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R.C. Burruss

Publications and source records attributed to R.C. Burruss.

At least 19 recordsLinked to original sources

Diagenetic palaeotemperatures from aqueous fluid inclusions: re-equilibration of inclusions in carbonate cements by burial heating

Diagenetic palaeotemperatures determined from aqueous fluid inclusions can be affected by re-equilibration during burial heating. Calculations based on the observed behaviour of inclusions in fluorite under external confining pressure allows prediction of the temperatures and depths of burial necessary to initiate re-equilibration of aqueous inclusions in the common size range 40 to 4 µm. Heating of 20° to 60°C over the initial trapping temperature may cause errors of 10° to 20°C in the homogenization temperature. This suggests re-equilibration may cause aqueous inclusions in carbonates to yield a poor record of their low-temperature history, but a useful record of the maximum temperature experienced by the host rock. Previous work suggests inclusions containing petroleum fluids will be less susceptible to re-equilibration.

Mineralogical Magazine

Determination of diffusion coefficients of carbon dioxide in water between 268 and 473 K in a high-pressure capillary optical cell with in situ Raman spectroscopic measurements

Accurate values of diffusion coefficients for carbon dioxide in water and brine at reservoir conditions are essential to our understanding of transport behavior of carbon dioxide in subsurface pore space. However, the experimental data are limited to conditions at low temperatures and pressures. In this study, diffusive transfer of carbon dioxide in water at pressures up to 45 MPa and temperatures from 268 to 473 K was observed within an optical capillary cell via time-dependent Raman spectroscopy. Diffusion coefficients were estimated by the least-squares method for the measured variations in carbon dioxide concentration in the cell at various sample positions and time. At the constant pressure of 20 MPa, the measured diffusion coefficients of carbon dioxide in water increase with increasing temperature from 268 to 473 K. The relationship between diffusion coefficient of carbon dioxide in water [D(CO 2 ) in m 2 /s] and temperature (T in K) was derived with Speedy–Angell power-law approach as: D(CO 2 )=D 0 [T/Ts-1] m where D 0 = 13.942 × 10 −9 m 2 /s, Ts = 227.0 K, and m = 1.7094. At constant temperature, diffusion coefficients of carbon dioxide in water decrease with pressure increase. However, this pressure effect is rather small (within a few percent).

Geochimica et Cosmochimica Acta

Carbon and hydrogen isotopic evidence for the origin of combustible gases in water-supply wells in north-central Pennsylvania

The origin of the combustible gases in groundwater from glacial-outwash and fractured-bedrock aquifers was investigated in northern Tioga County, Pennsylvania. Thermogenic methane (CH 4 ) and ethane (C 2 H 6 ) and microbial CH 4 were found. Microbial CH 4 is from natural in situ processes in the shale bedrock and occurs chiefly in the bedrock aquifer. The δ 13 C values of CH 4 and C 2 H 6 for the majority of thermogenic gases from water wells either matched or were between values for the samples of non-native storage-field gas from injection wells and the samples of gas from storage-field observation wells. Traces of C 2 H 6 with microbial CH 4 and a range of C and H isotopic compositions of CH 4 indicate gases of different origins are mixing in sub-surface pathways; gas mixtures are present in groundwater. Pathways for gas migration and a specific source of the gases were not identified. Processes responsible for the presence of microbial gases in groundwater could be elucidated with further geochemical study.

Pennsylvania

Carbon and hydrogen isotopic reversals in deep basin gas: Evidence for limits to the stability of hydrocarbons

During studies of unconventional natural gas reservoirs of Silurian and Ordovician age in the northern Appalachian basin we observed complete reversal of the normal trend of carbon isotopic composition, such that ??13C methane (C1) >??13C ethane (C2) >??13C propane (C3). In addition, we have observed isotopic reversals in the ??2H in the deepest samples. Isotopic reversals cannot be explained by current models of hydrocarbon gas generation. Previous observations of partial isotopic reversals have been explained by mixing between gases from different sources and thermal maturities. We have constructed a model which, in addition to mixing, requires Rayleigh fractionation of C2 and C3 to cause enrichment in 13C and create reversals. In the deepest samples, the normal trend of increasing enrichment of 13C and 2H in methane with increasing depth reverses and 2H becomes depleted as 13C becomes enriched. We propose that the reactions that drive Rayleigh fractionation of C2 and C3 involve redox reactions with transition metals and water at late stages of catagenesis at temperatures on the order of 250-300??C. Published ab initio calculated fractionation factors for C-C bond breaking in ethane at these temperatures are consistent with our observations. The reversed trend in ??2H in methane appears to be caused by isotopic exchange with formation water at the same temperatures. Our interpretation that Rayleigh fractionation during redox reactions is causing isotopic reversals has important implications for natural gas resources in deeply buried sedimentary basins. ?? 2010.

Organic Geochemistry

Determination of methane concentrations in water in equilibrium with sI methane hydrate in the absence of a vapor phase by in situ Raman spectroscopy

Most submarine gas hydrates are located within the two-phase equilibrium region of hydrate and interstitial water with pressures (P) ranging from 8 to 60 MPa and temperatures (T) from 275 to 293 K. However, current measurements of solubilities of methane in equilibrium with hydrate in the absence of a vapor phase are limited below 20 MPa and 283.15 K, and the differences among these data are up to 30%. When these data were extrapolated to other P-T conditions, it leads to large and poorly known uncertainties. In this study, in situ Raman spectroscopy was used to measure methane concentrations in pure water in equilibrium with sI (structure one) methane hydrate, in the absence of a vapor phase, at temperatures from 276.6 to 294.6 (??0.3) K and pressures at 10, 20, 30 and 40 (??0.4%) MPa. The relationship among concentration of methane in water in equilibrium with hydrate, in mole fraction [X(CH4)], the temperature in K, and pressure in MPa was derived as: X(CH4) = exp [11.0464 + 0.023267 P - (4886.0 + 8.0158 P)/T]. Both the standard enthalpy and entropy of hydrate dissolution at the studied T-P conditions increase slightly with increasing pressure, ranging from 41.29 to 43.29 kJ/mol and from 0.1272 to 0.1330 kJ/K ?? mol, respectively. When compared with traditional sampling and analytical methods, the advantages of our method include: (1) the use of in situ Raman signals for methane concentration measurements eliminates possible uncertainty caused by sampling and ex situ analysis, (2) it is simple and efficient, and (3) high-pressure data can be obtained safely. ?? 2007 Elsevier Ltd. All rights reserved.

Geochimica et Cosmochimica Acta

Specific storage volumes: A useful tool for CO2 storage capacity assessment

Subsurface geologic strata have the potential to store billions of tons of anthropogenic CO2; therefore, geologic carbon sequestration can be an effective mitigation tool used to slow the rate at which levels of atmospheric CO2 are increasing. Oil and gas reservoirs, coal beds, and saline reservoirs can be used for CO2 storage; however, it is difficult to assess and compare the relative storage capacities of these different settings. Typically, CO2 emissions are reported in units of mass, which are not directly applicable to comparing the CO2 storage capacities of the various storage targets. However, if the emission values are recalculated to volumes per unit mass (specific volume) then the volumes of geologic reservoirs necessary to store CO2 emissions from large point sources can be estimated. The factors necessary to convert the mass of CO2 emissions to geologic storage volume (referred to here as Specific Storage Volume or 'SSV') can be reported in units of cubic meters, cubic feet, and petroleum barrels. The SSVs can be used to estimate the reservoir volume needed to store CO2 produced over the lifetime of an individual point source, and to identify CO2 storage targets of sufficient size to meet the demand from that given point source. These storage volumes also can then be projected onto the land surface to outline a representative "footprint," which marks the areal extent of storage. This footprint can be compared with the terrestrial carbon sequestration capacity of the same land area. The overall utility of this application is that the total storage capacity of any given parcel of land (from surface to basement) can be determined, and may assist in making land management decisions. ?? Springer Science+Business Media, LLC 2006.

Natural Resources Research

In situ study of mass transfer in aqueous solutions under high pressures via Raman spectroscopy: A new method for the determination of diffusion coefficients of methane in water near hydrate formation conditions

A new method was developed for in situ study of the diffusive transfer of methane in aqueous solution under high pressures near hydrate formation conditions within an optical capillary cell. Time-dependent Raman spectra of the solution at several different spots along the one-dimensional diffusion path were collected and thus the varying composition profile of the solution was monitored. Diffusion coefficients were estimated by the least squares method based on the variations in methane concentration data in space and time in the cell. The measured diffusion coefficients of methane in water at the liquid (L)-vapor (V) stable region and L-V metastable region are close to previously reported values determined at lower pressure and similar temperature. This in situ monitoring method was demonstrated to be suitable for the study of mass transfer in aqueous solution under high pressure and at various temperature conditions and will be applied to the study of nucleation and dissolution kinetics of methane hydrate in a hydrate-water system where the interaction of methane and water would be more complicated than that presented here for the L-V metastable condition. ?? 2006 Society for Applied Spectroscopy.

Applied Spectroscopy

Geochemical investigation of the potential for mobilizing non-methane hydrocarbons during carbon dioxide storage in deep coal beds

Coal samples of different rank (lignite to anthracite) were extracted in the laboratory with supercritical CO2 (40 ??C; 10 MPa) to evaluate the potential for mobilizing non-methane hydrocarbons during CO2 storage (sequestration) or enhanced coal bed methane recovery from deep (???1-km depth) coal beds. The total measured alkane concentrations mobilized from the coal samples ranged from 3.0 to 64 g tonne-1 of dry coal. The highest alkane concentration was measured in the lignite sample extract; the lowest was measured in the anthracite sample extract. Substantial concentrations of polycyclic aromatic hydrocarbons (PAHs) were also mobilized from these samples: 3.1 - 91 g tonne-1 of dry coal. The greatest amounts of PAHs were mobilized from the high-volatile bituminous coal samples. The distributions of aliphatic and aromatic hydrocarbons mobilized from the coal samples also varied with rank. In general, these variations mimicked the chemical changes that occur with increasing degrees of coalification and thermal maturation. For example, the amount of PAHs mobilized from coal samples paralleled the general trend of bitumen formation with increasing coal rank. The coal samples yielded hydrocarbons during consecutive extractions with supercritical CO2, although the amount of hydrocarbons mobilized declined with each successive extraction. These results demonstrate that the potential for supercritical CO2 to mobilize non-methane hydrocarbons from coal beds, and the effect of coal rank on this process, are important to consider when evaluating deep coal beds for CO2 storage.

Energy and Fuels

Diamond-anvil cell observations of a new methane hydrate phase in the 100-MPa pressure range

A new high-pressure phase of methane hydrate has been identified based on its high optical relief, distinct pressure-temperature phase relations, and Raman spectra. In-situ optical observations were made in a hydrothermal diamond-anvil cell at temperatures between -40?? and 60 ??C and at pressures up to 900 MPa. Two new invariant points were located at -8.7 ??C and 99 MPa for the assemblage consisting of the new phase, structure I methane hydrate, ice Ih, and water, and at 35.3 ??C and 137 MPa for the new phase-structure I methane hydrate-water-methane vapor. Existence of the new phase is critical for understanding the phase relations among the hydrates at low to moderate pressures, and may also have important implications for understanding the hydrogen bonding in H2O and the behavior of water in the planetary bodies, such as Europa, of the outer solar system.

Journal of Physical Chemistry A

Transformations in methane hydrates

Detailed study of pure methane hydrate in a diamond cell with in situ optical, Raman, and x-ray microprobe techniques reveals two previously unknown structures, structure II and structure H, at high pressures. The structure II methane hydrate at 250 MPa has a cubic unit cell of a = 17.158(2) A?? and volume V = 5051.3(13) A??3; structure H at 600 MPa has a hexagonal unit cell of a = 11.980(2) A??, c = 9.992(3) A??, and V = 1241.9(5) A??3. The compositions of these two investigated phases are still not known. With the effects of pressure and the presence of other gases in the structure, the structure II phase is likely to dominate over the known structure I methane hydrate within deep hydrate-bearing sediments underlying continental margins.

Proceedings of the National Academy of Sciences of

Paleofluid-flow circulation within a Triassic rift basin: Evidence from oil inclusions and thermal histories

The migration of subsurface fluid flow within continental rift basins has been increasingly recognized to significantly affect the thermal history of sediments and petroleum formation. To gain insight into these paleofluid flow effects, the thermal history of the Taylorsville basin in Virginia was reconstructed from fluid-inclusion studies, apatite fission-track data, and vitrinite reflectance data. Models of thermal history indicate that the basin was buried to the thermal maximum at 200 Ma; a cooling event followed during which the eastern side of the basin cooled earlier and faster than the western side, suggesting that there was a differential uplift and topographically driven fluid flow. This hypothesis is supported by analyses of secondary oil and aqueous inclusions trapped in calcite and quartz veins during the uplift stage. Gas chromatograms of inclusion oils exhibit variable but extensive depletion of light molecular-weight hydrocarbons. The relative abundance of n-alkanes, petrographic observations, and the geological data indicate that the alteration process on these inclusion oils was probably neither phase separation nor biodegradation, but water washing. Water:oil ratios necessary to produce the observed alteration are much greater than 10000:1. These exceedingly high ratios are consistent with the migration of inclusion oils along with fluid flow during the early stages of basin evolution. The results provide significant evidence about the role of a subsurface flow system in modifying the temperature structure of the basin and the composition of petroleum generated within the basin.

Geological Society of America Bulletin

Extremely acid Permian lakes and ground waters in North America

Evaporites hosted by red beds (red shales and sandstones), some 275-265 million years old, extend over a large area of the North American mid- continent. They were deposited in non-marine saline lakes, pans and mud- flats, settings that are typically assumed to have been alkaline. Here we use laser Raman microprobe analyses of fluid inclusions trapped in halites from these Permian deposits to argue for the existence of highly acidic (pH < 1) lakes and ground waters. These extremely acidic systems may have extended over an area of 200,000 km2. Modern analogues of such systems may be natural acid lake and groundwater systems (pH ~2-4) in southern Australia. Both the ancient and modern acid systems are characterized by closed drainage, arid climate, low acid-neutralizing capacity, and the oxidation of minerals such as pyrite to generate acidity. The discovery of widespread ancient acid lake and groundwater systems demands a re-evaluation of reconstructions of surface conditions of the past, and further investigations of the geochemistry and ecology of acid systems in general.

Nature

Water quality in the vicinity of Mosquito Creek Lake, Trumbull County, Ohio, in relation to the chemistry of locally occurring oil, natural gas, and brine

Environmental samples collected in the Mosquito Creek Lake area were used to characterize water quality in relation to the chemistry of locally occurring oil, natural gas, and brine and to establish baseline water quality. Mosquito Creek Lake (a manmade reservoir) and the shallow bedrock aquifers near the lake are major sources of potable water in central Trumbull County. The city of Warren relies on the lake as a sole source of potable water. Some of the lake bottom may be in direct hydraulic connection with the underlying aquifers. The city of Cortland, along the southeastern shore of the lake, relies on the Cussewago Sandstone aquifer as a sole source of potable water. This aquifer subcrops beneath the glacio-fluvial sediments that underlie the lake. Nearly all residential homes around the lake, with the exception of homes in the city of Cortland, rely on domestic supply wells as a source of potable water. Oil and natural gas exploration and production have been ongoing in the Mosquito Creek Lakearea since the discovery of the historic Mecca Oil Pool in the Mississippian Berea and Cussewago Sandstones in 1860. Since the late 1970' s, the major drilling objective and zone of production is the Lower Silurian Clinton sandstone. The oil and natural gas resources of the Mosquito Creek Lake area, including reservoir pressure, production history, and engineering and abandonment practices are described in this report. The chemical and isotopic characteristics of the historic Mecca oil and natural gas are very different than those of the Clinton sandstone oil and natural gas. Gas chromatograms show that Mecca oil samples are extensively altered by biodegradation, whereas Clinton sandstone oils are not. Extensive alteration of Mecca oil is consistent with their occurrence at very shallow depths (less than 100 ft below land surface) where microbial activity can affect their composition. Also, the carbon-isotope composition of dissolved methane gas from Berea and Cussewago Sandstone water samples indicates that the gas is microbially generated, whereas the Clinton sandstone gases are thermogenically generated. Methane gas, in addition to crude oil, occurs naturally in the shallow Berea and Cussewago Sandstone aquifers in the Mosquito Creek Lake area and concentrations of dissolved methane are significant in the city of Cortland public-supply wells and in the domestic-supply wells near the southern shore of the lake. Water associated with oil and gas in the Clinton sandstone is a brine with high concentrations of chloride. Water from the Berea and Cussewago Sandstones, however, is fresh and potable. The contrasting geochemical characteristics are important for addressing water-quality issues that relate to oil and natural gas development in the Mosquito Creek area. A reexamination of the geologic framework and results of a subsurface-gas survey show that crude oil in the historic Mecca Oil Pool probably does not seep into Mosquito Creek Lake. Environmental samples show no evidence of any measurable release of oil, gas, or brine from the deeper Clinton sandstone oil and gas wells to the shallow aquifers, the lake, or lake tributaries. Brine is not associated with the hydrocarbons in the shallow Berea-Cussewago aquifer system and therefore cannot be a source of brine contamination. A mixing diagram constructed for dissolved bromide and chloride in surface water and water-supply wells shows no demonstrable mixing of these water resources with brine from the Clinton sandstone. There is some notable salinity in surface waters; however, the water is bromide poor, and a mixing diagram indicates that some local ground waters are influenced by halite solutions, presumably derived from leaching of road salt or from septic effluent.

Ohio

Constraints on the thermal history of Taylorsville Basin, Virginia, U.S.A., from fluid-inclusion and fission-track analyses: Implications for subsurface geomicrobiology experiments

Microbial populations have been found at the depth of 2621-2804 m in a borehole near the center of Triassic Taylorsville Basin, Virginia. To constrain possible scenarios for long-term survival in or introduction of these microbial populations to the deep subsurface, we attempted to refine models of thermal and burial history of the basin by analyzing aqueous and gaseous fluid inclusions in calcite/quartz veins or cements in cuttings from the same borehole. These results are complemented by fission-track data from the adjacent boreholes. Homogenization temperatures of secondary aqueous fluid inclusions range from 120?? to 210??C between 2027- and 3069-m depth, with highest temperatures in the deepest samples. The salinities of these aqueous inclusions range from 0 to ??? 4.3 eq wt% NaCl. Four samples from the depth between 2413 and 2931 m contain both two-phase aqueous and one-phase methane-rich inclusions in healed microcracks. The relative CH4 and CO2 contents of these gaseous inclusions was estimated by microthermometry and laser Raman spectroscopy. If both types of inclusions in sample 2931 m were trapped simultaneously, the density of the methane-rich inclusions calculated from the Peng - Robinson equation of state implies an entrapment pressure of 360 ?? 20 bar at the homogenization temperature (162.5 ?? 12.5??C) of the aqueous inclusions. This pressure falls between the hydrostatic and lithostatic pressures at the present depth 2931 m of burial. If we assume that the pressure regime was hydrostatic at the time of trapping, then the inclusions were trapped at 3.6 km in a thermal gradient of ??? 40??C/km. The high temperatures recorded by the secondary aqueous inclusions are consistent with the pervasive resetting of zircon and apatite fission-track dates. In order to fit the fission-track length distributions of the apatite data, however, a cooling rate of 1-2??C/Ma following the thermal maximum is required. To match the integrated dates, the thermal maximum would have occurred at ??? 200 Ma. The timing of the maximum temperature is consistent with rapid burial of the Taylorsville Basin to twice its present-day depth and thermal re-equilibration with a 40??C/km geothermal gradient, followed by slow exhumation. The results may imply that the microorganisms did not survive in situ, but were transported from the cooler portions of the basin sometime after maximum burial and heating.

Chemical Geology

Petrogenesis and geological history of a uranium source rock: a case study in northeastern Washington, U.S.A.

A small (4 km 2 ) drainage basin in northeastern Washington contains highly uraniferous groundwater and highly uraniferous peaty sediments of Holocene age. The U is derived from granitic bedrock that underlies the entire drainage basin and that contains 9–16 ppm U. This local bedrock was studied by petrographic, chemical and isotopic methods to determine conditions of its petrogenesis and post-emplacement history that may have contributed to its present high U content and source-rock capability. The original magma was derived by anatexis of Precambrian continental crust of probable mixed metaigneous and metasedimentary character. Mineral-melt partitioning controlled the enrichment of U in chemically evolved phases of the crystallizing melt. Following emplacement in the upper crust at ∼100Ma, the pluton interacted with meteoric-hydrothermal water at ambient temperatures 300°C. Locally intense fracturing promoted alteration, and fracturing and alteration probably continued during later regional uplift in the Eocene. Regional uplift was followed by low-temperature alteration and weathering in the middle to late Tertiary. The combined result of hydrothermal alteration and low-temperature alteration and weathering was the redistribution of U from primary mineral hosts such as allanite to new sites on fracture surfaces and in secondary minerals such as hematite. Zones of highly fractured and altered rock show the most obvious evidence of this process. A model is proposed in which high-angle fractures beneath the drainage basin were the sites of Tertiary supergene enrichments of U. Recent glacio-isostatic uplift has elevated these older enriched zones to shallow levels where they are now being leached by oxidizing groundwater. The chemistry, mineralogy, texture and geological history of this U source-rock suggest criteria for locating other granitic terrane that may contain uraniferous waters and associated young surficial U deposits. The details of U distribution and mobility at this site also apply to the general topic of U mobility in granitic rocks.

Washington