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1.
Cycling of methane (CH4) in Tomales Bay, a 28-km2 temperature estuary in northern California with relatively low inputs of organic carbon, was studied over a 1-yr period. Water column CH4 concentrations showed spatial and temporal variability (range=8–100 nM), and were supersaturated with respect to the atmosphere by a factor of 2–37. Rates of net water column CH4 production-oxidation were determined by in situ experiments, and were not found to be significantly different from zero. Fluxes across the sediment-water interface, determined by direct measurement using benthic chambers, varied from ?0.1 μmol m?2 d?1 to +16 μmol m?2 d?1 (positive fluxes into water). Methane concentrations in the two perennial creeks feeding the bay varied annually (140–950 nM); these creeks were a significant CH4 source to the bay during winter. In addition, mass-balance calculations indicate a significant additional inter CH4 source, which is hypothesized to result from storm-related runoff from dairy farms adjacent to the bay. Systemwide CH4 budgets of the 16-km2 inner bay indicate benthic production (110 mol d?1) and atmospheric evasion (110 mol d?1) dominated during summer, while atmospheric evasion (160 mol d?1) and runoff from dairy farms (90 mol d?1) dominated during winter.  相似文献   

2.
This work presents the results from evaluating the gases sorbed by coal samples extracted from the Paleocene Guasare Coalfield (Marcelina Formation, northwestern Venezuela), as well as by their distinct maceral concentrates. The aim of this work has been to obtain an initial experimental main value of the gas content per unit weight of high volatile bituminous A coal samples from the open-pit Paso Diablo mine. An additional goal was to study differences in the CH4 storage ability of the distinct maceral groups forming part of the coal matrix. Both the coal samples and the maceral concentrates were studied by thermogravimetric analysis (TGA) in order to determine the temperature to be used in subsequent experiments. On-line analyses of hydrocarbons (C1, C2, C3) and CO2 yielded gas concentrations, plus δ13C values. Thermogenic gas is prevalent in the Guasare coals with vitrinite reflectance (%Ro) values from 0.65% to 0.88%. The amount of gas retained in the coals and maceral concentrates was measured with a special device that allows determination of the volume of gas sorbed by a solid sample subjected to controlled thermal treatment. The average coalbed gas concentration obtained was 0.51 cm3/g. The following list of maceral concentrates shows the relative capacity for the volume of sorbed gas per unit weight: inertinite > low-density vitrinite > liptinite ≈ high-density vitrinite. It is concluded that the gas volumes retained in the distinct maceral concentrates are not controlled by porosity but rather by their microscopic morphology.  相似文献   

3.
Generation of dust particles from the Owens Lake playa creates a severe air pollution hazard in the western United States. Much of the dust produced from the dry lakebed is derived from salts formed by evaporation of saline groundwater that often contains high concentrations of dissolved arsenic (As). The objectives of this research were to study the spatial distribution of dissolved arsenic in the shallow groundwater, and to examine factors affecting arsenic solubility and speciation. Evapoconcentration, redox potential, pH, and mineral solubility were examined as factors regulating arsenic biogeochemistry. Dissolved arsenic concentrations ranged from 0.1 to 96 mg L−1 and showed a general increase from the shoreline to the center of the lakebed. Arsenic concentrations were strongly correlated to electrical conductivity (EC) and δD suggesting that evapoconcentration is an important process regulating total As concentrations. Arsenite [As(III)] was the dominant form of inorganic arsenic at Eh values less than about −170 mV while arsenate [As(V)] was predominant at higher Eh values. Organic arsenic was negligible (<0.21%) in all shallow groundwater samples. Dissolved arsenic concentrations do not appear to be strongly regulated by solid-phase reactions. Solid-phase arsenic concentrations generally ranged between 4.0 and 42.6 mg kg−1 and a maximum concentration range (20 to 40 mg kg−1) was reached as solution concentration increased up to 80 mg L−1, indicating minimal sorption and/or precipitation of arsenic. Chemical equilibrium modeling indicated that orpiment (As2S3) was the only solid phase with a positive saturation index (indicating over-saturation), but only at high arsenic and sulfide concentrations. The findings of this research are important for assessing the potential environmental impacts of elevated arsenic concentrations on dust mitigation efforts taking place at Owens Dry Lake.  相似文献   

4.
Carbon isotope fractionation factors reported for aerobic bacterial oxidation of CH4(αCH4-CO2) range from 1.003 to 1.039. In a series of experiments designed to monitor changes in the carbon isotopic fractionation of CH4 by Type I and Type II methanotrophic bacteria, we found that the magnitude of fractionation was largely due to the first oxidation step catalyzed by methane monooxygenase (MMO). The most important factor that modulates the (αCH4-CH3OH) is the fraction of the total CH4 oxidized per unit time, which strongly correlates to the cell density of the growth cultures under constant flow conditions. At cell densities of less than 0.1 g/L, fractionation factors greater than 1.03 were observed, whereas at cell densities greater than 0.5 g/L the fractionation factors decreased to as low as 1.002. At low cell densities, low concentrations of MMO limit the amount of CH4 oxidized, while at higher cell densities, the overall rates of CH4 oxidation increase sufficiently that diffusion of CH4 from the gaseous to dissolved state and into the cells is likely the rate-determining step. Thus, the residual CH4 is more fractionated at low cell densities, when only a small fraction of the total CH4 has been oxidized, than at high cell densities, when up to 40% of the influent CH4 has been utilized. Therefore, since Rayleigh distillation behavior is not observed, δ13C values of the residual CH4 cannot be used to infer the amount oxidized in either laboratory or field-studies. The measured (αCH4-CH3OH) was the same for both Type I and Type II methanotrophs expressing particulate or soluble MMO. However, large differences in the δ13C values of biomass produced by the two types of methanotrophs were observed. Methylosinus trichosporium OB3b (Type II) produced biomass with δ13C values about 15‰ higher than the dissimilated CO2, whereas Methylomonas methanica (Type I) produced biomass with δ13C values only about 6‰ higher than the CO2. These effects were independent of the magnitude of the initial carbon isotope fractionation caused by MMO and were relatively constant despite changing ratios of assimilatory to dissimilatory carbon transformation by the organisms. This suggests that the difference in biomass carbon isotopes is primarily due to differences in the fractionation effect at the formaldehyde branch point in the metabolic pathway, rather than assimilation of CO2 by Type II methanotrophs.  相似文献   

5.
《Applied Geochemistry》1999,14(5):607-620
Molecular and isotopic analyses of core gas samples from 3 permafrost research core holes (92GSCTAGLU, 92GSCKUMAK, 92GSCUNIPKAT; sample core depths ranging from 0.36 to 413.82 m) in the Mackenzie Delta of the Northwest Territories of Canada reveal the presence of hydrocarbon gases from both microbial and thermogenic sources. Analyses of most headspace and blended gas samples from the ice-bonded permafrost portion of the core holes yielded C1/(C2+C3) hydrocarbon gas ratios and CH4–C isotopic compositions (δ13C CH4) indicative of microbially sourced CH4 gas. However, near the base of ice-bonded permafrost and into the underlying non-frozen stratigraphic section, an increase in ethane (C2) concentrations, decreases in C1/(C2+C3) hydrocarbon gas ratios, and CH4–C isotopic (δ13C CH4) data indicate the presence of hydrocarbon gases derived from a thermogenic source. The thermogenic gas below permafrost in the Mackenzie Delta likely migrated from deeper hydrocarbon accumulations and/or directly from thermally mature hydrocarbon source rocks.  相似文献   

6.
Hydraulic fracturing of shale deposits has greatly increased the productivity of the natural gas industry by allowing it to exploit previously inaccessible reservoirs. Previous research has demonstrated that this practice has the potential to contaminate shallow aquifers with methane (CH4) from deeper formations. This study compares concentrations and isotopic compositions of CH4 sampled from domestic groundwater wells in Letcher County, Eastern Kentucky in order to characterize its occurrence and origins in relation to both neighboring hydraulically fractured natural gas wells and surface coal mines. The studied groundwater showed concentrations of CH4 ranging from 0.05 mg/L to 10 mg/L, thus, no immediate remediation is required. The δ13C values of CH4 ranged from −66‰ to −16‰, and δ2H values ranged from −286‰ to −86‰, suggesting an immature thermogenic and mixed biogenic/thermogenic origin. The occurrence of CH4 was not correlated with proximity to hydraulically fractured natural gas wells. Generally, CH4 occurrence corresponded with groundwater abundant in Na+, Cl−, and HCO3−, and with low concentrations of SO42−. The CH4 and SO42−concentrations were best predicted by the oxidation/reduction potential of the studied groundwater. CH4 was abundant in more reducing waters, and SO42− was abundant in more oxidizing waters. Additionally, groundwater in greater proximity to surface mining was more likely to be oxidized. This, in turn, might have increased the likelihood of CH4 oxidation in shallow groundwater.  相似文献   

7.
《Applied Geochemistry》1995,10(5):505-516
Stable isotopic ratios of C and H in dissolved CH4 and C in dissolved inorganic C in the ground water of a crude-oil spill near Bemidji, Minnesota, support the concept of CH4 production by acetate fermentation with a contemporaneous increase in HCO3− concentration. Methane concentrations in the saturated zone decrease from 20.6 mg L−1 to less than 0.001 mg L−1 along the investigated flow path. Dissolved N2 and Ar concentrations in the ground water below the oil plume are 25 times lower than background; this suggests that gas exsolution is removing dissolved CH4 (along with other dissolved gases) from the ground water. Oxidation of dissolved CH4 along the flow path seems to be minimal because no measurable change in isotopic composition of CH4 occurs with distance from the oil body. However, CH4 is partly oxidized to CO2 as it diffuses upward from the ground water through a 5- to 7-m thick unsaturated zone; theδ13C of the remaining CH4 increases, theδ13C of the CO2 decreases, and the partial pressure of CO2 increases.Calculations of C fluxes in the saturated and unsaturated zones originating from the degradation of the oil plume lead to a minimum estimated life expectancy of 110 years. This is a minimum estimate because the degradation of the oil body should slow down with time as its more volatile and reactive components are leached out and preferentially oxidized. The calculated life expectancy is an order of magnitude estimate because of the uncertainty in the average linear ground-water velocities and because of the factor of 2 uncertainty in the calculation of the effective CO2 diffusion coefficient.  相似文献   

8.
In order to examine the fluxes of methane (CH4) from the Indian estuaries, measurements were carried out by collecting samples from 26 estuaries along the Indian coast during high discharge (wet) and low water discharge (dry) periods. The CH4 concentrations in the estuaries located along the west coast of India were significantly higher (113?±?40 nM) compared to the east coast of India (27?±?6 nM) during wet and dry periods (88?±?15 and 63?±?12 nM, respectively). Supersaturation of CH4 was observed in the Indian estuaries during both periods ((0.18 to 22.3?×?103 %). The concentrations of CH4 showed inverse relation with salinity indicating that freshwater is a significant source. Spatial variations in CH4 saturation were associated with the organic matter load suggesting that its decomposition may be another source in the Indian estuaries. Fluxes of CH4 ranged from 0.01 to 298 μmol m?2 day?1 (mean 13.4?±?5 μmol m?2 day?1) which is ~30 times lower compared to European estuaries (414 μmol m?2 day?1). The annual emission from Indian estuaries, including Pulicat and Adyar, amounted to 0.39?×?1010 g CH4?year?1 with the surface area of 0.027?×?106 km2 which is significantly lower than that in European estuaries (2.7?±?6.8?×?1010 g CH4?year?1 with the surface area of 0.03?×?106 km2). This study suggests that Indian estuaries are a weak source for atmospheric CH4 than European estuaries and such low fluxes were attributed to low residence time of water and low decomposition of organic matter within the estuary. The CH4 fluxes from the Indian estuaries are higher than those from Indian mangroves (0.01?×?1010 g CH4?year?1) but lower than those from Indian inland waters (210?×?1010 g CH4?year?1).  相似文献   

9.
The shallow aquifer beneath the Western Snake River Plain (Idaho, USA) exhibits widespread elevated arsenic concentrations (up to 120 μg L−1). While semi-arid, crop irrigation has increased annual recharge to the aquifer from approximately 1 cm prior to a current rate of >50 cm year−1. The highest aqueous arsenic concentrations are found in proximity to the water table (all values >50 μg L−1 within 50 m) and concentrations decline with depth. Despite strong vertical redox stratification within the aquifer, spatial distribution of aqueous species indicates that redox processes are not primary drivers of arsenic mobilization. Arsenic release and transport occur under oxidizing conditions; groundwater wells containing dissolved arsenic at >50 μg L−1 exhibit elevated concentrations of O2 (average 4 mg L−1) and NO3 (average 8 mg L−1) and low concentrations of dissolved Fe (<20 μg L−1). Sequential extractions and spectroscopic analysis of surficial soils and sediments indicate solid phase arsenic is primarily arsenate and is present at elevated concentrations (4–45 mg kg−1, average: 17 mg kg−1) relative to global sedimentary abundances. The highest concentrations of easily mobilized arsenic (up to 7 mg kg−1) are associated with surficial soils and sediments visibly stained with iron oxides. Batch leaching experiments on these materials using irrigation waters produce pore water arsenic concentrations approximating those observed in the shallow aquifer (up to 152 μg L−1). While As:Cl aqueous phase relationships suggest minor evaporative enrichment, this appears to be a relic of the pre-irrigation environment. Collectively, these data indicate that infiltrating irrigation waters leach arsenic from surficial sediments to the underlying aquifer.  相似文献   

10.
Groundwaters in the confined aquifers of the Chianan and Ilan coastal plains of Taiwan are rich in dissolved methane (CH4). Serious endemic “blackfoot disease”, which occurred in the Chianan plain, especially during AD1950-1970, has been demonstrated to have arisen from drinking highly reducing groundwater with abnormal arsenic and humic substance levels. In order to explore the origin of CH4 and its hydrological implications, stable carbon isotope ratios (δ13C) and radiocarbon (14C) ages of exsolved CH4, dissolved inorganic carbon (DIC), and sedimentary biogenic sediments from a total of 34 newly completed water wells at 16 sites were determined. The main results obtained are as follows: (1) The δ13CCH4 (−65‰ to −75‰) values indicate that, except for one thermogenic sample (δ13CCH4=38.2‰) from the Ilan plain, all CH4 samples analyzed were produced via microbially mediated CO2 reduction. Many δ13CDIC values are considerably greater than −10‰ and even up to 10‰ due to Rayleigh enrichment during CO2 reduction. (2) Almost all the 14C ages of CH4 samples from the shallow aquifer (I) (<60 m depth) are greater than the 14C ages of coexisting DIC and sediments, suggesting the presence of CH4 from underlying aquifers. (3) The 14C ages of coexisting CH4, DIC and sediments from aquifer (II) of the Chianan plain are essentially equal, reflecting in-situ generation of CH4 and DIC from decomposition of sedimentary organic matter and sluggishness of the groundwater flow. On the other hand, both CH4 and DIC from each individual well of the relatively deep aquifers (III) and (IV) in the Chianan plain are remarkably younger than the deposition of their coexisting sediments, indicating that current groundwaters entered these two aquifers much later than the deposition of aquifer sediments. (4) Each CH4 sample collected from the Ilan plain is older than coexisting DIC, which in turn is distinctly older than the deposition of respective aquifer sediments, demonstrating the presence of much older CO2 and CH4 from underlying strata.  相似文献   

11.
A laboratory investigation was carried out to examine the mechanism of arsenic (As) mobilization under flooded conditions (24 and 240 h) in 18 alluvial soils of Punjab, North–West India. Total dissolved As increased from a range of 3–16 μg L?1 (mean 9 μg L?1) to a range of 33–1,761 μg L?1 (mean 392 μg L?1) with the increase in flooding period from 24 to 240 h. The amount of As mobilization varied depending upon redox potential (pe) created by flooding conditions. After 24 h of flooded conditions, pe of soil water suspension ranged from ?1.75 to 0.77 (mean ?0.24). Increasing the flooding period to 240 h, pe of soil water suspension decreased in the range of ?4.49 to ?2.74 (mean ?3.29). Pourbaix diagram identified arsenate (HAsO4 2?) as predominant species in most of the alluvial soil–water suspensions under oxidized conditions, after 24 h of equilibration period, which ultimately transformed to arsenite (H3AsO3 0) after 240 h of anaerobic condition due to more reduced status. The solid phase identified was orpiment (As2S3). Identification of iron and manganese species in alluvial soil water suspension by Pourbaix diagram indicated decline in both soluble Fe2+ and SO4 2? concentration due to the formation of iron sulfide mineral phase after 240 h under anaerobic conditions. In these soils, decline in soluble Fe was also due to the precipitation of vivianite [Fe3(PO4)2·8H2O]. Elevated arsenic content and low pe value were measured in aquifers located in paddy growing fields comparative to aquifers of other sites. Large degree of variability in As concentrations was recorded in aquifers located at same sites. Thus, it is better to analyze each aquifer for their As content rather than to depends on the prediction on As content of neighbouring wells. The present investigation elucidates that flood irrigation practices in Punjab for growing paddy crop could induce the geochemical conditions favorable to mobilize arsenic from surface soils which could eventually elevate its content in the underlying shallow aquifers. Water abstracted from these aquifers by hand pumps or tube wells for drinking purposes could create hazards for local population due to loading with arsenic concentration above the safe limits. Thus, to avoid further contamination of shallow aquifers with arsenic, it is advisable to shift the flooded rice cultivation to other upland crops having lesser water requirement.  相似文献   

12.
Methane (CH4) is a powerful greenhouse gas and its largest reservoir on Earth is held in marine sediments. CH4 in marine sediments is mainly stored in gas-hydrate reservoirs and deep sedimentary strata along continental margins, where large amounts of deep-sourced CH4 ascend to different degrees toward the seafloor. However, the amount of deep-sourced CH4 and its role in subseafloor carbon and sulfur cycling remains poorly constrained. We analyzed sulfate (SO42?) profiles of 157 sites along with previous published 85 sites to determine the regional distribution and amount of SO42? reduction for an area of 1.23 × 105 km2 of the northern South China Sea. Then we compared these obtained results with estimates based on sedimentation rates from the same area. Significantly higher regional SO42? flux estimates based on SO42? profiles (4.26 × 10?3 Tmol a?1), compared to lower estimates based on sedimentation rates (1.23 × 10?3 Tmol a?1), reflect abundant ascending deep-sourced CH4. The difference of the regional SO42? flux estimates (3.03 × 10?3 Tmol a?1) represents the amount of SO42? reduced by CH4 through the anaerobic oxidation of CH4 (AOM). Deep-sourced CH4 contributes 71% to total SO42? consumption in the study area, largely exceeding SO42? consumption by organoclastic sulfate reduction. Our findings substantiate that deep-sourced CH4 governs subseafloor carbon and sulfur cycling to a previously underrated extent, fueling extensive chemosynthesis-based ecosystems along continental slope and rise.  相似文献   

13.
Environmental geochemistry of high arsenic groundwater at Hetao plain was studied on the basis of geochemical survey of the groundwater and a core sediment. Arsenic concentration in groundwater samples varies from 76 to 1093 μg/L. The high arsenic groundwater mostly appears to be weakly alkaline. The concentrations of NO3− and SO42− are relatively low, while the concentrations of DOC, NH4+, dissolved Fe and sulfide are relatively great. Analysis of arsenic speciation in 21 samples shows that arsenic is present in the solution predominantly as As(III), while particulate arsenic constitutes about 10% of the total arsenic. Methane is detected in five samples with the greatest content being 5107 μg/L. The shallow aquifer in Hangjinhouqi of western Hetao plain is of strongly reducing condition. The arsenic content in 23 core sediment samples varies from 7.7 to 34.6 mg/kg, with great value in clay and mild clay layer. The obvious positive relationship in content between Fe2O3, Mn, Sb, B, V and As indicates that the distribution of arsenic in the sediments may be related to Fe and Mn oxides, and the mobilization of Sb, B and V may be affected by similar geochemical processes as that of As.  相似文献   

14.
The effects of long-term exposure to elevated atmospheric CO2 (ambient + 340 ppmv) on carbon cycling were investigated for two plant communities in a Chesapeake Bay brackish marsh, one dominated by the C3 sedgeSchoenplectus americanus and the other by the C4 grassSpartina patens. Elevated CO2 resulted in a significant increase in porewater concentrations of DIC at 30 cm depth (p < 0.1). The CO2 treatment also yielded increases in DOC (15 to 27%) and dissolved CH4 (12–18%) in the C3 marsh (means for several depths over the period of June 1998 and June 1999), but not at a significant level. Elevated CO2 increased mean ecosystem emissions of CO2 (34–393 g C m−2 yr−1) and CH4 (0.21–0.40 g C m−2 yr−1) in the C3 community, but the effects were only significant on certain dates. For example, CO2 enrichment increased C export to the atmosphere in the C3 community during one of two winter seasons measured (p = 0.09). In the C4 community, gross photosynthesis responded relatively weakly to elevated CO2 (18% increase, p > 0.1), and the concomitant effects on dissolved carbon concentrations, respiration, and CH4 emissions were small or absent. We concluded that elevated CO2 has the potential to increase dissolved inorganic carbon export to estuaries.  相似文献   

15.
The δ13C values of dissolved HCO3? in 75 water samples from 15 oil and gas fields (San Joaquin Valley, Calif., and the Houston-Galveston and Corpus Christi areas of Texas) were determined to study the sources of CO2 of the dissolved species and carbonate cements that modify the porosity and permeability of many petroleum reservoir rocks. The reservoir rocks are sandstones which range in age from Eocene through Miocene. The δ13C values of total HCO3? indicate that the carbon in the dissolved carbonate species and carbonate cements is mainly of organic origin.The range of δ13C values for the HCO3? of these waters is ?20–28 per mil relative to PDB. This wide range of δ13C values is explained by three mechanisms. Microbiological degradation of organic matter appears to be the dominant process controlling the extremely low and high δ13C values of HCO3? in the shallow production zones where the subsurface temperatures are less than 80°C. The extremely low δ13C values (< ?10 per mil) are obtained in waters where concentrations of SO42? are more than 25 mg/l and probably result from the degradation of organic acid anions by sulfate-reducing bacteria (SO42? + CH3COO? → 2HCO3? + HS?). The high δ13C values probably result from the degradation of these anions by methanogenic bacteria (CH3COO? + H2OaiHCO3? + CH4).Thermal decarboxylation of short-chain aliphatic acid anions (principally acetate) to produce CO2 and CH4 is probably the major source of CO2 for production zones with subsurface temperatures greater than 80°C. The δ13C values of HCO3? for waters from zones with temperatures greater than 100°C result from isotopic equilibration between CO2 and CH4. At these high temperatures, δ13C values of HCO3? decrease with increasing temperatures and decreasing concentrations of these acid anions.  相似文献   

16.
《Applied Geochemistry》2001,16(4):419-436
The chemical and isotopic compositions of gases from hydrocarbon systems of the Taranaki Basin of New Zealand (both offshore and onshore) show wide variation. The most striking difference between the western and south-eastern groups of gases is the helium content and its isotopic ratio. In the west, the Maui gas is over an order of magnitude higher in helium concentration (up to 190 μmol mol−1) and its 3He/4He ratio of 3.8 RA (where RA=the air 3He/4He ratio of 1.4×10−6) is approximately half that of upper mantle helium issuing from volcanic vents of the Taupo Volcanic Zone. In the SE, the Kupe South and most Kapuni natural gases have only a minor mantle helium input of 0.03–0.32 RA and low total helium concentrations of 10–19 μmol mol−1. The 3He/C ratio (where C represents the total carbon in the gas phase) of the samples measured including those from a recent study of on-shore Taranaki natural gases are generally high at locations where the surface heat flow is high. The 3He/CO2 ratio of the Maui gases of 5 to 18×10−9 is higher than the MORB value of 0.2 to 0.5×10−9, a feature found in other continental basins such as the Pannonian and Vienna basins and in many high helium wells in the USA. Extrapolation to zero CO2/3He and CO2/C indicates δ13C(CO2) values between −7 and −5‰ close to that of MORB CO2. The remaining CO2 would appear to be mostly organically-influenced with δ13C(CO2) c.−15‰. There is some evidence of marine carbonate CO2 in the gases from the New Plymouth field. The radiogenic 4He content (Herad) varies across the Taranaki Basin with the highest Herad/C ratios occurring in the Maui field. δ13C(CH4) becomes more enriched in 13C with increasing Herad and hydrocarbon maturity. Because 3He/4He is related to the ratio of mantle to radiogenic crustal helium and 3He/C is virtually constant in the Maui field, there is a correlation between RC/RA (where RC=air-corrected 3He/4He) and δ13C(CH4) in the Maui and New Plymouth fields, with the more negative δ13C(CH4) values corresponding to high 3He/4He ratios. A correlation between 3He/4He and δ13C(CO2) was also observed in the Maui field. In the fields adjacent to Mt Taranaki (2518 m andesitic volcano), correlations of some parameters, particularly CO2/CH4, C2H6/CH4 and δ13C(CH4), are present with increasing depth of the gas reservoir and with distance from the volcanic cone.  相似文献   

17.
《Applied Geochemistry》2001,16(7-8):895-910
Coalbed gases in the Lower Silesian Coal Basin (LSCB) of Poland are highly variable in both their molecular and stable isotope compositions. Geochemical indices and stable isotope ratios vary within the following ranges: hydrocarbon (CHC) index CHC=CH4/(C2H6+ C3H8) from 1.1 to 5825, wet gas (C2+) index C2+=(C2H6+ C3H8+ C4H10+ C5H12) / (CH4+ C2H6+ C3H8+ C4H10+ C5H12) 100 (%) from 0.0 to 48.3%, CO2–CH4 (CDMI) index CDMI=CO2/(CO2+ CH4) 100 (%) from 0.1 to 99.9%, δ13C(CH4) from −66.1 to −24.6‰, δD(CH4) from −266 to −117‰, δ13C(C2H6) from −27.8 to −22.8‰, and δ13C(CO2) from −26.6 to 16.8‰. Isotopic studies reveal the presence of 3 genetic types of natural gases: thermogenic (CH4, higher gaseous hydrocarbons, and CO2), endogenic CO2, and microbial CH4 and CO2. Thermogenic gases resulted from coalification processes, which were probably completed by Late Carboniferous and Early Permian time. Endogenic CO2 migrated along the deep-seated faults from upper mantle and/or magma chambers. Minor volumes of microbial CH4 and CO2 occur at shallow depths close to the abandoned mine workings. “Late-stage” microbial processes have commenced in the Upper Cretaceous and are probably active at present. However, depth-related isotopic fractionation which has resulted from physical and physicochemical (e.g. diffusion and adsorption/desorption) processes during gas migration cannot be neglected. The strongest rock and gas outbursts occur only in those parts of coal deposits of the LSCB which are dominated by large amounts of endogenic CO2.  相似文献   

18.
The Pleistocene Kimitsu aquifer was selected for examination of the relationship between groundwater age and chemical evolution of Ca(HCO3)2-type groundwater. For the most part, the aquifer is confined and composed mainly of quartz and feldspar with a small amount of calcite. The groundwater ages calculated by 14C were adjusted by using a carbon mass-balance method and corrected for effects of 14C diffusion. Groundwater ages in the Kimitsu aquifer vary from modern (upgradient) to approximately 2,400 years at 4.4 km from the edge of the recharge area. The 14C age was verified by groundwater velocity calculated from the hydraulic gradient and hydraulic conductivity. The confined groundwater evolved to Ca(HCO3)2-type around 50 years after recharge and this has been maintained for more than 8,300 years due to low chemical reactivity, derived from equilibrium with calcite, kaolinite and Ca-montmorillonite. In addition, high pH prevents the dissolution of Fe and Mn. Consequently, the rate of increase in electrical conductivity ranges from 10 to 30 μS/cm per 1,000 years. On the other hand, leakage from the deep region, which is recognized from high Cl– levels, causes remarkable increases in CH4 and HCO3 – concentrations, resulting in an apparent sulfidic zone at 500-m depth in most downgradient regions.  相似文献   

19.
Methylmercury cation (CH3Hg+) is known to have a strong affinity for organic matter in soil, sedimentary, and aquatic environments. The objective of this study is to determine the dominant ligands binding CH3Hg+ in humic acids by evaluating several CH3Hg+-ligand complexation models, using mercury LIII-edge extended X-ray absorption fine structure (EXAFS). The model CH3Hg+ binding ligands examined in this study include thiol (-SH), hydrogen polysulfide (-SSH or -SSSH), sulfide (-S-), disulfide (-SS-), carboxyl (-COOH), and amine (-NH2). Based on the atomic geometry around mercury in each model structure, we distinguished CH3Hg+-binding ligands in two different humic acids (soil and aquatic). We observed CH3Hg+ preferentially binds to thiol ligands. After saturating reactive thiol ligands, the majority of CH3Hg+ binds to carboxyl ligands rather than to amine or other reduced sulfur ligands than thiol. We found no evidence of significant CH3Hg+-sulfide/disulfide or CH3Hg+-hydrogen polysulfide complexes in any samples. When CH3Hg+ binds to a humic ligand, the C-Hg bond in CH3Hg+ remains intact. Some heavy atoms are proximately coordinated around the mercury atom in the sample containing the highest CH3Hg+ levels used in this study.  相似文献   

20.
Element geochemistry of gold arsenic and mineralogical features of their sulfides in the Carlin-type gold depostis of the Qinling region are discussed in this paper.The initial contents of ore-forming elements such as glod and arsenic are high the ore-bearing rock series in the Qinling region.Furthermore,both the metals are concentrated mainly in the diagenetic pyrite.Study on the mineralogy of arsenic-bearing sulfide minerals in the ores demonstrated that there is a poistive correlation between gold and arsenic in the sulfide minerals.Available evidence suggests that gold in the As-bearing sulfide minerals in likely to be presented as a charge species(Au ),and it is most possible for it to replace the exxcess arsenic at the site of iron and war probably deposited together with arsenic as solid in the sulfide minerals. Pyrite is composed of(Aux^3 ,Fe1-2^2 )([AsS]x^3-[S2]1-x^2-),and arenopyrite of (Aux^3 ,Fe1-x^3 )([AsS]x^3-[AsS2]1-x^3-).The occurrence of glod in the As-sulfied minerals from the Carlin-type gold depostis in the Qinling region has been confirmed by electron probe and transmission electron microscopic studies.The results show that gold was probably depostied together with arsenicas coupled solid solutions in sulfide minerals in the early stage of mineralization.Metallogenic chemical reactions concerning gold deposition in the Carlin-type As-rich gold deposits would involve oxidation of glod and concurrent reduction of arsenic.Later,the deposited gold as solid was remobilized and redistributed as exsolutions,as a result of increasing hydrothermal alteration and crystallization,and decreasing resistance to refractoriness of the host minerals.Gold occurs as sub-microscopic grains(ranging from 0.04tp 0.16μm in diameter)of native gold along micro factures in and crystalline grains of the sulfiedes.  相似文献   

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