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Results for “Journal of Physics and Chemistry of Solids”

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USGS1977

Cell dimensions and antiferromagnetism of lunar and terrestrial ilmenite single crystals

X-Ray diffraction and anisotropic magnetic measurements have been made on single crystals of lunar ilmenite and on terrestrial ilmenite from Bancroft, Ontario, Canada and the Ilmen Mountains, U.S.S.R. The elongated c "> c -axis of lunar ilmenite, previously reported, is confirmed by new measurements. The shorter c "> c -axis found in terrestrial specimens is ascribed to Fe 3+ substitution for Ti 4+ in the titanium layer. Magnetic measurements on the same specimens show that, in agreement with the Ishikawa-Shirane et al . model, the initial shortening of the c "> c -axis by the above substitution of small amounts of Fe 3+ (<8%) causes an increase in Fe 2+ −Fe 2+ exchange coupling through Fe 3+ in the titanium layer that lowers the Néel transition temperature. The Weiss temperatures and other magnetic parameters confirm this model proposed by Ishikawa and Shirane et al . Additional transitions found in one of the terrestrial specimens (Bancroft) have been ascribed to a small amount of an exsolved spinel phase, possibly a solid solution phase of magnetite-ülvospinel. The spinel phase is localized in hematite-rich blebs which exsolved from the host ilmenite-rich phase.

Journal of Physics and Chemistry of Solids↗

USGS1967

Pressure derivatives of elastic moduli of fused quartz to 10 kb

Measurements of the longitudinal and shear moduli were made on fused quartz to 10 kb at 24·5°C. The anomalous behavior of the bulk modulus K at low pressure, ∂K ∂P < 0 "> ∂K∂P< 0 , begins to approach the “normal” behavior of solids, ∂K ∂P > 0 "> ∂K∂P> 0 , at higher pressures. The pressure derivative of the rigidity modulus ∂G ∂P "> ∂G∂P remains constant and negative for the pressure range covered. A 15-kb hydrostatic pressure vessel is described for use with ultrasonic pulse instrumentation for precise measurements of elastic moduli and density changes with pressure. The placing of the transducer outside the pressure medium, and the use of C -ring pressure seals result in ease of operation and simplicity of design.

Journal of Physics and Chemistry of Solids↗

USGS1977

Anisotropic magnetic susceptibility of erbium and ytterbium in zircon, ZrSiO4

Magnetic susceptibility measurements have been made for both Er- and Yb-doped (1̃0 3 ppm) zircon single crystals with the magnetic field perpendicular and parallel to the [001] axis. Large susceptibility anisotropies were found in both cases. Our observed anisotropies of ZrSiO 4 : Yb indicate small populations (1̃9%) of Yb ions at the axial (tetragonal) sites, as the susceptibility of ZrSiO 4 : Yb would be nearly isotropic if the Yb ions only occupied the orthorhombic sites. For Er 3+ in orthorhombic sites of zircon, our data indicate that the first excited state is paramagnetic with g x = 9 and g y 5̃ at 20 cm −1 above the ground state ( g x 0̃, g y 1̃5). The first excited state is quite similar to the ground states observed for Er 3+ in many host lattices

Journal of Physics and Chemistry of Solids↗

USGS1971

Magnetic susceptibility and triangular exchange coupling in the tourmaline mineral group

Magnetic susceptibilities of three iron-rich tourmaline crystals from Mexquitic (Mexico), Pierpont (New York), and Madagascar with different and known chemical compositions have been studied from 8° to 300°K. The iron atoms in the tourmaline crystal structure, space group R3m , a∼15·9, c∼7·2 , are situated at the three corners of an equilateral triangle and are close enough for magnetic exchange interaction. For buergerite, the Mexquitic sample, the susceptibility data lead to an exchange constant J/k of 7·5°K. Although the amount of aluminum would be sufficient to fill point position 18(c) exactly, the magnetic data are consistent with some substitution of ferric iron for aluminum, as previously determined from X-ray and neutron diffraction studies. Some aluminum thus replaces iron in position 9(b). Exchange constants were also estimated for the other two magnesium-iron specimens, of which the madagascar sample is aluminum deficient. The results agree with the evidence from optical spectra that there is considerable deviation from octahedral symmetry in the oxygen coordination polyhedra about the 9(b) and 18(c) point positions.

New York↗

USGS2002

Infrared spectral behavior of fine particulate solids

Transmission and emission spectra of clouds and layers of fine particulate samples of quartz, magnesium oxide, and aluminum oxide in the 6.5-35-??m wavelength range are presented. They demonstrate that the behavior of layers of particles constitutes a good analogue for a cloud of particles; that individual micrometer-sized particles emit most where they absorb most; that as the size of the particle is increased, the emission features reverse polarity and the spectrum approaches that of one obtained from a polished plate; and that as the particle layer-thickness increases, radiative interaction becomes increasingly important so that the emission maximum shifts from the strongest to weaker features, or produces a maximum at the Christiansen wavelength.

Journal of Physical Chemistry↗

USGS2003

CO2 hydrate: Synthesis, composition, structure, dissociation behavior, and a comparison to structure I CH4 hydrate

Structure I (sI) carbon dioxide (CO 2 ) hydrate exhibits markedly different dissociation behavior from sI methane (CH 4 ) hydrate in experiments in which equilibrated samples at 0.1 MPa are heated isobarically at 13 K/h from 210 K through the H 2 O melting point (273.15 K). The CO 2 hydrate samples release only about 3% of their gas content up to temperatures of 240 K, which is 22 K above the hydrate phase boundary. Up to 20% is released by 270 K, and the remaining CO 2 is released at 271.0 plusmn; 0.5 K, where the sample temperature is buffered until hydrate dissociation ceases. This reproducible buffering temperature for the dissociation reaction CO 2 ·nH 2 O = CO 2 (g) + nH 2 O(1 to s) is measurably distinct from the pure H 2 O melting point at 273.15 K, which is reached as gas evolution ceases. In contrast, when si CH 4 hydrate is heated at the same rate at 0.1 MPa, >95% of the gas is released within 25 K of the equilibrium temperature (193 K at 0.1 MPa). In conjunction with the dissociation study, a method for efficient and reproducible synthesis of pure polycrystalline CO 2 hydrate with suitable characteristics for material properties testing was developed, and the material was characterized. CO 2 hydrate was synthesized from CO 2 liquid and H 2 O solid and liquid reactants at pressures between 5 and 25 MPa and temperatures between 250 and 281 K. Scanning electron microscopy (SEM) examination indicates that the samples consist of dense crystalline hydrate and 50-300 μm diameter pores that are lined with euhedral cubic hydrate crystals. Deuterated hydrate samples made by this same procedure were analyzed by neutron diffraction at temperatures between 4 and 215 K; results confirm that complete conversion of water to hydrate has occurred and that the measured unit cell parameter and thermal expansion are consistent with previously reported values. On the basis of measured weight gain after synthesis and gas yields from the dissociation experiments, approximately all cages in the hydrate structure are filled such that n ≈ 5.75.

Journal of Physical Chemistry B↗

USGS2011

Groundwater chemistry near an impoundment for produced water, Powder River Basin, Wyoming, USA

The Powder River Basin is one of the largest producers of coal-bed natural gas (CBNG) in the United States. An important environmental concern in the Basin is the fate of the large amounts of groundwater extracted during CBNG production. Most of this produced water is disposed of in unlined surface impoundments. A 6-year study of groundwater flow and water chemistry at one impoundment, Skewed Reservoir, has produced the most detailed data set for any impoundment in the Basin. Data were collected from a network of 21 observation wells and three suction lysimeters. A groundwater mound formed atop bedrock within initially unsaturated, unconsolidated deposits underlying the reservoir. Heterogeneity in physical and chemical properties of sediments resulted in complex groundwater flow paths and highly variable groundwater chemistry. Sulfate, bicarbonate, sodium, and magnesium were the dominant ions in all areas, but substantial variability existed in relative concentrations; pH varied from less than 3 to more than 9, and total dissolved solids concentrations ranged from less than 5000 to greater than 100,000 mg/L. Selenium was a useful tracer of reservoir water; selenium concentrations exceeded 300 μg/L in samples obtained from 18 of the 24 sampling points. Groundwater travel time from the reservoir to a nearby alluvial aquifer (a linear distance of 177 m) was calculated at 474 days on the basis of selenium concentrations. The produced water is not the primary source of solutes in the groundwater. Naturally occurring salts and minerals within the unsaturated zone, dissolved and mobilized by infiltrating impoundment water, account for most of the solute mass in groundwater. Gypsum dissolution, cation-exchange, and pyrite oxidation appear to be important reactions. The complex geochemistry and groundwater flow paths at the study site underscore the difficulty in assessing effects of surface impoundments on water resources within the Powder River Basin.

Wyoming↗

USGS2020

Timescales and processes of methane hydrate formation and breakdown, with application to geologic systems

Gas hydrate is an ice-like form of water and low molecular weight gas stable at temperatures of roughly -10ºC to 25ºC and pressures of ~3 to 30 MPa in geologic systems. Natural gas hydrates sequester an estimated one-sixth of Earth’s methane and are found primarily in deepwater marine sediments on continental margins, but also in permafrost areas and under continental ice sheets. When gas hydrate is removed from its stability field, its breakdown has implications for the global carbon cycle, ocean chemistry, marine geohazards, and interactions between the geosphere and the ocean-atmosphere system. Gas hydrate breakdown can also be artificially driven as a component of studies assessing the resource potential of these deposits. Furthermore, geologic processes and perturbations to the ocean-atmosphere system (e.g., warming temperatures) can cause not only dissociation, but also more widespread dissolution of hydrate or even formation of new hydrate in reservoirs. Linkages between gas hydrate and disparate aspects of Earth’s near-surface physical, chemical, and biological systems render an assessment of the rates and processes affecting the persistence of gas hydrate an appropriate Centennial Grand Challenge. This paper reviews the thermodynamic controls on methane hydrate stability and then describes the relative importance of kinetic, mass transfer, and heat transfer processes in the formation and breakdown (dissociation and dissolution) of gas hydrate. Results from numerical modeling, laboratory, and some fields studies are used to summarize the rates of hydrate formation and breakdown, followed by an extensive treatment of hydrate dynamics in marine and cryospheric gas hydrate systems.

Journal of Geophysical Research-Solid Earth↗

USGS1999

Formation of natural gas hydrates in marine sediments 1. Conceptual model of gas hydrate growth conditioned by host sediment properties

The stability of submarine gas hydrates is largely dictated by pressure and temperature, gas composition, and pore water salinity. However, the physical properties and surface chemistry of deep marine sediments may also affect the thermodynamic state, growth kinetics, spatial distributions, and growth forms of clathrates. Our conceptual model presumes that gas hydrate behaves in a way analogous to ice in a freezing soil. Hydrate growth is inhibited within fine-grained sediments by a combination of reduced pore water activity in the vicinity of hydrophilic mineral surfaces, and the excess internal energy of small crystals confined in pores. The excess energy can be thought of as a "capillary pressure" in the hydrate crystal, related to the pore size distribution and the state of stress in the sediment framework. The base of gas hydrate stability in a sequence of fine sediments is predicted by our model to occur at a lower temperature (nearer to the seabed) than would be calculated from bulk thermodynamic equilibrium. Capillary effects or a build up of salt in the system can expand the phase boundary between hydrate and free gas into a divariant field extending over a finite depth range dictated by total methane content and pore-size distribution. Hysteresis between the temperatures of crystallization and dissociation of the clathrate is also predicted. Growth forms commonly observed in hydrate samples recovered from marine sediments (nodules, and lenses in muds; cements in sands) can largely be explained by capillary effects, but kinetics of nucleation and growth are also important. The formation of concentrated gas hydrates in a partially closed system with respect to material transport, or where gas can flush through the system, may lead to water depletion in the host sediment. This "freeze-drying" may be detectable through physical changes to the sediment (low water content and overconsolidation) and/or chemical anomalies in the pore waters and metastable presence of free gas within the normal zone of hydrate stability.

Journal of Geophysical Research B: Solid Earth↗