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1.
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   

2.
Gas adsorption isotherms of Akabira coals were established for pure carbon dioxide (CO2), methane (CH4), and nitrogen (N2). Experimental data fit well into the Langmuir model. The ratio of sorption capacity of CO2, CH4, and N2 is 8.5:3.5:1 at a lower pressure (1.2 MPa) regime and becomes 5.5:2:1 when gas pressure increases to 6.0 MPa. The difference in sorption capacity of these three gases is explained by differences in the density of the three gases with increasing pressure. A coal–methane system partially saturated with CH4 at 2.4 MPa adsorption pressure was experimentally studied. Desorption behavior of CH4 by injecting pure CO2 (at 3.0, 4.0, 5.0, and 6.0 MPa), and by injecting the CO2–N2 mixture and pure N2 (at 3.0 and 6.0 MPa) were evaluated. Results indicate that the preferential sorption property of coal for CO2 is significantly higher than that for CH4 or N2. CO2 injection can displace almost all of the CH4 adsorbed on coal. When modeling the CH4–CO2 binary and CH2–CO2–N2 ternary adsorption system by using the extended Langmuir (EL) equation, the EL model always over-predicted the sorbed CO2 value with a lower error, while under-predicting the sorbed CH4 with a higher error. A part of CO2 may dissolve into the solid organic structure of coal, besides its competitive adsorption with other gases. According to this explanation, the EL coefficients of CO2 in EL equation were revised. The revised EL model proved to be very accurate in predicting sorbed ratio of multi-component gases on coals.  相似文献   

3.
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   

4.
Fluxes of methane (CH4) and carbon dioxide (CO2) to the atmosphere at 52 sites within a salt marsh were measured by a dark static chamber technique from mid July to mid September. Mean CH4 fluxes ranged from 0.2 mg m?2 d?1 to 11.0 mg m?2 d?1, with an overall average of 1.6 mg m?2 d?1. Flux of CH4 was inversely correlated (r2=0.23, p = 0.001) with salinity of the upper porewater at the site, suggesting the dominant role of SO4 2? in inhibiting methanogenesis in salt-marsh sediments. The combination of salinity and water table position was able to explain only 29% of the variance in CH4 emission. Mean soil flux of CO2 ranged from 0.3 g m?2 d?1 to 3.7 g m?2 d?1, with an overall average of 2.5 g m?2 d?1; it was correlated with aboveground biomass (positive, r2=0.38, p = 0.001) and position of the water table (negative, r2 = 0.55, p = 0.001). The combination of biomass and water table position accounted for 63% of the variance in CO2 flux. There were high variations in gas flux within the six plant communities. The sequences were CH4: upland edge > panne > pool > middle marsh > low marsh > high marsh, and CO2: middle marsh > low marsh > upland edge > high marsh > panne > pool. Compared to other salt-marsh systems, this Bay of Fundy marsh emits small amounts of CH4 and CO2.  相似文献   

5.
Natural gas reservoirs in organic-rich shales in the Appalachian and Michigan basins in the United States are currently being produced via hydraulic fracturing. Stratigraphically-equivalent shales occur in the Canadian portion of the basins in southwestern Ontario with anecdotal evidence of gas shows, yet there has been no commercial shale gas production to date. To provide baseline data in the case of future environmental issues related to hydraulic fracturing and shale gas production, such as leakage of natural gas, saline water, and/or hydraulic fracturing fluids, and to evaluate hydrogeochemical controls on natural gas accumulations in shallow groundwater in general, this study investigates the origin and distribution of natural gas and brine in shallow aquifers across southwestern Ontario. An extensive geochemical database of major ion and trace metal chemistry and methane concentrations of 1010 groundwater samples from shallow, domestic wells in bedrock and overburden aquifers throughout southwestern Ontario was utilized. In addition, select wells (n = 36) were resampled for detailed dissolved gas composition, δ13C of CH4, C2, C3, and CO2, and δD of CH4. Dissolved gases in groundwater from bedrock and overburden wells were composed primarily of CH4 (29.7–98.6 mol% of total gas volume), N2 (0.8–66.2 mol%), Ar + O2 (0.2–3.4 mol%), and CO2 (0–1.2 mol%). Ethane was detected, but only in low concentrations (<0.041 mol%), and no other higher chain hydrocarbons were present, except for one well in overburden overlying the Dundee Formation, which contained 0.81 mol% ethane and 0.21 mol% propane. The highest methane concentrations (30 to >100 in situ % saturation) were found in bedrock wells completed in the Upper Devonian Kettle Point Formation, Middle Devonian Hamilton Group and Dundee Formation, and in surficial aquifers overlying these organic-rich shale-bearing formations, indicating that bedrock geology is the primary control on methane occurrences. A few (n = 40) samples showed Na–Cl–Br evidence of brine mixing with dilute groundwater, however only one of these samples contained high (>60 in situ % saturation) CH4. The relatively low δ13C values of CH4 (−89.9‰ to −57.3‰), covariance of δD values of CH4 and H2O, positive correlation between δ13C values of CH4 and CO2, and lack of higher chain hydrocarbons (C3+) in all but one dissolved gas sample indicates that the methane in groundwater throughout the study area is primarily microbial in origin. The presence or absence of alternative electron acceptors (e.g. dissolved oxygen, Fe, NO3, SO4), in addition to organic substrates, controls the occurrence of microbial CH4 in shallow aquifers. Microbial methane has likely been accumulating in the study area, since at least the Late Pleistocene to the present, as indicated by the co-variance and range of δD values of CH4 (−314‰ to −263‰) and associated groundwater (−19‰ to −6‰ δD-H2O).  相似文献   

6.
A mathematical model was developed to predict the coal bed methane (CBM) production and carbon dioxide (CO2) sequestration in a coal seam accounting for the coal seam properties. The model predictions showed that, for a CBM production and dewatering process, the pressure could be reduced from 15.17 MPa to 1.56 MPa and the gas saturation increased up to 50% in 30 years for a 5.4 × 105 m2 of coal formation. For the CO2 sequestration process, the model prediction showed that the CO2 injection rate was first reduced and then slightly recovered over 3 to 13 years of injection, which was also evidenced by the actual in seam data. The model predictions indicated that the sweeping of the water in front of the CO2 flood in the cleat porosity could be important on the loss of injectivity. Further model predictions suggested that the injection rate of CO2 could be about 11 × 103 m3 per day; the injected CO2 would reach the production well, which was separated from the injection well by 826 m, in about 30 years. During this period, about 160 × 106 m3 of CO2 could be stored within a 21.4 × 105 m2 of coal seam with a thickness of 3 m.  相似文献   

7.
Permian Khuff reservoirs along the east coast of Saudi Arabia and in the Arabian Gulf produce dry sour gas with highly variable nitrogen concentrations. Rough correlations between N2/CH4, CO2/CH4 and H2S/CH4 suggest that non-hydrocarbon gas abundances are controlled by thermochemical sulfate reduction (TSR). In Khuff gases judged to be unaltered by TSR, methane δ13C generally falls between −40‰ and −35‰ VPDB and carbon dioxide δ13C between −3‰ and 0‰ VPDB. As H2S/CH4 increases, methane δ13C increases to as much as −3‰ and carbon dioxide δ13C decreases to as little as −28‰. These changes are interpreted to reflect the oxidation of methane to carbon dioxide.Khuff reservoir temperatures, which locally exceed 150 °C, appear high enough to drive the reduction of sulfate by methane. Anhydrite is abundant in the Khuff and fine grained nodules are commonly rimmed with secondary calcite cement. Some cores contain abundant pyrite, sphalerite and galena. Assuming that nitrogen is inert, loss of methane by TSR should increase N2/CH4 of the residual gas and leave δ15N unaltered. δ15N of Paleozoic gases in Saudi Arabia varies from −7‰ to 1‰ vs. air and supports the TSR hypothesis. N2/CH4 in gases from stacked Khuff reservoirs varies by a factor of 19 yet the variation in δ15N (0.3–0.5‰) is trivial.Because the relative abundance of hydrogen sulfide is not a fully reliable extent of reaction parameter, we have attempted to assess the extent of TSR using plots of methane δ13C versus log(N2/CH4). Observed variations in these parameters can be fitted using simple Rayleigh models with kinetic carbon isotope fractionation factors between 0.98 and 0.99. We calculate that TSR may have destroyed more than 90% of the original methane charge in the most extreme instance. The possibility that methane may be completely destroyed by TSR has important implications for deep gas exploration and the origin of gases rich in nitrogen as well as hydrogen sulfide.  相似文献   

8.
In order to better understand the spatiotemporal variations and interrelationships of greenhouse gases (GHG), monthly surface fluxes and profile concentrations of GHG (CO2, N2O and CH4) in karst areas in the Guizhou Province, southwest China, were measured from June 2006 to May 2007. GHG fluxes showed high variability, with a range of 460.9?C1,281.2?mg?m?2?h?1 for CO2, ?25.4 to 81.5???g?m?2?h?1 for N2O and ?28.7 to ?274.9???g?m?2?h?1 for CH4, but no obvious seasonal change trends of the fluxes existed. Profile concentrations of CO2, N2O and CH4 varied between 0.5 and 31.5?mL?L?1, 0.273 and 0.734, and 0.1 and 3.5???L?L?1, respectively. In general, concentrations of CO2 and N2O increased with depth, while CH4 had an inverse trend. However, in October, November and January, the reversal of depth patterns of GHG concentrations took place below 15?cm, close to the soil?Crock interface. The spatiotemporal distribution of CO2 in soil profile was significantly positively correlated with that of N2O (p?<?0.05?C0.01) and negatively correlated with that of CH4 (p?<?0.01). The correlation analysis showed that soil temperature and moisture may be responsible for GHG dynamics in the soils, rather than the exchange of GHG between land and atmosphere.  相似文献   

9.
The Late Miocene Muaraenim Formation in southern Sumatra contains thick coal sequences, mostly of low rank ranging from lignite to sub-bituminous, and it is believed that these thick low rank coals are the most prospective for the production of coal seam gas (CSG), otherwise known as coalbed methane (CBM), in Indonesia.As part of a major CSG exploration project, gas exploration drilling operations are being undertaken in Rambutan Gasfields in the Muaraenim Formation to characterize the CSG potential of the coals. The first stage of the project, which is described here, was designed to examine the gas reservoir properties with a focus on coal gas storage capacity and compositional properties. Some five CSG exploration boreholes were drilled in the Rambutan Gasfield, south of Palembang. The exploration boreholes were drilled to depths of ~ 1000 m into the Muaraenim Formation. Five major coal seams were intersected by these holes between the depths of 450 and 1000 m. The petrography of coal samples collected from these seams showed that they are vitrinite rich, with vitrinite contents of more than 75% (on a mineral and moisture free basis). Gas contents of up to 5.8 m3/t were measured for the coal samples. The gas desorbed from coal samples contain mainly methane (CH4) ranging from 80 to 93% and carbon dioxide (CO2) ranging from 6 to 19%. The composition of the gas released into the production borehole/well is, however, much richer in CH4 with about 94 to 98% CH4 and less than 5% CO2.The initial results of drilling and reservoir characterization studies indicate suitable gas recovery parameters for three of the five coal seams with a total thickness of more than 30 m.  相似文献   

10.
Peatlands are a large potential source of methane (CH4) to the atmosphere. In order to investigate the effects of climate change on CH4 emission from northern ombrotrophic peatlands, a simulation model coupling water table dynamics with methane emission was developed for the Mer Bleue Bog in Ontario, Canada. The model was validated against reported values of CH4 flux from field measurements and the model outputs exhibited high sensitivity to acrotelm thickness, leaf area index, transmissivity and slope of water table. With a 2–4°C temperature rise over the 4-year simulation period, the rate of CH4 release dropped significantly to under 0.1 mg m−2 day−1. On the other hand, mean CH4 emission increased by >26-fold when the increase in precipitation was >15%. When looking at the combined effects, the highest CH4 release (13.3 mg m−2 day−1) was attained under the scenario of 2°C temperature rise and 25% precipitation increase. Results obtained in this study highlight the importance of avoiding more extreme climate change, which would otherwise lead to enhanced methane release from peatlands and further atmospheric warming through positive feedback.  相似文献   

11.
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   

12.
Freshwater marshes could be a source of greenhouse gases emission because they contain large amounts of soil carbon and nitrogen. These emissions are strongly influenced by exogenous nitrogen. We investigate the effects of exogenous nitrogen on ecosystem respiration (CO2), CH4 and N2O emissions from freshwater marshes in situ in the Sanjiang Plain Northeast of China during the growing seasons of 2004 and 2005, using a field fertilizer experiment and the static opaque chamber/GC techniques. The results show that there were no significant differences in patterns of seasonal variations of CO2 and CH4 among the fertilizer and non-fertilizer treatments, but the seasonal patterns of N2O emission were significantly influenced by the exogenous nitrogen. Seasonal averages of the CO2 flux from non-fertilizer and fertilizer were 987.74 and 1,344.35 mg m −2 h −1, respectively, in 2004, and 898.59 and 2,154.17 mg m −2 h −1, respectively, in 2005. And the CH4 from the control and fertilizer treatments were 6.05 and 13.56 mg m −2 h −1 and 0.72 and 1.88 mg m −2 h −1, respectively, in 2004 and 2005. The difference of N2O flux between the fertilizer and non-fertilizer treatments is also significant either in 2004 and 2005. On the time scale of 20-, 100-, and 500-year periods, the integrated global warming potential (GWP) of CO2 + CH4 + N2O released during the two growing seasons for the treatment of fertilizer was 97, 94 and 89%, respectively, higher than that for the control, which suggested that the nitrogen fertilizer can enhance the GWP of the CH4 and N2O either in long time or short time scale.  相似文献   

13.
Characterization of coal reservoirs and determination of in-situ physical coal properties related to transport mechanism are complicated due to having lack of standard procedures in the literature. By considering these difficulties, a new approach has been developed proposing the usage of relationships between coal rank and physical coal properties. In this study, effects of shrinkage and swelling (SS) on total methane recovery at CO2 breakthrough (TMRB), which includes ten-year primary methane recovery and succeeding enhanced coalbed methane (ECBM) recovery up to CO2 breakthrough, and CO2 sequestration have been investigated by using rank-dependent coal properties. In addition to coal rank, different coal reservoir types, molar compositions of injected fluid, and parameters within the extended Palmer & Mansoori (P&M) permeability model were considered. As a result of this study, shrinkage and swelling lead to an increase in TMRB. Moreover, swelling increased CO2 breakthrough time and decreased displacement ratio and CO2 storage for all ranks of coal. Low-rank coals are affected more negatively than high-rank coals by swelling. Furthermore, it was realized that dry coal reservoirs are more influenced by swelling than others and saturated wet coals are more suitable for eliminating the negative effects of CO2 injection. In addition, it was understood that it is possible to reduce swelling effect of CO2 on cleat permeability by mixing it with N2 before injection. However, an economical optimization is required for the selection of proper gas mixture. Finally, it is concluded from sensitivity analysis that elastic modulus is the most important parameter, except the initial cleat porosity, controlling SS in the extended P&M model by highly affecting TMRB.  相似文献   

14.
New isotopic and chemical data on the sodium bicarbonate water and associated gases from the Razdolnoe Spa located in the coastal zone of Primorsky Kray of the Russian Far East, together with previous stable isotope data (δ18O, δD, δ13C), allow elucidation of the origin and evolution of the groundwater and gases from the spa. The water is characterized by low temperature (12 °C), TDS – 2.5–6.0 g/L, high contents of B (∼5 mg/L) and F (4.5 mg/L) and low contents of Cl and SO4. Water isotopic composition indicates its essentially meteoric origin which may comply with an older groundwater that was recharged under different (colder) climatic conditions. Major components of bubbling gases are CH4 (68 vol%), N2 (28%) and CO2 (4%). The obtained values δ13C and δD for CO2 and CH4 definitely indicate the marine microbial origin of methane. Thus the high methane content in the waters relates to the biochemical processes and presence of a dispersed organic matter in the host rocks. Based on the regional hydrogeology and the geological structure of the Razdolnoe Spa, Mesozoic fractured rocks containing Na–HCO3 mineral water and gases are reservoir rocks, a chemical composition of water and gases originates in different environmental conditions.  相似文献   

15.
CO2 pilot injection studies, with site-specific geologic assessment and engineering reservoir design, can be instrumental for demonstrating both incremental enhanced oil recovery and permanent geologic storage of greenhouse gases. The purpose of this paper is to present the geologic and reservoir analyses in support of a field pilot test that will evaluate the technical and economic feasibility of commercial-scale CO2-enhanced oil recovery to increase oil recovery and extend the productive life of the Citronelle Oil Field, the largest conventional oil field in Alabama (SE USA). Screening of reservoir depth, oil gravity, reservoir pressure, reservoir temperature, and oil composition indicates that the Cretaceous-age Donovan sand, which has produced more than 169 × 106 bbl in Citronelle Oil Field, is amenable to miscible CO2 flooding. The project team has selected an 81 ha (200 ac) 5-spot test site with one central gas injector, two producers, and two initially temporarily abandoned production wells that are now in production. Injection is planned in two separate phases, each consisting of 6,804 t (7,500 short tons) of food-grade CO2. The Citronelle Unit B-19-10 #2 well (Permit No. 3232) is the CO2 injector for the first injection test. The 14-1 and 16-2 sands of the upper Donovan are the target zones. These sandstone units consist of fine to medium-grained sandstone that is enveloped by variegated mudstone. Both of these sandstone units were selected based on the distribution of perforated zones in the test pattern, production history, and the ability to correlate individual sandstone units in geophysical well logs. The pilot injections will evaluate the applicability of tertiary oil recovery to Citronelle Field and will provide a large volume of information on the pressure response of the reservoirs, the mobility of fluids, time to breakthrough, and CO2 sweep efficiency. The results of the pilot injections will aid in the formulation of commercial-scale reservoir management strategies that can be applied to Citronelle Field and other geologically heterogeneous oil fields and the design of similar pilot injection projects.  相似文献   

16.
The in situ redox potential (Eh) in anoxic groundwater with high methane and iron contents (approximately 12.3 and 28.4 mg/L, respectively) was potentiometrically measured to identify the processes that control Eh. The measured Eh ranged from −213 to −187 mV; it had an inverse correlation with the concentration of methane and no correlation with that of iron. The saturation indices indicate that goethite and amorphous FeS were nearly at solubility equilibrium. A comparison of the measured Eh with those calculated for the particular redox pairs indicates that either Fe2+/FeOOH or CH4/CO2, but not sulfur redox pairs, controlled the measured Eh. The inverse relationship between measured Eh and methane concentration suggests possible control of the redox conditions by the CH4/CO2 redox pair. Furthermore, the equilibrium solubility state of goethite, which has higher crystallinity and lower solubility than Fe(OH)3 indicates that the iron reaction was electrochemically irreversible. This further supports the contribution of the CH4/CO2 pair to controlling the measured Eh of groundwater.  相似文献   

17.
A unique dataset from paired low- and high-temperature vents at 9°50′N East Pacific Rise provides insight into the microbiological activity in low-temperature diffuse fluids. The stable carbon isotopic composition of CH4 and CO2 in 9°50′N hydrothermal fluids indicates microbial methane production, perhaps coupled with microbial methane consumption. Diffuse fluids are depleted in 13C by ∼10‰ in values of δ13C of CH4, and by ∼0.55‰ in values of δ13C of CO2, relative to the values of the high-temperature source fluid (δ13C of CH4 =−20.1 ± 1.2‰, δ13C of CO2 =−4.08 ± 0.15‰). Mixing of seawater or thermogenic sources cannot account for the depletions in 13C of both CH4 and CO2 at diffuse vents relative to adjacent high-temperature vents. The substrate utilization and 13C fractionation associated with the microbiological processes of methanogenesis and methane oxidation can explain observed steady-state CH4 and CO2 concentrations and carbon isotopic compositions. A mass-isotope numerical box model of these paired vent systems is consistent with the hypothesis that microbial methane cycling is active at diffuse vents at 9°50′N. The detectable 13C modification of fluid geochemistry by microbial metabolisms may provide a useful tool for detecting active methanogenesis.  相似文献   

18.
This study investigates the occurrence of greenhouse gases (GHGs) and the role of groundwater as an indirect pathway of GHG emissions into surface waters in a gaining stretch of the Triffoy River agricultural catchment (Belgium). To this end, nitrous oxide (N2O), methane (CH4) and carbon dioxide (CO2) concentrations, the stable isotopes of nitrate, and major ions were monitored in river and groundwater over 8 months. Results indicated that groundwater was strongly oversaturated in N2O and CO2 with respect to atmospheric equilibrium (50.1 vs. 0.55 μg L?1 for N2O and 14,569 vs. 400 ppm for CO2), but only marginally for CH4 (0.45 vs. 0.056 μg L?1), suggesting that groundwater can be a source of these GHGs to the atmosphere. Nitrification seemed to be the main process for the accumulation of N2O in groundwater. Oxic conditions prevailing in the aquifer were not prone for the accumulation of CH4. In fact, the emissions of CH4 from the river were one to two orders of magnitude higher than the inputs from groundwater, meaning that CH4 emissions from the river were due to CH4 in-situ production in riverbed or riparian zone sediments. For CO2 and N2O, average emissions from groundwater were 1.5?×?105 kg CO2 ha?1 year?1 and 207 kg N2O ha?1 year?1, respectively. Groundwater is probably an important source of N2O and CO2 in gaining streams but when the measures are scaled at catchment scale, these fluxes are probably relatively modest. Nevertheless, their quantification would better constrain nitrogen and carbon budgets in natural systems.  相似文献   

19.
A detailed model is presented of methane photochemistry in the primitive terrestrial atmosphere along with speculation about its interpretation. Steady-state CH4 mixing ratios of 10−6–10−4 could have been maintained by a methane source of about 1011 cm−2 s−1, which is comparable to the modern biogenic methane production rate. In the absence of a source, methane would have disappeared in <104 years, being either oxidized, or polymerized into more complex hydrocarbons. The source strength needed to maintain a steady CH4 mixing ratio and the degree to which methane could have polymerized to form higher hydrocarbons depend upon the amount of CO2 present in the early atmosphere. The dependence on H2 is much weaker. Infrared absorption by methane, and especially by other hydrocarbon species, may have supplemented the greenhouse warming due to carbon dioxide. A radiative model is needed to establish this effect quantitatively. The destruction of the methane greenhouse early in the Proterozoic may have triggered the Huronian glaciation.These calculations also suggest that atmospheres rich in both CO2 and CH4 may be photochemically unstable with respect to conversion to CO.  相似文献   

20.
This paper contributes to the understanding of the genesis of epigenetic, hypogene BIF-hosted iron deposits situated in the eastern part of Ukrainian Shield. It presents new data from the Krivoy Rog iron mining district (Skelevatske–Magnetitove deposit, Frunze underground mine and Balka Severnaya Krasnaya outcrop) and focuses on the investigation of ore genesis through application of fluid inclusion petrography, microthermometry, Raman spectroscopy and baro-acoustic decrepitation of fluid inclusions. The study investigates inclusions preserved in quartz and magnetite associated with the low-grade iron ores (31–37% Fe) and iron-rich quartzites (38–45% Fe) of the Saksaganskaya Suite, as well as magnetite from the locally named high-grade iron ores (52–56% Fe). These high-grade ores resulted from alteration of iron quartzites in the Saksaganskiy thrust footwall (Saksaganskiy tectonic block) and were a precursor to supergene martite, high-grade ores (60–70% Fe). Based on the new data two stages of iron ore formation (metamorphic and metasomatic) are proposed.The metamorphic stage, resulting in formation of quartz veins within the low-grade iron ore and iron-rich quartzites, involved fluids of four different compositions: CO2-rich, H2O, H2O–CO2(± N2–CH4)–NaCl(± NaHCO3) and H2O–CO2(± N2–CH4)–NaCl. The salinities of these fluids were relatively low (up to 7 mass% NaCl equiv.) as these fluids were derived from dehydration and decarbonation of the BIF rocks, however the origin of the nahcolite (NaHCO3) remains unresolved. The minimum P–T conditions for the formation of these veins, inferred from microthermometry are Tmin = 219–246 °C and Pmin = 130–158 MPa. The baro-acoustic decrepitation analyses of magnetite bands indicated that the low-grade iron ore from the Skelevatske–Magnetitove deposit was metamorphosed at T = ~ 530 °C.The metasomatic stage post-dated and partially overlapped the metamorphic stage and led to the upgrade of iron quartzites to the high-grade iron ores. The genesis of these ores, which are located in the Saksaganskiy tectonic block (Saksaganskiy ore field), and the factors controlling iron ore-forming processes are highly controversial. According to the study of quartz-hosted fluid inclusions from the thrust zone the metasomatic stage involved at least three different episodes of the fluid flow, simultaneous with thrusting and deformation. During the 1st episode three types of fluids were introduced: CO2–CH4–N2(± C), CO2(± N2–CH4) and low salinity H2O–N2–CH4–NaCl (6.38–7.1 mass% NaCl equiv.). The 2nd episode included expulsion of the aqueous fluids H2O–N2–CH4–NaCl(± CO2, ± C) of moderate salinities (15.22–16.76 mass% NaCl equiv.), whereas the 3rd event involved high salinity fluids H2O–NaCl(± C) (20–35 mass% NaCl equiv.). The fluids most probably interacted with country rocks (e.g. schists) supplying them with CH4 and N2. The high salinity fluids were most likely either magmatic–hydrothermal fluids derived from the Saksaganskiy igneous body or heated basinal brines, and they may have caused pervasive leaching of Fe from metavolcanic and/or the BIF rocks. The baro-acoustic decrepitation analyses of magnetite comprising the high-grade iron ore showed formation T = ~ 430–500 °C. The fluid inclusion data suggest that the upgrade to high-grade Fe ores might be a result of the Krivoy Rog BIF alteration by multiple flows of structurally controlled, metamorphic and magmatic–hydrothermal fluids or heated basinal brines.  相似文献   

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