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Results for “Journal of Solid State Chemistry”

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12 recordsLinked to original sources
USGS1987

Kinetics and mechanisms of iron sulfide reductions in hydrogen and in carbon monoxide

The reduction of iron sulfides by hydrogen and by carbon monoxide has been studied using plug flow and thermogravimetric methods. The reactions were studied in the 523–723°K temperature range and were found to be first-order processes. Plug flow studies were used to correlate reaction rates between pyrite and the gases as a function of the surface area of the pyrite. The rate of H 2 S formation increases with the surface area of the pyrite sample. The results of thermogravimetric experiments indicate that the reactions consist of several steps. Rate constants for the pyrite reduction by H 2 and by CO were obtained. The activation energies increased with degree of reduction. Values of E a were 113.2 (step I) and 122.5 kJ/mole (step II) for pyrite reduction with CO and 99.4 (step I), 122.4 (step II), 125.2 (step III), and 142.6 kJ/mole (step IV) for pyrite reduction with hydrogen.

Journal of Solid State Chemistry↗
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↗
USGS2001

Regional water-quality analysis of 2,4-D and dicamba in river water using gas chromatography-isotope dilution mass spectrometry

Gas chromatography with isotope dilution mass spectrometry (GC-MS) and enzyme-linked immunosorbent assay (ELISA) were used in regional National Water Quality Assessment studies of the herbicides, 2,4-D and dicamba, in river water across the United States. The GC-MS method involved solid-phase extraction, derivatized with deuterated 2,4-D, and analysis by selected ion monitoring. The ELISA method was applied after preconcentration with solid-phase extraction. The ELISA method was unreliable because of interference from humic substances that were also isolated by solid-phase extraction. Therefore, GC-MS was used to analyzed 80 samples from river water from 14 basins. The frequency of detection of dicamba (28%) was higher than that for 2,4-D (16%). Concentrations were higher for dicamba than for 2,4-D, ranging from less than the detection limit (7lt; 0.05 μg/L) to 3.77μg/L, in spite of 5 times more annual use of 2,4-D as compared to dicamba. These results suggest that 2,4-D degrades more rapidly in the environment than dicamba.

International Journal of Environmental Analytical ↗
USGS2019

Carbon chemistry of intact versus chronically drained peatlands in the southeastern USA

The Great Dismal Swamp (GDS) is a large temperate swamp in Virginia/North Carolina with peat soils historically resistant to microbial decomposition. However, this peatland has been subject to ~200 years of disturbance during which extensive drainage, fire suppression, and wide-spread logging have increased decomposition and dramatically decreased the distribution of Atlantic white cedar (AWC). The purpose of this study was to determine the impact of long-term drainage and AWC loss on the carbon chemistry of GDS peats. Peat cores were collected from three drained GDS vegetation communities (pocosin, AWC, and red maple-black gum) and compared to cores collected from an intact, undrained AWC peatland at the Alligator River National Wildlife Refuge (AR) in North Carolina, USA. The AR peats had higher lignin content in the deeper peat intervals, and lignin content and % organic carbon were largely invariant with depth compared to the GDS peats. The concentrations of syringyl group phenols were greater in the surface layers of GDS peats, likely reflecting the selective removal of AWC and transition from gymnosperms to angiosperms. Acid to aldehyde ratios for vanillyl and syringyl group phenols indicated that the GDS peats were more decomposed, particularly at depth, and that this occurred under aerobic conditions. Moreover, solid state 13C NMR confirmed a coincident loss of carbohydrates and increase in recalcitrant byproducts of carbohydrate degradation with depth. These data indicate that long-term drainage has accelerated the decomposition of peat at the GDS, reducing the capacity and stability of the carbon sink.

Virginia, North Carolina↗
USGS2012

Comparison of the TRM of the Yellowstone Group and the DRM of some Pearlette ash beds

Air fall ash beds (Pearlette) originating from rhyolitic eruptions in the Yellowstone‐Island Park region of Wyoming and Idaho are discontinuous but widespread throughout the western United States. Accumulation and deposition of ashes occurred in low‐energy fluvial and lacustrine environments. These ash beds have been correlated, according to their chemistry and remanent magnetism, with specific eruptions of tuffs of the Pleistocene Yellowstone Group. Type O Pearlette ash beds are normally magnetized and correlate with the Lava Creek Tuff (0.60 m.y.), whereas type S Pearlette ash beds are reversely magnetized and correlate with the Mesa Falls Tuff (1.22 m.y.). The mean direction of detrital remanent magnetization (DRM) of 11 type O Pearlette ash beds is identical to the mean direction of thermal remanent magnetization (TRM) of the Lava Creek Tuff after correcting for differences in site latitude and longitude. Considered separately, only 2 of the 13 Pearlette ash beds studied possess mean inclinations significantly shallower than, and only 4 have mean declinations significantly different from, those of their correlative tuffs. Identical directions of magnetization measured from evenly laminated and highly contorted type O ash suggest that a readjustment of magnetic grains in water‐saturated ash shortly after deposition may account for the close agreement of TRM and DRM.

Idaho, Montana, Wyoming↗
USGS2008

Cement manufacture and the environment - Part I: Chemistry and technology

Hydraulic (chiefly portland) cement is the binding agent in concrete and mortar and thus a key component of a country's construction sector. Concrete is arguably the most abundant of all manufactured solid materials. Portland cement is made primarily from finely ground clinker, which itself is composed dominantly of hydraulically active calcium silicate minerals formed through high-temperature burning of limestone and other materials in a kiln. This process requires approximately 1.7 tons of raw materials perton of clinker produced and yields about 1 ton of carbon dioxide (CO2) emissions, of which calcination of limestone and the combustion of fuels each contribute about half. The overall level of CO2 output makes the cement industry one of the top two manufacturing industry sources of greenhouse gases; however, in many countries, the cement industry's contribution is a small fraction of that from fossil fuel combustion by power plants and motor vehicles. The nature of clinker and the enormous heat requirements of its manufacture allow the cement industry to consume a wide variety of waste raw materials and fuels, thus providing the opportunity to apply key concepts of industrial ecology, most notably the closing of loops through the use of by-products of other industries (industrial symbiosis). In this article, the chemistry and technology of cement manufacture are summarized. In a forthcoming companion article (part II), some of the environmental challenges and opportunities facing the cement industry are described. Because of the size and scope of the U.S. cement industry, the analysis relies primarily on data and practices from the United States.

Journal of Industrial Ecology↗
USGS2000

Nitrite fixation by humic substances: Nitrogen-15 nuclear magnetic resonance evidence for potential intermediates in chemodenitrification

Studies have suggested that NO − 2 , produced during nitrification and denitrification, can become incorporated into soil organic matter and, in one of the processes associated with chemodenitrification, react with organic matter to form trace N gases, including N 2 O. To gain an understanding of the nitrosation chemistry on a molecular level, soil and aquatic humic substances were reacted with 15 N-labeled NaNO 2 , and analyzed by liquid phase 15 N and 13 C nuclear magnetic resonance (NMR). The International Humic Substances Society (IHSS) Pahokee peat and peat humic acid were also reacted with Na 15 NO 2 and analyzed by solid-state 15 N NMR. In Suwannee River, Armadale, and Laurentian fulvic acids, phenolic rings and activated methylene groups underwent nitrosation to form nitrosophenols (quinone monoximes) and ketoximes, respectively. The oximes underwent Beckmann rearrangements to 2° amides, and Beckmann fragmentations to nitriles. The nitriles in turn underwent hydrolysis to 1° amides. Peaks tentatively identified as imine, indophenol, or azoxybenzene nitrogens were clearly present in spectra of samples nitrosated at pH 6 but diminished at pH 3. The 15 N NMR spectrum of the peat humic acid exhibited peaks corresponding with N-nitroso groups in addition to nitrosophenols, ketoximes, and secondary Beckmann reaction products. Formation of N-nitroso groups was more significant in the whole peat compared with the peat humic acid. Carbon-13 NMR analyses also indicated the occurrence of nitrosative demethoxylation in peat and soil humic acids. Reaction of 15 N-NH 3 fixated fulvic acid with unlabeled NO − 2 resulted in nitrosative deamination of aminohydroquinone N, suggesting a previously unrecognized pathway for production of N 2 gas in soils fertilized with NH 3

Soil Science Society of America Journal↗
USGS2018

Groundwater salinity mapping using geophysical log analysis within the Fruitvale and Rosedale Ranch oil fields, Kern County, California, USA

A method is presented for deriving a volume model of groundwater total dissolved solids (TDS) from borehole geophysical and aqueous geochemical measurements. While previous TDS mapping techniques have proved useful in the hydrogeologic setting in which they were developed, they may yield poor results in settings with lithological heterogeneity, complex water chemistry, or limited data. Problems arise because of assumed values for empirical constants in Archie’s Equation, unrealistic porosity and temperature gradients, or bicarbonate-rich groundwater. These issues become critical in complex geologic settings such as the San Joaquin Valley of California, USA. To address this, a method to map TDS in three dimensions is applied to the Fruitvale and Rosedale Ranch oil fields near Bakersfield, California. Borehole resistivity, porosity, and temperature data are used to derive TDS using Archie’s Equation, and are then kriged to interpolate TDS. Archie’s a and m (tortuosity factor and cementation exponent, respectively) are found by comparing model predictions, after kriging, to TDS measurements, and minimizing the differences via mathematical optimization. Contributions of abundant bicarbonate ions to TDS were corrected using an empirical model. This work was motivated by federal and state law requirements to monitor and protect underground sources of drinking water. Modeling shows the legally significant boundary of 10,000 ppm TDS is at ~1,067 m below sea level in Rosedale Ranch, and deepens into Fruitvale to ~1,341 m. Mapping groundwater TDS at this resolution reveals that TDS is primarily controlled by depth, recharge, stratigraphy, and in some places, by faulting and facies changes.

California↗
USGS2008

Limited occurrence of denitrification in four shallow aquifers in agricultural areas of the United States

The ability of natural attenuation to mitigate agricultural nitrate contamination in recharging aquifers was investigated in four important agricultural settings in the United States. The study used laboratory analyses, field measurements, and flow and transport modeling for monitoring well transects (0.5 to 2.5 km in length) in the San Joaquin watershed, California, the Elkhorn watershed, Nebraska, the Yakima watershed, Washington, and the Chester watershed, Maryland. Ground water analyses included major ion chemistry, dissolved gases, nitrogen and oxygen stable isotopes, and estimates of recharge date. Sediment analyses included potential electron donors and stable nitrogen and carbon isotopes. Within each site and among aquifer-based medians, dissolved oxygen decreases with ground water age, and excess N 2 from denitrification increases with age. Stable isotopes and excess N 2 imply minimal denitrifying activity at the Maryland and Washington sites, partial denitrification at the California site, and total denitrification across portions of the Nebraska site. At all sites, recharging electron donor concentrations are not sufficient to account for the losses of dissolved oxygen and nitrate, implying that relict, solid phase electron donors drive redox reactions. Zero-order rates of denitrification range from 0 to 0.14 μmol N L −1 d −1 , comparable to observations of other studies using the same methods. Many values reported in the literature are, however, orders of magnitude higher, which is attributed to a combination of method limitations and bias for selection of sites with rapid denitrification. In the shallow aquifers below these agricultural fields, denitrification is limited in extent and will require residence times of decades or longer to mitigate modern nitrate contamination.

Journal of Environmental Quality↗
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↗
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↗
USGS2001

Modeling consolidation and dewatering near the toe of the northern Barbados accretionary complex

At the toe of the northern Barbados accretionary complex, temperature and pore water chemistry data indicate that fluid flow is channeled along the décollement and other shallow thrust faults. We examine mechanisms that may prevent consolidation and maintain high permeability over large sections of the décollement. High-resolution bulk density data from five boreholes show that the décollement is well consolidated at some sites while other sites remain underconsolidated. Underconsolidated décollement behavior is associated with kilometer-scale negative-polarity seismic reflections from the décollement plane that have been interpreted to be fluid conduits. We use a coupled fluid flow/consolidation model to simulate the loading response of a 10-km-long by 680-m-thick slice of sediment as it enters the accretionary complex. The simulations capture 185 ka (5 km) of subduction, with a load function representing the estimated effective stress of the overriding accretionary prism (3.8° taper angle). Simulation results of bulk density in the décollement 3.2 km arcward of the deformation front are compared with observations. The results show that persistent high pore pressures at the arcward edge of the simulation domain can explain underconsolidated behavior. The scenario is consistent with previous modeling results showing that high pore pressures can propagate intermittently along the décollement from deeper in the complex. Simulated seaward fluxes in the décollement (1–14 cm yr −1 ) lie between previous estimates from modeling studies of steady state (<1 cm yr −1 ) and transient (>1 m yr −1 ) flow. Maximum simulated instantaneous fluid sources (2.5×10 −13 s −1 ) are comparable to previous estimates. The simulations show minor swelling of incoming sediments (fluid sources ∼−3×10 −15 s −1 ) up to 3 km before subduction that may help to explain small-scale shearing and normal faulting proximal to the protodécollement.

Atlantic Ocean, Northern Barbados Accretionary Com↗