Supercritical gas sorption on moist coals   总被引：2，自引：1，他引：1  

Stuart Day  Richard Sakurovs  Steve Weir 《International Journal of Coal Geology》2008,74(3-4):203-214

The effect of moisture on the CO₂ and CH₄ sorption capacity of three bituminous coals from Australia and China was investigated at 55 °C and at pressures up to 20 MPa. A gravimetric apparatus was used to measure the gas adsorption isotherms of coal with moisture contents ranging from 0 to about 8%. A modified Dubinin–Radushkevich (DR) adsorption model was found to fit the experimental data under all conditions. Moisture adsorption isotherms of these coals were measured at 21 °C. The Guggenheim–Anderson–de Boer (GAB) model was capable of accurately representing the moisture isotherms over the full range of relative pressures.Moist coal had a significantly lower maximum sorption capacity for both CO₂ and CH₄ than dry coal. However, the extent to which the capacity was reduced was dependent upon the rank of the coal. Higher rank coals were less affected by the presence of moisture than low rank coals. All coals exhibited a certain moisture content beyond which further moisture did not affect the sorption capacity. This limiting moisture content was dependent on the rank of the coal and the sorbate gas and, for these coals, corresponded approximately to the equilibrium moisture content that would be attained by exposing the coal to about 40–80% relative humidity. The experimental results indicate that the loss of sorption capacity by the coal in the presence of water can be simply explained by volumetric displacement of the CO₂ and CH₄ by the water. Below the limiting moisture content, the CO₂ sorption capacity reduced by about 7.3 kg t^− 1 for each 1% increase in moisture. For CH₄, sorption capacity was reduced by about 1.8 kg t^− 1 for each 1% increase in moisture.The heat of sorption calculated from the DR model decreased slightly on addition of moisture. One explanation is that water is preferentially attracted to high energy adsorption sites (that have high energy by virtue of their electrostatic nature), expelling CO₂ and CH₄ molecules.  相似文献   

A novel time-series station in the Wadden Sea (NW Germany): First results on continuous nutrient and methane measurements     

Maik Grunwald  Olaf Dellwig  Gerd Liebezeit  Bernhard Schnetger  Rainer Reuter  Hans-Jürgen Brumsack 《Marine Chemistry》2007

In autumn 2002 a time-series station was installed in the tidal inlet between the Islands of Langeoog and Spiekeroog (Southern North Sea, NW Germany) to continuously measure physical, chemical, and meteorological parameters, even during extreme weather conditions (gale-force storms, drifting ice). Inside the pole of the station sensor tubes are installed in direction of the prevailing tidal currents. The tubes are equipped with hydrographic sensors (pressure, temperature, conductivity) and allow retrieval of water for nutrient analysis by automated instruments located inside the pole. Dissolved methane and the nutrients ammonia, nitrite, nitrate, phosphate, and silicate are measured at the station.  相似文献   

IODP 311航次底栖有孔虫碳稳定同位素对天然气水合物地质系统的指示     

李清  王家生  王晓芹  陈祈  陈洪仁 《地球科学进展》2008,23(11):1161-1166

为了探索海洋天然气水合物背景下有孔虫特征的响应,对综合大洋钻探计划(IODP) 311航次岩芯沉积物中底栖有孔虫Uvigerina peregrina和Bulimina mexicana进行了初步研究。通过对冷泉站位U1328和毗邻的非冷泉站位U1327沉积物中底栖有孔虫Uvigerina peregrina和Bulimina mexicana的显微形貌特征和碳、氧稳定同位素测试等,证实有孔虫壳体未受到后期成岩作用的改造和自生碳酸盐岩的交代影响,有孔虫壳体的碳稳定同位素呈现明显的负偏。其中U1327站位中U.peregrina δ¹³C为-0.67‰～-2.75‰（PDB）,B.mexicana δ¹³C为-0.51‰～-1.52‰（PDB）;U1328站位中U.peregrina δ¹³C为 -0.72‰～-2.71‰（PDB）,B.mexicanaδ¹³C为 -0.58‰～-1.45‰（PDB）。底栖有孔虫壳体的碳稳定同位素负偏成因可能与水合物不稳定分解释放的甲烷厌氧氧化作用和食物源有关,因而可较好地指示海底天然气水合物系统地质背景。  相似文献   

The hydrogeochemistry of methane: Evidence from English groundwaters   总被引：2，自引：0，他引：2  

W.G. Darling  D.C. Gooddy 《Chemical Geology》2006,229(4):293-312

The presence of methane (CH₄) in groundwater is usually only noticed when it rises to high concentrations; to date rather little is known about its production or natural ‘baseline’ conditions. Evidence from a range of non-polluted groundwater environments in England, including water supply aquifers, aquicludes and thermal waters, reveals that CH₄ is almost always detectable, even in aerobic conditions. Measurements of potable waters from Cretaceous, Jurassic and Triassic carbonate and sandstone aquifers reveal CH₄ concentrations of up to 500 μg/l, but a mean value of < 10 μg/l. However, aquiclude and thermal waters from the Carboniferous and Triassic typically contain in excess of 1500 μg/l. Such high concentrations have so far only been found at redox (Eh) potentials below 0 mV, but in general CH₄ concentration and Eh value are poorly correlated. This suggests a lack of thermodynamic equilibrium, which is confirmed by comparing pe values calculated from the redox couple C(4)/C(− 4) with those derived from Eh. Genesis of CH₄ appears to occur on two timescales: a rapid if low rate of production from labile carbon in anaerobic microsites in the soil, and a much longer, millennium scale of production from more refractory carbon. Methane is rarely measured in groundwater; there is no single ionic determinand which acts universally as a proxy, but a combination of high HCO₃ and low SO₄ concentrations, or the reverse, is an indication that high amounts of CH₄ may be present.  相似文献   

Potential for irradiation of methane to form complex organic molecules in impact craters: Implications for Mars, Titan and Europa     

John Parnell  Martin Baron  Paula Lindgren 《Journal of Geochemical Exploration》2006,89(1-3):322

The release of methane from crater sites following meteorite impact is a possible consequence of the thermal alteration of organic matter, or tapping of reservoired gas of biogenic or abiogenic origin. At least the latter is feasible on Mars. Methane and higher hydrocarbons are susceptible to polymerization and precipitation by radioactive minerals. Where such minerals are present in impact target rocks, the craters can be a preferred site for carbon concentration, and the formation of complex organic molecules. On icy bodies, such as Titan and Europa, methane released by impact could be a fuel for prebiotic chemistry involving other forms of irradiation.  相似文献   

A methane fuse for the Cambrian explosion: carbon cycles and true polar wander   总被引：1，自引：0，他引：1  

Joseph L. Kirschvink  Timothy D. Raub 《Comptes Rendus Geoscience》2003,335(1):65-78

The dramatic diversification of animal groups known as the Cambrian Explosion (evolution's ‘Big Bang’) remains an unsolved puzzle in Earth Science. The Vendian–Cambrian interval is characterized by anomalously high rates of apparent plate motion, interpreted as True Polar Wander (TPW), and by more than a dozen large, high-frequency perturbations in carbon isotopes that dwarf all others observed through the past 65 million years. We suggest that these biological, tectonic, and geochemical events are intimately related in the following fashion. First, tropical continental margins and shelf-slopes which formed during fragmentation of the supercontinent Rodinia accumulated massive quantities of isotopically-light organic carbon during Late Neoproterozoic time, as indicated by strikingly heavy isotope ratios in inorganic carbon during interglacial intervals. Second, an initial phase of Vendian TPW moved these organic-rich deposits to high latitude, where conditions favored trapping biogenic methane in layers of gas hydrate and perhaps permafrost. Continued sedimentation during Late Vendian time added additional hydrate/gas storage volume and stabilized underlying units until the geothermal gradient moved them out of the clathrate stability field, building up deep reservoirs of highly pressurized methane. Finally, a burst of TPW brought these deposits back to the Tropics, where they gradually warmed and were subjected to regional-scale thermohaline eddy variation and related sedimentation regime changes. Responding to the stochastic character of such changes, each reservoir reached a critical failure point independently at times throughout the Cambrian. By analogy with the Late Paleocene Thermal Maximum event, these methane deposits yield transient, greenhouse-induced pulses of global warming when they erupt. Temperature correlates powerfully with biodiversity; the biochemical kinetics of metabolism at higher temperature decrease generation time and maintain relatively rich and dense invertebrate populations. Repeated thermal pulses along with progressive disruption and alteration of global ocean circulation patterns by TPW could cause the increase in diversity that accompanied the radiation of metazoans. We suggest that a methane ‘fuse’ ignited the Cambrian Evolutionary Explosion.  相似文献   

Global methane emission through mud volcanoes and its past and present impact on the Earth’s climate—a comment     

Alexei V. Milkov  Giuseppe Etiope 《International Journal of Earth Sciences》2005,94(3):490-492

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DEM simulations of methane hydrate exploitation by thermal recovery and depressurization methods     

《Computers and Geotechnics》2016

Methane hydrate (MH, also called fiery ice) exists in forms of pore filling, cementing and load-bearing skeleton in the methane hydrate bearing sediment (MHBS) and affects its mechanical behavior greatly. To study the changes of macro-scale and micro-scale mechanical behaviors of MHBS during exploitation by thermal recovery and depressurization methods, a novel 2D thermo-hydro-mechanical bonded contact model was proposed and implemented into a platform of distinct element method (DEM), PFC2D. MHBS samples were first biaxially compressed to different deviator stress levels to model different in-situ stress conditions. With the deviator stress maintained at constant, the temperature was then raised to simulate the thermal recovery process or the pore water pressure (i.e. confining pressure for MH bond) was decreased to simulate the depressurization process. DEM simulation results showed that: during exploitation, the axial strain increased with the increase of temperature (in the thermal recovery method) or decrease of pore water pressure (in the depressurization method); sample collapsed during MH dissociation if the deviator stress applied was larger than the compression strength of a pure host sand sample; sample experienced volume contraction but its void ratio was slightly larger than the pure host sand sample at the same axial strain throughout the test. By comparison with the laboratory test results, the new model was validated to be capable of reproducing the exploitation process by thermal recovery and depressurization methods. In addition, some micro-scale parameters, such as contact distribution, bond distribution, and averaged pure rotation rate, were also analyzed to investigate their relationships with the macroscopic responses.  相似文献   

Numerical modeling study of mineralization induced by methane cold seep at the sea bottom     

《Marine and Petroleum Geology》2016

In order to investigate the response of authigenic minerals to gas hydrate geo-systems, the biogeochemical processes and its induced mineralization were predicted by employing the comprehensive reactive transport modeling approach. Based on the available data extracted from the northern continental slope area of the South China Sea, a 1-D vertical column model was developed. Three cases with different upward methane flux rates and three cases with different mineral compositions, i.e., a total of six cases were designed to investigate the effects of variations in the depth of sulfate methane transition zone (SMTZ) and in the mineral composition on the formation of authigenic minerals. The simulation results indicate that the SMTZ depth influenced by both the upward methane flux rate and the initial composition played an important role in the formation of authigenic minerals. The AOM reaction is intensive at the interface, and the precipitation amount of calcite is large, which is mainly controlled by AOM. When the methane leakage rate is 20 times higher than the base case, aragonite starts to precipitate. During the simulation, oligoclase, k-feldspar, smectite-Na, smectite-Ca, chlorite dissolved. Our study specific to this area as a starting point may provide a quantitative approach for investigating carbonate and pyrite formation in hydrate-bearing sediments accounting for methane oxidation and sulfate reduction. The method presented here and the model built in this study can be used for other sites with similar conditions. In addition, this study may serve as an indication for the potential natural gas hydrate reservoir in depth, and is also significant for marine carbon and sulfur cycle.  相似文献   

Methane-derived authigenic carbonates from active hydrocarbon seeps of the St. Lawrence Estuary,Canada     

Denis Lavoie  Nicolas Pinet  Mathieu Duchesne  Andrée Bolduc  Richard Larocque 《Marine and Petroleum Geology》2010

Nearly 2000 pockmarks with diameters ranging from a few tens of meters up to 700 m are present on the seafloor of the St. Lawrence Estuary in eastern Canada. Coring of some pockmarks resulted in the recovery of various-sized and shaped carbonate concretions in a predominantly silty mud matrix. Petrographic and geochemical data on four authigenic carbonate concretions are reported as well as data from shell material in the unconsolidated sediment. Video observations and echo-sounder images indicate that the sampled pockmarks are actively gas venting. The video images show significant look-alike microbial mats in areas where gas is venting. The carbonate concretions are primarily made up of carbonate cements with varying percentage of shell fragments, micrite particles and fine-grained clastics. Orthorhombic crystal morphology and diagenetic fabrics including isopachous layers and botryoids characterize the aragonite cement. Oxygen isotopes ratios for the cement crusts do not record any thermal anomaly at the site of precipitation with δ¹⁸O_VPDB ratios (+3‰) in equilibrium with cold (5 °C) deep marine waters, whereas significant negative δ¹³C_VPDB ratios (−9.9 to −33.5‰) for cement and shell material within concretions indicate that the carbonates largely derive from the microbial oxidation of methane. The δ¹³C_VPDB ratios of aragonite shells (−2.7 to −5.6‰) taken from unconsolidated sediments at some distance from the concretions/vents show variable dilution of HCO₃⁻ with negative δ¹³C_VPDB ratios derived from microbial oxidation of methane with isotopically normal (0‰) marine bicarbonate. These results are in agreement with other lines of evidence suggesting that pockmarks formed through the recent and still active release of gas from a reservoir within the Paleozoic sedimentary succession.  相似文献