. Each of these complexes possesses a five-coordinate magnesium that adopts a trigonal bipyramidal geometry. In the absence of a Lewis base, the reaction with H-DIP yields a soluble trinuclear complex, [Mg(DIP){sub 2}]{sub 3} (2b). The Mg metal centers in 2b adopt a linear arrangement with a four-coordinate central metal while the outer metal centers are reduced to just three-coordinate. Solution spectroscopic methods suggest that while 2b remains intact, the monomeric species (1, 2a, and 3) are involved in equilibria, which facilitate intermolecular ligand transfer.

The structures of the high and low-density amorphous phases of ice are studied using several techniques. The diffraction patterns of high and low density amorphous ice are analyzed using reverse Monte Carlo methods and compared with molecular dynamics simulations of these phases. The spectra of crystalline and amorphous phases of ice obtained by Raman and incoherent inelastic neutron scattering are analyzed to yield structural features for comparison with the results of molecular dynamics and Reverse Monte Carlo analysis. The structural details obtained indicate that there are significant differences between the structure of liquid water and the amorphous phases of ice.

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It is known that filtered cathodic-arc-deposited ta-C films have outstanding properties even within the family of diamondlike materials. However, filtering of macroparticles is usually incomplete or accompanied by significant plasma losses. Ongoing research effort is directed towards the following goals: (1) complete elimination of macro- and nanoparticles from the vacuum arc plasma, (2) increase of plasma utilization in the cathodic-arc and macroparticle-filter system, (3) precise control and reproducibility of film deposition, and (4) synthesis of ultrathin films (< 5 nm) that meet requirements of the magnetic storage industry. The development of new filters, in particular the ''Twist Filter'', enables cathodic arc plasma deposition to synthesize ultrathin ta-C films of 3 nm on heads that pass corrosion and other relevant tests. We describe the Twist Filter system and report about recent ta-C tests results. In light of these results, even thinner films seem to be possible.

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A study of zeolite crystallization from sol-gel precursors using the vapor phase transport synthesis method has been performed. Zeolites (ZSM-5, ZSM-48, Zeolite P, and Sodalite) were crystallized by contacting vapor phase organic or organic-water mixtures with dried sodium silicate and dried sodium alumino-silicate gels. For each precursor gel, a ternary phase system of vapor phase organic reactant molecules was explored. The vapor phase reactant mixtures ranged from pure ethylene diamene, triethylamine, or water, to an equimolar mixture of each. In addition, a series of gels with varied physical and chemical properties were crystallized using the same vapor phase solvent mixture for each gel. The precursor gels and the crystalline products were analyzed via Scanning Electron Microscopy, Electron Dispersive Spectroscopy, X-ray mapping, X-ray powder diffraction, nitrogen surface area, Fourier Transform Infrared Spectroscopy, and thermal analyses. The product phase and purity as a function of the solvent mixture, precursor gel structure, and precursor gel chemistry is discussed.