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1.
Small angle neutron scattering techniques have been applied to investigate the phase behavior of CO2 injected into coal and possible changes in the coal pore structure that may result from this injection. Three coals were selected for this study: the Seelyville coal from the Illinois Basin (Ro = 0.53%), Baralaba coal from the Bowen Basin (Ro = 0.67%), and Bulli 4 coal from the Sydney Basin (Ro = 1.42%). The coals were selected from different depths to represent the range of the underground CO2 conditions (from subcritical to supercritical) which may be realized in the deep subsurface environment. The experiments were conducted in a high pressure cell and CO2 was injected under a range of pressure conditions, including those corresponding to in-situ hydrostatic subsurface conditions for each coal. Our experiments indicate that the porous matrix of all coals remains essentially unchanged after exposure to CO2 at pressures up to 200 bar (1 bar = 105 Pa). Each coal responds differently to the CO2 exposure and this response appears to be different in pores of various sizes within the same coal. For the Seelyville coal at reservoir conditions (16 °C, 50 bar), CO2 condenses from a gas into liquid, which leads to increased average fluid density in the pores (ρpore) with sizes (r) 1 × 105 ≥ r ≥ 1 × 104 Å (ρpore ≈ 0.489 g/cm3) as well as in small pores with size between 30 and 300 Å (ρpore ≈ 0.671 g/cm3). These values are by a factor of three to four higher than the density of bulk CO2 (ρCO2) under similar thermodynamic conditions (ρCO2 ≈ 0.15 g/cm3). At the same time, in the intermediate size pores with r ≈ 1000 Å the average fluid density is similar to the density of bulk fluid, which indicates that adsorption does not occur in these pores. At in situ conditions for the Baralaba coal (35 OC, 100 bar), the average fluid density of CO2 in all pores is lower than that of the bulk fluid (ρpore / ρCO2 ≈ 0.6). Neutron scattering from the Bulli 4 coal did not show any significant variation with pressure, a phenomenon which we assign to the extremely small amount of porosity of this coal in the pore size range between 35 and 100,000 Å.  相似文献   

2.
CO2, CH4, and N2 adsorption and gas-induced swelling were quantified for block Blind Canyon, Pittsburgh #8 and Pocahontas Argonne Premium coals that were dried and structurally relaxed at 75 °C in vacuum. Strain measurements were made perpendicular and parallel to the bedding plane on ~ 7 × 7 × 7 mm3 coal blocks and gravimetric sorption measurements were obtained simultaneously on companion coal blocks exposed to the same gaseous environment. The adsorption amount and strain were determined after equilibration at P  ≤ 1.8 MPa. There is a strong non-linear correlation between strain and the quantity of gas adsorbed and the results for all gases and coals studied follow a common pattern. The dependence of the coal matrix shrinkage/swelling coefficient (Cgc) on the type and quantity of gas adsorbed is seen by plotting the ratio between the strain and the adsorbate concentration against the adsorbate concentration. In general, Cgc increases with increasing adsorbate concentration over the range of ~ 0.1 to 1.4 mmol/g. Results from the dried block coals are compared to CO2 experiments using native coals with an inherent level of moisture as received. The amount of CO2 adsorbed using native coals (assuming no displacement of H2O by CO2) is significantly less than the dried coals. The gas-induced strain (S) and adsorption amount (M) were measured as a function of time following step changes in CO2, CH4, and N2 pressure from vacuum to 1.8 MPa. An empirical diffusion equation was applied to the kinetic data to obtain the exponent (n) for time dependence for each experiment. The data for all coals were pooled and the exponent (n) evaluated using an ANOVA statistical analysis method. Values for (n) near 0.5 were found to be independent on the coal, the gas or type of measurement (e.g., parallel strain, perpendicular strain, and gas uptake). These data support the use of a Fickian diffusion model framework for kinetic analysis. The kinetic constant k was determined using a unipore diffusion model for each experiment and the data were pooled for ANOVA analysis. For dry coal, statistically significant differences for k were found for the gases (CO2 > N2 > CH4) and coals (Pocahontas >Blind Canyon > Pittsburgh #8) but not for the method of the kinetic measurement (e.g., strain or gas uptake). For Blind Canyon and Pittsburgh #8 coal, the rate of CO2 adsorption and gas-induced strain for dry coal was significantly greater than that of the corresponding native coal. For Pocahontas coal the rates of CO2 adsorption and gas-induced strain for dry and native coal were indistinguishable and may be related to its low native moisture and minimal amount of created porosity upon drying.  相似文献   

3.
Coal is present in the Alberta Foothills/Mountains in five zones: the Kootenay, Gething, Gates, Brazeau and Coalspur coal zones. For coalbed-methane (CBM) evaluation purposes, they can be divided into shallow (less than 1000 m depth) and deep (greater than 1000 m depth) coal zones. The potential gas content of all shallow coal zones totals about 878 × 109 m3 (31 Tcf) of CBM, which is considered an inferred, initial, in-place, coalbed-methane resource estimate based on limited data. The limited amount of data on formation testing and measured gas content indicate that the inferred resource is bordering on the speculative category.The gas content of all deep coal zones (deeper than 1000 m) totals 2.8 × 1012 m3 (about 99 Tcf) of in-place coalbed-methane gas. Consequently, the total ultimate coalbed-methane resource could be 3.7 × 1012 m3 (130 Tcf). However, coalbed-methane recovery from deep coals is generally not attempted because of the high cost of drilling and the low permeability that results from high overburden load and stress.The only (limited) Foothills coalbed-methane production has been from the southern Alberta Kootenay Coal Zone, which is very prospective for coalbed-methane production. The shallow Gates Coal Zone in the central and northern Foothills is also prospective, but needs to be better tested. The best potential for coalbed methane in the Coalspur Coal Zone is in the Edson area (Entrance Syncline and Triangle Zone). The Kootenay and Gates coal zones are not well defined in the northern part of the Calgary (NTS 82O) map sheet.  相似文献   

4.
Small angle scattering techniques (SAXS and SANS) have been used to investigate the microstructural properties of the subbituminous coals (Rmax 0.42–0.45%) from the Huntly Coalfield, New Zealand. Samples were collected from the two thick (> 5 m) coal seams in the coalfield and have been analysed for methane and carbon dioxide sorption capacity, petrography, pore size distribution, specific surface area and porosity.Specific surface area (SSA) available for carbon dioxide adsorption, extrapolated to a probe size of 4 Å, ranged from 1.25 × 106 cm? 1 to 4.26 × 106 cm? 1 with total porosity varying from 16% to 25%. Porosity was found to be predominantly composed of microporosity, which contributed the majority of the available SSA. Although considerable variation was seen between samples, the results fit well with published rank trends.Gas holding capacity at the reservoir pressure (approximately 4 MPa) ranged from 2.63 to 4.18 m3/t for methane on a dry, ash-free basis (daf) and from 22.00 to 23.72 m3/t daf for carbon dioxide. The resulting ratio of CO2:CH4 ranged from 5.7 to 8.6, with an average of 6.7:1.Holding capacities for both methane and carbon dioxide on a dry ash free basis (daf) were found to be correlated with sample microporosity. However, holding capacities for the two gases on an as analysed (aa) basis (that is including mineral matter and moisture), showed no such correlation. Carbon dioxide (aa) does show a negative correlation with both specific surface area and microporosity. As the coals have low inorganic matter content, the reversal is thought to be related to moisture which is likely concentrated in the pore size range 12.5–125 Å. Methane holding capacity, both daf and aa, correlates with macroporosity, thus suggesting that the holding capacity of micropores is diminished by the presence of moisture in the pores.  相似文献   

5.
Stable isotopes of injected CO2 act as useful tracers in carbon capture and storage (CCS) because the CO2 itself is the carrier of the tracer signal and remains unaffected by sorption or partitioning effects. At the Ketzin pilot site (Germany), carbon stable isotope composition (δ13C) of injected CO2 at the injection well was analyzed over a time period of 4 months. Occurring isotope variances resulted from the injection of CO2 from two different sources (an oil refinery and a natural gas-reservoir). The two gases differed in their carbon isotope composition by more than 27‰. In order to find identifiable patterns of these variances in the reservoir, more than 250 CO2-samples were collected and analyzed for their carbon isotope ratios at an observation well 100 m distant from the injection well. An isotope ratio mass spectrometer connected to a modified Thermo Gasbench system allowed quick and cost effective isotope analyses of a high number of CO2 gas specimens. CO2 gas from the oil refinery (δ13C = −30.9‰, source A) was most frequently injected and dominated the reservoir δ13C values at the injection site. Sporadic injection of the CO2 from the natural gas-reservoir (δ13C = −3.5‰, source B) caused isotope shifts of up to +5‰ at the injection well. These variances provided a potential ideal tracer for CO2 migration behavior. Based on these findings, tracer input signals that were injected during the last 2 years of injection could be reconstructed with the aid of an isotope mixing model and CO2 delivery schedules. However, in contrast to the injection well, δ13C values at the observation well showed no variances and a constant value of −28.5‰ was measured at 600 m depth. This is in disagreement with signals that would be expected if the input signals from the injection would arrive at the observation well. The lack of isotope signals at the observation well suggests that parts of the reservoir are filled with CO2 that is immobilized.  相似文献   

6.
Time- and position-resolved synchrotron small angle X-ray scattering data were acquired from samples of two Australian coal seams: Bulli seam (Bulli 4, Ro = 1.42%, Sydney Basin), which naturally contains CO2 and Baralaba seam (Ro = 0.67%, Bowen Basin), a potential candidate for sequestering CO2. This experimental approach has provided unique, pore-size-specific insights into the kinetics of CO2 sorption in the micro- and small mesopores (diameter 5 to 175 Å) and the density of the sorbed CO2 at reservoir-like conditions of temperature and hydrostatic pressure.For both samples, at pressures above 5 bar, the density of CO2 confined in pores was found to be uniform, with no densification in near-wall regions. In the Bulli 4 sample, CO2 first flooded the slit pores between polyaromatic sheets. In the pore-size range analysed, the confined CO2 density was close to that of the free CO2. The kinetics data are too noisy for reliable quantitative analysis, but qualitatively indicate faster kinetics in mineral-matter-rich regions.In the Baralaba sample, CO2 preferentially invaded the smallest micropores and the confined CO2 density was up to five times that of the free CO2. Faster CO2 sorption kinetics was found to be correlated with higher mineral matter content but, the mineral-matter-rich regions had lower-density CO2 confined in their pores. Remarkably, the kinetics was pore-size dependent, being faster for smaller pores.These results suggest that injection into the permeable section of an interbedded coal-clastic sequence could provide a viable combination of reasonable injectivity and high sorption capacity.  相似文献   

7.
Boom Clay is studied as a potential host formation for the disposal of high-and intermediate level long-lived radioactive waste in Belgium. In such a geological repository, generation of gases (mainly H2 from anaerobic corrosion) will be unavoidable. In order to make a good evaluation of the balance between gas generation vs. gas dissipation for a particular waste form and/or disposal concept, good estimates for gas diffusion coefficients of dissolved gases are essential. In order to obtain an accurate diffusion coefficient for dissolved hydrogen in saturated Boom Clay, diffusion experiments were performed with a recently developed through-diffusion set-up for dissolved gases. Due to microbial activity in the test set-up, conversion of hydrogen into methane was observed within several experiments. A complex sterilisation procedure was therefore developed in order to eliminate microbiological disturbances. Only by a combination of heat sterilisation, gamma irradiation and the use of a microbial inhibitor, reliable, reproducible and accurate H2(g) diffusion coefficients (measured at 21 °C) for samples oriented parallel (Deff = 7.25 × 10−10 m2/s and Deff = 5.51 × 10−10 m2/s) and perpendicular (Deff = 2.64 × 10−10 m2/s) to the bedding plane were obtained.  相似文献   

8.
Three sets of pyrolysis experiments were performed on extracted coal (Ro% 0.39), coal (initial bitumen 13.5 mg/g coal) and bitumen enriched coal (total bitumen 80.9 mg/g coal) at two heating rates of 2 °C/h and 20 °C/h in confined systems (gold capsules). For all three experiments, the yields of bitumen, Σn-C8+, aromatic components and ΣC2–5 at first increase and then decrease with increasing EASY%Ro and reach the highest values within the EASY%Ro ranges of 0.67–1.08, 1.07–1.19, 1.46–1.79 and 1.46–1.68, respectively. In contrast, C1/ΣC1–5 ratio at first decreases and then increases with EASY%Ro and reaches a minimum value in EASY%Ro range of 0.86–1.08, closely corresponding to the maximum values of the yields of bitumen and Σn-C8+. Methane yields increase consistently with EASY%Ro. Nearly half of the maximum yield of methane from kerogen was generated at EASY%Ro > 2.2. The differences in methane yields among the three experiments at the same thermal stress are relatively minor at EASY%Ro < 2.2, but are greater with thermal stress at EASY%Ro > 2.2. This demonstrates that the kerogen always retained relatively more hydrogen and hydrocarbon generative potential at the postmature stage of bitumen rich coal than the extracted coal or coal.The maximum yield of ethane is 20–25% higher in the bitumen rich coal experiment than the extracted coal or coal, while the maximum yields of C3, C4 and C5 in the former are double to triple those in the latter. This result demonstrates that the added bitumen in bitumen rich coal substantially increased the generation of these wet gases. However, the averaged values of activation energies (with the same frequency factors) for both the generation and cracking of individual wet gases are similar and do not show consistent trends among the three experiments. For all three experiments, activation energies for the generation and cracking of wet gases are significantly lower than those in previously published oil pyrolysis experiments with same frequency factors (Pan et al., 2012; Organic Geochemistry 45, 29–47). Methane δ13C values at the maximum temperature or EASY%Ro are close to those of initial wet gases, especially C3, implying that the major part of methane shared a common initial precursor with wet gases, i.e., free and bound liquid alkanes.  相似文献   

9.
Chemical and isotopic compositions have been measured for CO2-rich bubbling gases discharging from cold springs in Wudalianchi intra-plate volcanic area, NE China. Observed 3He/4He ratios (2–3 RA) and δ13C values of CO2 (−5‰ to −3‰) indicate the occurrence of a mantle component released and transferred to the surface by the Cenozoic extension-related magmatic activities. The CO2/3He ratios are in wide range of (0.4–97 × 109). Based on the apparent mixing trend in a 3He/4He and δ13C of CO2 diagram from all published data, the extracted magmatic end-member in the Wudalianchi Volcano has 3He/4He, δ13C and CO2/3He value of ∼3.2 RA, ∼−4.6‰ and ∼6 × 1010, respectively. These values suggest that the volatiles originate from the sub-continental lithospheric mantle (SCLM) in NE China and represent ancient fluids captured by prior metasomatic events, as revealed by geothermal He and CO2 from the adjacent Changbaishan volcanic area.  相似文献   

10.
An experimental study on the origin of ferric and ferrous carbonate-silicate melts, which can be considered as the potential metasomatic oxidizing agents and diamond forming media, was performed in the (Ca,Mg)CO3-SiO2-Al2O3-(Mg,Fe)(Cr,Fe,Ti)O3 system, at 6.3 GPa and 1350–1650 °C. At 1350–1450 °C and ?O2 of FMQ + 2 log units, carbonate–silicate melt, coexisting with Fe3 +-bearing ilmenite, pyrope-almandine and rutile, contained up to 13 wt.% of Fe2O3. An increase in the degree of partial melting was accompanied by decarbonation and melt enrichment with CO2, up to 21 wt.%. At 1550–1650 °C excess CO2 segregated as a separate fluid phase. The restricted solubility of CO2 in the melt indicated that investigated system did not achieve the second critical point at 6.3 GPa. At 1350–1450 °C and ?O2 close to CCO buffer, Fe2 +-bearing carbonate–silicate melt was formed in association with pyrope-almandine and Fe3 +-bearing rutile. It was experimentally shown that CO2-rich ferrous carbonate-silicate melt can be an effective waterless medium for the diamond crystallization. It provides relatively high diamond growth rates (3–5 μm/h) at P,T-conditions, corresponding to the formation of most natural diamonds.  相似文献   

11.
We investigate the helium, carbon and oxygen–hydrogen isotopic systematics and CO2/3He ratios of 8 water and 6 gas samples collected from 12 geothermal fields in western Anatolia (Turkey). 3He/4He ratios of the samples (R) normalized to the atmospheric 3He/4He ratio (RA = 1.39 × 10? 6) range from 0.27 to 1.67 and are significantly higher than the crustal production value of 0.05. Fluids with relatively high R / RA values are generally found in areas of significant heat potential (K?z?ldere and Tuzla fields). CO2/3He ratios of the samples, ranging from 1.6 × 109 to 2.3 × 1014, display significant variation and are mostly higher than values typical of an upper mantle source (2 × 109). The δ13C (CO2) and δ13C (CH4) values of all fluids vary from ? 8.04 to + 0.35‰ and ? 25.80 to ? 23.92‰ (vs. PDB), respectively. Stable isotope values (δ18O–δD) of the geothermal waters are conformable with the Mediterranean Meteoric Water Line and indicate a meteoric origin. The temperatures calculated by gas geothermometry are significantly higher than estimates from chemical geothermometers, implying that either equilibrium has not been attained for the isotope exchange reaction or that isotopic equilibration was disturbed due to gas additions en route to the surface.Evaluation of He–CO2 abundances indicates that hydrothermal degassing and calcite precipitation (controlled probably by adiabatic cooling due to degassing) significantly fractionate the elemental ratio (CO2/3He) in geothermal waters. Such processes do not affect gas phase samples to anywhere near the same extent. For the gas samples, mixing between mantle and various crustal sources appears to be the main control on the observed He–C systematics: however, crustal inputs dominate the CO2 inventory. Considering that limestone is the main source of carbon (～ 70 to 97% of the total carbon inventory), the carbon flux from the crust is found to be at least 20 times that from the mantle. As to the He-inventory, the mantle-derived component is found to vary up to 21% of the total He content and is probably transferred to the crust by fluids degassed from deep mantle melts generated in association with the elevated geotherm and adiabatic melting accompanying current extension. The range of 3He/enthalpy ratios (0.000032 to 0.19 × 10? 12 cm3 STP/J) of fluids in western Anatolia is consistent with the release of both helium and heat from contemporary additions of mantle-derived magmas to the crust. The deep faults appear to have facilitated the deep circulation of the fluids and the transport of mantle volatiles and heat to the surface.  相似文献   

12.
The linkage between the iron and the carbon cycles is of paramount importance to understand and quantify the effect of increased CO2 concentrations in natural waters on the mobility of iron and associated trace elements. In this context, we have quantified the thermodynamic stability of mixed Fe(III) hydroxo-carbonate complexes and their effect on the solubility of Fe(III) oxihydroxides. We present the results of carefully performed solubility measurements of 2-line ferrihydrite in the slightly acidic to neutral–alkaline pH ranges (3.8–8.7) under constant pCO2 varying between (0.982–98.154 kPa) at 25 °C.The outcome of the work indicates the predominance of two Fe(III) hydroxo carbonate complexes FeOHCO3 and Fe(CO3)33−, with formation constants log*β°1,1,1 = 10.76 ± 0.38 and log β°1,0,3 = 24.24 ± 0.42, respectively.The solubility constant for the ferrihydrite used in this study was determined in acid conditions (pH: 1.8–3.2) in the absence of CO2 and at T = (25 ± 1) °C, as log*Ks,0 = 1.19 ± 0.41.The relative stability of the Fe(III)-carbonate complexes in alkaline pH conditions has implications for the solubility of Fe(III) in CO2-rich environments and the subsequent mobilisation of associated trace metals that will be explored in subsequent papers.  相似文献   

13.
Sequestration of carbon dioxide in unmineable coal seams is an option to reduce carbon dioxide emissions. It is well known that the interaction of carbon dioxide with unconfined coal induces swelling. This paper contributes three-dimensional strain distribution in confined coal at microstructural level using high-resolution X-ray computerized tomography data and image analysis. Swelling and compression/compaction of regions in the coal matrix occurs with CO2 uptake. Normal strain varies between ? 1.15% and 0.93%, ? 3.11% and 0.94%, ? 0.43% and 0.30% along x, y and z axes respectively. Volumetric strain varies between ? 4.25% and 1.25%. The positive strains reported are consistent with typical range for unconstrained swelling. However, the average volumetric strains value (? 0.34%) reflect overall volume reduction. Overall swelling is apparently influenced by the confining stresses. The magnitudes of normal strains are heterogeneous and anisotropic. The swelling vs. compression/compaction observed after CO2 uptake is localized and likely lithotype dependant.  相似文献   

14.
Subduction of heterogeneous lithologies (sediments and altered basalts) carries a mixture of volatile components (H2O ± CO2) into the mantle, which are later mobilized during episodes of devolatilization and flux melting. Several petrologic and thermodynamic studies investigated CO2 decarbonation to better understand carbon cycling at convergent margins. A paradox arose when investigations showed little to no decarbonation along present day subduction geotherms at subarc depths despite field based observations. Sediment diapirism is invoked as one of several methods for carbon transfer from the subducting slab. We employ high-resolution 2D petrological–thermomechanical modeling to elucidate the role subduction dynamics has with respect to slab decarbonation and the sediment diapirism hypothesis. Our thermodynamic database is modified to account for H2O–CO2 binary fluids via the following lithologies: GLOSS average sediments (H2O: 7.29 wt.% & CO2: 3.01 wt.%), carbonated altered basalts (H2O: 2.63 wt.% & CO2: 2.90 wt.%), and carbonated peridotites (H2O: 1.98 wt.% & CO2: 1.50 wt.%). We include a CO2 solubility P–x[H2O wt.%] parameterization for sediment melts. We parameterize our model by varying two components: slab age (20, 40, 60, 80 Ma) and convergence velocity (1, 2, 3, 4, 5, 6 cm year− 1). 59 numerical models were run and show excellent agreement with the original code base. Three geodynamic regimes showed significant decarbonation. 1) Sedimentary diapirism acts as an efficient physical mechanism for CO2 removal from the slab as it advects into the hotter mantle wedge. 2) If subduction rates are slow, frictional coupling between the subducting and overriding plate occurs. Mafic crust is mechanically incorporated into a section of the lower crust and undergoes decarbonation. 3) During extension and slab rollback, interaction between hot asthenosphere and sediments at shallow depths result in a small window (~ 12.5 Ma) of high integrated CO2 fluxes (205 kg m− 3 Ma− 1).  相似文献   

15.
Streams and rivers are major exporters of C and other dissolved materials from watersheds to coastal waters. In streams and rivers, substantial amounts of terrigenous organic C is metabolized and degassed as CO2 to the atmosphere. A long-term evaluation of CO2 dynamics in streams is essential for understanding factors controlling CO2 dynamics in streams in response to changes in climate and land-use. Long-term changes in the partial pressure of CO2 (pCO2) were computed in the Anacostia River and the lower Potomac River in the Chesapeake Bay watershed. Long-term estimates were made using routine monitoring data of pH, total alkalinity, and dissolved nutrients from 1985 to 2006 at 14 stations. Longitudinal variability in pCO2 dynamics was also investigated along these rivers downstream of the urban Washington D.C. metropolitan area. Both rivers were supersaturated with CO2 with respect to atmospheric CO2 levels (392 μatm) and the highly urbanized Anacostia waters (202–9694 μatm) were more supersaturated than the Potomac waters (557–3800 μatm). Long-term variability in pCO2 values may be due to changes in river metabolism and organic matter and nutrient loadings. Both rivers exchange significant amounts of CO2 with the atmosphere (i.e., Anacostia at 0.2–72 mmol m−2 d−1 and Potomac at 0.12–24 mmol m−2 d−1), implying that waterways receiving organic matter and nutrient subsidies from urbanized landscapes have the potential to increase river metabolism and atmospheric CO2 fluxes along the freshwater–estuarine continuum.  相似文献   

16.
The Upper Paleozoic section contains a tight gas sandstone reservoir (of 2.75 × 1012 m3) in the Ordos Basin, central China. The measured porosities (< 10%) and permeabilities (generally < 1 mD) are the result of significant mechanical and chemical compaction and precipitation of carbonate, quartz and authigenic clay cements. Fluid inclusion geochemistry and kinetic modeling (generation of gaseous components and δ13C1) were integrated to constrain the timing of gas charge into the tight reservoir. The modeling results indicate that the natural gases in the present reservoir are similar to gases liberated from quartz inclusions in both composition and stable carbon isotope values and also similar to gas generated from Upper Paleozoic coal. The similar geochemistry suggests that an important phase of quartz cementation must have occurred after gas emplacement in the reservoirs during regional uplift at the end of the Cretaceous. The latest carbonate cement, postdating quartz cementation, consumed most of the late CO2 generated from coal at high maturity (RO > 1.7%) and reduced the reservoir quality dramatically. On the contrary, tight sandstones from non-producing areas have fluid inclusions that were trapped in quartz cements much earlier. These data indicate that natural gas migrated into the Upper Paleozoic reservoir when it still retained high porosity and permeability. The reservoir continued to experience porosity and permeability reduction from continued quartz and carbonate cementation after gas charging due to low gas saturation. Comparison of the relative timing of gas charging with that of sandstone cementation can help to predict areas of risk during tight gas exploration and development.  相似文献   

17.
Laboratory experiments were conducted to investigate the adsorption kinetic behavior of pure and mixed gases (CO2, CH4, approximately equimolar CO2 + CH4 mixtures, and He) on a coal sample obtained from the Black Warrior Basin at the Littleton Mine (Twin Pine Coal Company), Jefferson County, west-central Alabama. The sample was from the Mary Lee coal zone of the Pottsville Formation (Lower Pennsylvanian). Experiments with three size fractions (45–150 µm, 1–2 mm, and 5–10 mm) of crushed coal were performed at 40 °C and 35 °C over a pressure range of 1.4–6.9 MPa to simulate coalbed methane reservoir conditions in the Black Warrior Basin and provide data relevant for enhanced coalbed methane recovery operations. The following key observations were made: (1) CO2 adsorption on both dry and water-saturated coal is much more rapid than CH4 adsorption; (2) water saturation decreases the rates of CO2 and CH4 adsorption on coal surfaces, but it appears to have minimal effects on the final magnitude of CO2 or CH4 adsorption if the coal is not previously exposed to CO2; (3) retention of adsorbed CO2 on coal surfaces is significant even with extreme pressure cycling; and (4) adsorption is significantly faster for the 45–150 μm size fraction compared to the two coarser fractions.  相似文献   

18.
Pristine diorite drill cores, obtained from the Äspö Hard Rock Laboratory (HRL, Sweden), were used to study the retention properties of fresh, anoxic crystalline rock material towards the redox-sensitive uranium. Batch sorption experiments and spectroscopic methods were applied for this study. The impact of various parameters, such as solid-to-liquid ratio (2–200 g/L), grain size (0.063–0.2 mm, 0.5–1 mm, 1–2 mm), temperature (room temperature and 10 °C), contact time (5–108 days), initial U(VI) concentration (3 × 10−9 to 6 × 10−5 M), and background electrolyte (synthetic Äspö groundwater and 0.1 M NaClO4) on the U(VI) sorption onto anoxic diorite was studied under anoxic conditions (N2). Comparatively, U(VI) sorption onto oxidized diorite material was studied under ambient atmosphere (pCO2 = 10−3.5 atm). Conventional distribution coefficients, Kd, and surface area normalized distribution coefficients, Ka, were determined. The Kd value for the U(VI) sorption onto anoxic diorite in synthetic Äspö groundwater under anoxic conditions by investigating the sorption isotherm amounts to 3.8 ± 0.6 L/kg which corresponds to Ka = 0.0030 ± 0.0005 cm (grain size 1–2 mm). This indicates a weak U sorption onto diorite which can be attributed to the occurrence of the neutral complex Ca2UO2(CO3)3(aq) in solution. This complex was verified as predominating U species in synthetic Äspö groundwater by time-resolved laser-induced fluorescence spectroscopy (TRLFS). Compared to U sorption at room temperature under anoxic conditions, U sorption is further reduced at decreased temperature (10 °C) and under ambient atmosphere. The U species in aqueous solution as well as sorbed on diorite were studied by in situ time-resolved attenuated total reflection Fourier-transform infrared (ATR FT-IR) spectroscopy. A predominant sorbing species containing a UO2(CO3)34− moiety was identified. The extent of U sorption onto diorite was found to depend more on the low sorption affinity of the Ca2UO2(CO3)3(aq) complex than on reduction processes of uranium.  相似文献   

19.
The Wangfeng gold deposit is located in Western Tian Shan and the central section of the Central Asian Orogenic Belt (CAOB). The deposit is mainly hosted in Precambrian metamorphic rocks and Caledonian granites and is structurally controlled by the Shenglidaban ductile shear zone. The gold orebodies consist of gold-bearing quartz veins and altered mylonite. The mineralization can be divided into three stages: quartz–pyrite veins in the early stage, sulfide–quartz veins in the middle stage, and quartz–carbonate veins or veinlets in the late stage. Ore minerals and native gold mainly formed in the middle stage. Four types of fluid inclusions were identified based on petrography and laser Raman spectroscopy: CO2–H2O inclusions (C-type), pure CO2 inclusions (PC-type), NaCl–H2O inclusions (W-type), and daughter mineral-bearing inclusions (S-type). The early-stage quartz contains only primary CO2–H2O fluid inclusions with salinities of 1.62 to 8.03 wt.% NaCl equivalent, bulk densities of 0.73 to 0.89 g/cm3, and homogenization temperatures of 256 °C–390 °C. Vapor bubbles are composed of CO2. The middle-stage quartz contains all four types of fluid inclusions, of which the CO2–H2O and NaCl–H2O types yield homogenization temperatures of 210 °C–340 °C and 230 °C–300 °C, respectively. The CO2–H2O fluid inclusions have salinities of 0.83 to 9.59 wt.% NaCl equivalent and bulk densities of 0.77 to 0.95 g/cm3, with vapor bubbles composed of CO2, CH4, and N2. Fluid inclusions in the late-stage quartz are NaCl–H2O solution with low salinities (0.35–3.87 wt.% NaCl equivalent) and low homogenization temperatures (122 °C–214 °C). The coexistence of inclusions of these four types in middle-stage quartz suggests that fluid boiling occurred in the middle-stage mineralization. Trapping pressures estimated from CO2–H2O inclusions are 110–300 MPa and 90–250 MPa for the early and middle stages, respectively, suggesting that gold mineralization mainly occurred at depths of about 10 km. In general, the Wangfeng gold deposit originated from a metamorphic fluid system characterized by low salinity, low density, and enrichment of CO2. Depressurized fluid boiling caused gold precipitation. Given the regional geology, ore geology, fluid-inclusion features, and ore-forming age, the Wangfeng gold deposit can be classified as a hypozonal orogenic gold deposit.  相似文献   

20.
Soils act as sources and sinks for greenhouse gases (GHG) such as carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O). Since both storage and emission capacities may be large, precise quantifications are needed to obtain reliable global budgets that are necessary for land-use management (agriculture, forestry), global change and for climate research. This paper discusses exclusively the soil emission-related processes and their influencing parameters. It reviews soil emission studies involving the most important land-cover types and climate zones and introduces important measuring systems for soil emissions. It addresses current shortcomings and the obvious bias towards northern hemispheric data.When using a conservative average of 300 mg CO2e m−2 h−1 (based on our literature review), this leads to global annual net soil emissions of ≥350 Pg CO2e (CO2e = CO2 equivalents = total effect of all GHG normalized to CO2). This corresponds to roughly 21% of the global soil C and N pools. For comparison, 33.4 Pg CO2 are being emitted annually by fossil fuel combustion and the cement industry.  相似文献   

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