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1.
The partitioning of arsenate between Paraho indirectly retorted and directly retorted oil shales and a combusted oil shale was examined with batch equilibrium adsorption isotherms. Arsenate adsorption was found to conform to the Freundlich adsorption model, and the combusted oil shale was found to have the greatest affinity for arsenate. The indirectly and directly retorted oil shale samples did not have statistically different affinities for arsenate. The greater adsorption capacity of combusted oil shale for arsenate was attributed to greater surface area and free iron oxide. Arsenate adsorption by combusted oil shale was not reversible. Upon dilution of the solution phase, arsenate did not desorb. Upon dilution of the retorted oil shale solutions, arsenate continued to be removed from solution. An evaluation of metal arsenate stability in the spent oil shale systems indicated that the retorted oil shale solutions were highly supersaturated with respect to magnesium and barium arsenates, whereas the combusted oil shale solutions were not supersaturated. The data were interpreted to indicate that adsorption reactions control arsenate solubility at short reaction times. As reaction times increase, precipitation reactions control soluble arsenate concentrations.  相似文献   

2.
During weathering, elements enriched in black shale are dispersed in the environment by aqueous and mechanical transport. Here a unique evaluation of the differential release, transport, and fate of Fe and 15 trace elements during progressive weathering of the Devonian New Albany Shale in Kentucky is presented. Results of chemical analyses along a weathering profile (unweathered through progressively weathered shale to soil) describe the chemically distinct pathways of the trace elements and the rate that elements are transferred into the broader, local environment. Trace elements enriched in the unweathered shale are in massive or framboidal pyrite, minor sphalerite, CuS and NiS phases, organic matter and clay minerals. These phases are subject to varying degrees and rates of alteration along the profile. Cadmium, Co, Mn, Ni, and Zn are removed from weathered shale during sulfide-mineral oxidation and transported primarily in aqueous solution. The aqueous fluxes for these trace elements range from 0.1 g/ha/a (Cd) to 44 g/ha/a (Mn). When hydrologic and climatic conditions are favorable, solutions seep to surface exposures, evaporate, and form Fe-sulfate efflorescent salts rich in these elements. Elements that remain dissolved in the low pH (<4) streams and groundwater draining New Albany Shale watersheds become fixed by reactions that increase pH. Neutralization of the weathering solution in local streams results in elements being adsorbed and precipitated onto sediment surfaces, resulting in trace element anomalies.Other elements are strongly adsorbed or structurally bound to solid phases during weathering. Copper and U initially are concentrated in weathering solutions, but become fixed to modern plant litter in soil formed on New Albany Shale. Molybdenum, Pb, Sb, and Se are released from sulfide minerals and organic matter by oxidation and accumulate in Fe-oxyhydroxide clay coatings that concentrate in surface soil during illuviation. Chromium, Ti, and V are strongly correlated with clay abundance and considered to be in the structure of illitic clay. Illite undergoes minimal alteration during weathering and is concentrated during illuvial processes. Arsenic concentration increases across the weathering profile and is associated with the succession of secondary Fe(III) minerals that form with progressive weathering. Detrital fluxes of particle-bound trace elements range from 0.1 g/ha/a (Sb) to 8 g/ha/a (Mo). Although many of the elements are concentrated in the stream sediments, changes in pH and redox conditions along the sediment transport path could facilitate their release for aqueous transport.  相似文献   

3.
The ability to properly manage the oxidation of pyritic minerals and associated acid mine drainage is dependent upon understanding the chemistry of the disposal environment. One accepted disposal method is placing pyritic-containing materials in the groundwater environment. The objective of this study was to examine solubility relationships of Al and Fe minerals associated with pyritic waste disposed in a low leaching aerobic saturated environment. Two eastern oil shales were used in this oxidizing equilibration study, a New Albany Shale (unweathered, 4.6 percent pyrite), and a Chattanooga Shale (weathered, 1.5 percent pyrite). Oil shale samples were equilibrated with distilled-deionized water from 1 to 180 d with a 1∶1 solid-to-solution ratio. The suspensions were filtered and the clear filtrates were analyzed for total cations and anions. Ion activities were calculated from total concentrations. Below pH 6.0, depending upon SO 4 2− activity, Al3+ solubility was controlled by AlOHSO4 (solid phase) for both shales. Initially, Al3+ solubility for the New Albany Shale showed equilibrium with amorphous Al(OH)3. The pH decreased with time, and Al3+ solubility approached equilibrium with AlOHSO4(s). Below pH 6.0, Fe3+ solubility appeared to be regulated by a basic iron sulfate solid phase with the stoichiometric composition of FeOHSO4(s). The results of this study indicate that below pH 6.0, Al3+ solubilities, are limited by basic Al and Fe sulfate solid phases (AlOHSO4(s) and FeHSO4(s)). The results from this study further indicate that the acidity in oil shale waters is produced from the hydrolysis of Al3+ and Fe3+ activities in solution. These results indicate a fundamental change in the stoichiometric equations used to predict acidity from iron sulfide oxidation. The results of this study also indicate that water quality predictions associated with acid mine drainage can be based on fundamental thermodynamic relationships. As a result, waste management decisions can be based on waste-specific/site-specific test methods.  相似文献   

4.
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5.
页岩油气是当前全球油气勘探和研究的热点,但其潜力评价一直是难点。该文以中国和北美的四套典型页岩为例,包括北美湖相Green River组、内陆海相Niobrara组、中国环境来评价相龙马溪组和济阳坳陷湖相页岩,发现页岩沉积环境与其油气潜力具有密切关系,因此可通过分析发现这四套页岩的沉积环境都具有页岩沉积环境评价其页岩油气潜力。通过微量元素、生物标志化合物、扫描电镜、X-CT和X射线衍射等方法,发现这四套页岩都具有一定的还原性和较高的生产力,且具有差异性。内陆海相Niobrara组页岩具有弱还原的沉积环境,在四套页岩中有机碳含量较低,呈块状沉积构造,裂缝与微裂缝较少,储集空间相对有限。焦石坝海相龙马溪组页岩为还原的沉积环境,岩石以富含有机质的硅质岩为主,可观察到大量的大孔隙与少量的微裂缝。Green River页岩和济阳坳陷页岩形成于陆相咸化的强还原沉积环境,有机碳含量高,页岩以纹层状结构为主,岩石组成脆性矿物含量高,含有大量的裂缝。可见,具有强还原沉积环境的页岩通常具有较好的勘探前景。  相似文献   

6.
Spark-source mass spectrometric analysis of pyrolyzed Green River oil shale for trace element distribution showed enhanced concentrations for only lithium and beryllium. In general, trace elemental concentrations were found to be below anticipated crustal amounts. There appears to be no promise of any substantial accumulation of any trace elements within the organic matrix of Green River oil shale.  相似文献   

7.
Benzene extractable aliphatic hydrocarbons from the New Albany Shale in the Illinois Basin were characterized by gas chromatography and mass spectrometry, and the total organic matter of the shale was characterized by solid state carbon-13 cross polarization magic angle spinning nuclear magnetic resonance. Core samples from a northwest-trending cross-section of the Illinois Basin were studied. Gas chromatography (GC) and gas chromatography-mass spectrometric analysis (GC/MS) data indicate a regional variation of the aliphatic composition of the shale extracts. A positive, linear relationship between the two ratios, pristane/n-C17 and phytane/n-C18, is indicated. The NMR results indicated that organic matter deposited in northwestern Illinois shale is relatively high in aliphatic hydrocarbon content while, in contrast, organic matter found in southeastern Illinois shale is relatively low in aliphatic hydrocarbon content. Our findings suggest that the organic variation of the shale is mainly due to the differences in thermal maturity of the shale organic matter and the use of pristane/n-C17 ratio as a thermal parameter in the study of oil may be extended to the study of the ancient sediments.  相似文献   

8.
The adsorption and desorption behavior of selenite by processed Green River Formation oil shales were examined. The selenite adsorption data could be quantitatively described by both the Freundlich and Langmuir isotherms. However, greaterR 2 values were obtained for the Freundlich isotherms. Furthermore, selenite adsorption was not a function of the extraction process. The adsorption of selenite by the processed oil shales was irreversible. Upon dilution of the equilibrium systems, additional selenite removal from solution occurred. A thermochemical analysis of the adsorption and desorption equilibrium solutions indicated that the solutions were undersaturated with respect to a number of metal selenite solids. This indicates that precipitation processes are not influencing selenite behavior. However, not all selenite minerals were examined in the evaluation because of the lack of thermochemical data. An insufficient equilibration period for the adsorption study or the alteration of processed oil shale solids as a result of hydration reactions may also have hastened the additional removal of selenite during the desorption studies.  相似文献   

9.
The determination of trace element release from geologic materials, such as oil shale and coal overburden, is important for proper solid waste management planning. The objective of this study was to determine a correlation between trace element residency and concentration to trace element release using the following methods: (1) sequential selective dissolution for determining trace element residencies, (2) toxicity characteristic leaching procedure (TCLP), and (3) humidity cell weathering study simulating maximum trace element release. Two eastern oil shales were used, a New albany shale that contains 4.6 percent pyrite, and a Chattanooga shale that contains 1.5 percent pyrite. Each shale was analyzed for elemental concentrations by soluble, adsorbed, organic, carbonate, and sulfide phases. All leachates were analyzed to determine total trace element concentrations. The results of the selective dissolution studies show that each trace element has a unique distribution between the various phases. Thus, it is possible to predict trace element release based on trace element residency. The TCLP results show that this method is suitable for assessing soluble trace element release but does not realistically assess potential hazards. The results of the humidity cell studies do demonstrate a more reasonable method for predicting trace element release and potential water quality hazards. The humidity cell methods, however, require months to obtain the required data with a large number of analytical measurements. When the selective dissolution data are compared to the trace element concentrations in the TCLP and humidity cell leachates, it is shown that leachate concentrations are predicted by the selective dissolution data. Therefore, selective dissolution may represent a rapid method to assess trace element release associated with acid mine drainage.  相似文献   

10.
鄂尔多斯盆地中南部发育有侏罗系延安组第二段和第三段陆相暗色厚层泥岩层系,矿物成分以石英、黏土为主,石英43%~56%,黏土矿物29%~33%。总有机碳(TOC)1.63%~3.89%,有机质成熟度Ro为0.59%~0.60%,含气量(CH4)0.25~0.85 m3/t,等温吸附实验表明延安组泥岩的甲烷吸附能力与总有机碳含量呈正相关关系。泥岩处于生物成因气阶段,具备页岩气形成的基本地质条件,并可对比美国密歇根盆地Antrim页岩和伊利诺斯盆地的New Albany页岩的地质条件。为查清黄陵北部侏罗系延安组页岩气的勘探潜力,通过分析勘查和化验测试资料,对其页岩气勘探潜力进一步评价认为:黄陵北部延安组泥岩分布范围和厚度较大,已进入生物成因气和热催化生气的中间阶段,有机质丰度较高,具备形成页岩气的成藏条件,页岩气潜力巨大。   相似文献   

11.
The engineering properties of solid waste produced by the combustion of Western oil shale are evaluated and discussed. Index properties and their variability, moisture—density relationships, shear strength, stress—strain characteristics, and hydraulic conductivity were evaluated in laboratory tests. Cementation caused by the formation of hydrous cements when combusted oil shale is exposed to water was found to be the most significant factor affecting its engineering properties. With increasing initial water content, shear strength increases and hydraulic conductivity decreases significantly, primarily because of cementation. Implications for the design of waste disposal embankments are discussed.  相似文献   

12.
Comprehensive understanding of chemical and mineralogical changes induced by weathering is valuable information when considering the supply of nutrients and toxic elements from rocks. Here minerals that release and fix major elements during progressive weathering of a bed of Devonian New Albany Shale in eastern Kentucky are documented. Samples were collected from unweathered core (parent shale) and across an outcrop excavated into a hillside 40 year prior to sampling. Quantitative X-ray diffraction mineralogical data record progressive shale alteration across the outcrop. Mineral compositional changes reflect subtle alteration processes such as incongruent dissolution and cation exchange. Altered primary minerals include K-feldspars, plagioclase, calcite, pyrite, and chlorite. Secondary minerals include jarosite, gypsum, goethite, amorphous Fe(III) oxides and Fe(II)-Al sulfate salt (efflorescence). The mineralogy in weathered shale defines four weathered intervals on the outcrop—Zones A–C and soil. Alteration of the weakly weathered shale (Zone A) is attributed to the 40-a exposure of the shale. In this zone, pyrite oxidization produces acid that dissolves calcite and attacks chlorite, forming gypsum, jarosite, and minor efflorescent salt. The pre-excavation, active weathering front (Zone B) is where complete pyrite oxidation and alteration of feldspar and organic matter result in increased permeability. Acidic weathering solutions seep through the permeable shale and evaporate on the surface forming abundant efflorescent salt, jarosite and minor goethite. Intensely weathered shale (Zone C) is depleted in feldspars, chlorite, gypsum, jarosite and efflorescent salts, but has retained much of its primary quartz, illite and illite–smectite. Goethite and amorphous FE(III) oxides increase due to hydrolysis of jarosite. Enhanced permeability in this zone is due to a 14% loss of the original mass in parent shale. Denudation rates suggest that characteristics of Zone C were acquired over 1 Ma. Compositional differences between soil and Zone C are largely attributed to illuvial processes, formation of additional Fe(III) oxides and incorporation of modern organic matter.  相似文献   

13.
Aromatic hydrocarbons from benzene extracts of New Albany Shale were characterized. A biomarker that has a molecular weight of 546 and a structural configuration consistent with that of an alkyl-aromatic hydrocarbon (C40H66) was tentatively identified. It was found that the relative concentrations of the biomarker are indicative of differing levels of thermal maturity of the shale organic matter. A 40-carbon bicyclic carotenoid (C40H48) is proposed as the geochemical precursor of this biomarker. Thermal maturity of the shale organic matter can also be differentiated by observing differences in “fingerprints” as obtained by field-ionization mass spectrometry on the aromatic hydrocarbon fraction. Using this technique, we found that the more mature shale samples from southeastern Illinois contain more low molecular weight extractable aromatic hydrocarbons and the less mature shale samples from northwestern Illinois contain more high molecular weight extractable aromatic hydrocarbons. It was demonstrated that field-ionization and tandem mass spectrometric techniques through fingerprint and individual compound identification, are useful for shale aromatic hydrocarbon fraction characterization and for thermal maturation interpretation.  相似文献   

14.
The hydrogeochemistry of saline-meteoric water interface zones in sedimentary basins is important in constraining the fluid migration history, chemical evolution of basinal brines, and physical stability of saline formation waters during episodes of freshwater recharge. This is especially germane for interior cratonic basins, such as the Michigan and Illinois basins. Although there are large differences in formation water salinity and hydrostratigraphy in these basins, both are relatively quiescent tectonically and have experienced repeated cycles of glaciation during the Pleistocene. Exploration for unconventional microbial gas deposits, which began in the upper Devonian-age Antrim Shale at the northern margin of the Michigan Basin, has recently extended into the age-equivalent New Albany Shale of the neighboring Illinois Basin, providing access to heretofore unavailable fluid samples. These reveal an extensive regional recharge system that has profoundly changed the salinity structure and induced significant biogeochemical modification of formation water elemental and isotope geochemistry.New-formation water and gas samples were obtained from Devonian-Mississippian strata in the Illinois Basin. These included exploration wells in the New Albany Shale, an organic-rich black shale of upper Devonian age, and formation waters from over- and underlying regional aquifer systems (Siluro-Devonian and Mississippian age). The hydrostratigraphic relations of major aquifers and aquitards along the eastern margin of the Illinois Basin critically influenced fluid migration into the New Albany Shale. The New Albany Shale formation water chemistry indicates significant invasion of meteoric water, with δD values as low as −46.05‰, into the shale. The carbon stable isotope system (δ13C values as high as 29.4‰), coupled with δ18O, δD, and alkalinity of formation waters (alkalinity ≤24.08 meq/kg), identifies the presence of microbial gas associated with meteoric recharge. Regional geochemical patterns identify the underlying Siluro-Devonian carbonate aquifer system as the major conduit for freshwater recharge into the fractured New Albany Shale reservoirs. Recharge from overlying Mississippian carbonates is only significant in the southernmost portion of the basin margin where carbonates directly overlie the New Albany Shale.Recharge of dilute waters (Cl− <1000 mM) into the Siluro-Devonian section has suppressed formation water salinity to depths as great as 1 km across the entire eastern Illinois Basin margin. Taken together with salinity and stable isotope patterns in age-equivalent Michigan Basin formation waters, they suggest a regional impact of recharge of δ18O- and δD-depleted fluids related to Pleistocene glaciation. Devonian black shales at both basin margins have been affected by recharge and produced significant volumes of microbial methane. This recharge is also manifested in different salinity gradients in the two basins because of their large differences in original formation water salinity. Given the relatively quiet tectonic history and subdued current topography in the midcontinent region, it is likely that repeated cycles of glacial meltwater invasion across this region have induced a strong disequilibrium pattern in fluid salinity and produced a unique class of unconventional shale-hosted gas deposits.  相似文献   

15.
Small diameter core samples were taken from outcrops of the Permian Phosphoria Formation and the Cretaceous Pierre Shale of the Western United States to determine the effects of weathering on organic matter in shale outcrops. While the Pierre Shale core showed no evidence of weathering, the Phosphoria Formation showed significant reduction of overall organic content and pronounced changes in organic composition over the near-surface interval of the core. Total organic carbon is lower by as much as 60% over the upper 2 ft of the core. Chloroform-soluble organic matter and total hydrocarbon (C15+) concentrations are 50% lower over this same interval. The ratio of saturated to aromatic hydrocarbons decreases steadily with core depth over the upper 2.6 ft of the core. Aromatic hydrocarbons are enriched in the stable carbon-13 isotope by an average of 1.7%. over this same interval. Shallow core samples also show a loss of n-paraffins relative to branched/cyclic compounds in the saturated C15+ fraction.Although the extent of weathering is variable, certain characteristic effects are recognizable and can be applied to the interpretation of outcrop data in organic geochemical studies.  相似文献   

16.
Soils derived from black shale can accumulate high concentrations of elements of environmental concern, especially in regions with semiarid to arid climates. One such region is the Colorado River basin in the southwestern United States where contaminants pose a threat to agriculture, municipal water supplies, endangered aquatic species, and water-quality commitments to Mexico. Exposures of Cretaceous Mancos Shale (MS) in the upper basin are a major contributor of salinity and selenium in the Colorado River. Here, we examine the roles of geology, climate, and alluviation on contaminant cycling (emphasis on salinity and Se) during weathering of MS in a Colorado River tributary watershed. Stage I (incipient weathering) began perhaps as long ago as 20 ka when lowering of groundwater resulted in oxidation of pyrite and organic matter. This process formed gypsum and soluble organic matter that persist in the unsaturated, weathered shale today. Enrichment of Se observed in laterally persistent ferric oxide layers likely is due to selenite adsorption onto the oxides that formed during fluctuating redox conditions at the water table. Stage II weathering (pedogenesis) is marked by a significant decrease in bulk density and increase in porosity as shale disaggregates to soil. Rainfall dissolves calcite and thenardite (Na2SO4) at the surface, infiltrates to about 1 m, and precipitates gypsum during evaporation. Gypsum formation (estimated 390 kg m−2) enriches soil moisture in Na and residual SO4. Transpiration of this moisture to the surface or exposure of subsurface soil (slumping) produces more thenardite. Most Se remains in the soil as selenite adsorbed to ferric oxides, however, some oxidizes to selenate and, during wetter conditions is transported with soil moisture to depths below 3 m. Coupled with little rainfall, relatively insoluble gypsum, and the translocation of soluble Se downward, MS landscapes will be a significant nonpoint source of salinity and Se to the Colorado River well into the future. Other trace elements weathering from MS that are often of environmental concern include U and Mo, which mimic Se in their behavior; As, Co, Cr, Cu, Ni, and Pb, which show little redistribution; and Cd, Sb, V, and Zn, which accumulate in Stage I shale, but are lost to varying degrees from upper soil intervals. None of these trace elements have been reported previously as contaminants in the study area.  相似文献   

17.
The Upper Ordovician-Lower Silurian Longmaxi Shale in the Upper Yangtze block represents one of the most important shale gas plays in China. The shale composition, porosity, organic thermal maturity, and methane sorption were investigated at the Qilongcun section in the Dingshan area, southeastern Sichuan Basin. The results show that the Upper Ordovician-Lower Silurian Longmaxi Shale contains: (1) sapropelic I organic matter; (2) a 40-m thick bedded sequence where total organic carbon (TOC) content is > 2%; (3) a 30-m thick layer at the base of the Longmaxi Shale with a brittle mineral content higher than 50%; and (4) a mean methane adsorption capacity of 1.80 cm3/g (7 MPa pressure). A positive correlation between TOC and sorbed gas indicates that organic matter content exerts an important control on methane storage capacity. Based on the analysis of the shale reservoir characteristics, the lower member of the Longmaxi Shale can thus be considered a favorable stratum for shale gas exploration and exploitation. It has similar reservoir characteristics with the Longmaxi Shale in the Jiaoshiba area tested with a high-yield industrial gas flow. However, based on tectonic analysis, differences in the level of industrial gas flow between the low-yield study area and the high-yield Jiaoshiba area may result from different tectonic preservation conditions. Evidence from these studies indicates the shale gas potential of the Longmaxi Shale is constrained by the reservoir and preservation conditions.  相似文献   

18.
页岩气以吸附态、游离态和溶解态存在于页岩储层中,其中吸附态为主要赋存状态,考察页岩气解吸特征对于我国页岩气勘探开发研究有着重要的理论指导意义。选取了位于南方海相页岩储区的四川和湖北荆门等地的页岩样品,对其常规地球化学性质进行了分析,结果表明页岩样品有机碳含量较高且发育较为成熟;采用MSB磁悬浮天平等温吸附仪进行等温解吸实验并对解吸速率和解吸效率进行计算,结果表明：30~10 MPa时页岩解吸量很低并且无明显变化;10~05 MPa时页岩解吸量迅速上升,该阶段为主要解吸段;吸附势理论可用于判断页岩气解吸情况和页岩样品解吸性能强弱,吸附势越大越不利于解吸  相似文献   

19.
The Shengli River-Changshe Mountain oil shale zone, located in the North Qiangtang depression, northern Tibet plateau, represents a potentially large marine oil shale resource in China. Twenty-eight samples including oil shale, micritic limestone and marl were collected from the Shengli River area to determine the contents and distribution patterns of rare earth elements (REEs) in marine oil shale. Oil shale samples from the Shengli River area have high ash yield (61.86–67.48%) and TOC content (8.02–13.67%) with low total sulfur (St,d) content (0.76–1.39%) and intermediate shale oil content (3.60–16.30%). The total rare earth element (ΣREE) content in oil shale samples is notably depleted (46.79–67.90 μg/g), approximately one third of the mean value of the North American Shale Composite (NASC), and lower than that of world-wide black shales and Chinese coals, but higher than that of world-wide coals and micritic limestone samples (29.21 μg/g) from the Shengli River area. The oil shale samples from the Shengli River area exhibit shale-like Chondrite or NASC-normalized REE patterns similar to those of micritic limestone and marl samples from this area, indicating that REEs of these different lithological samples may have been derived from a similar terrigenous source.REE contents of oil shale samples are highly positive correlated with ash yield and show a positive correlation with Fe and a weakly positive correlation with organic sulfur, and the vertical variations of REEs mainly follow those of Si, Al, K and Ti. All these facts indicate that the REE contents in oil shale seams are mainly controlled by clay minerals and, to a lesser extent, by pyrite, as well as partly associated with oil shale organic constituents. Rare earth elements in the Shengli River oil shale have originated from two sources: a felsic volcanic rock source and a clastic or/and limestone source.  相似文献   

20.
The determination of trace element concentrations in oil shale before mining and retorting is required for proper solid-waste management planning. Using routine Fischer assay oil yield data collected during resource characterization as indicators of potential trace element concentrations could lead to a standard method of identifying strata containing high trace element levels. In order to determine a correlation between trace element concentrations and oil yield, shale samples were selected from four statigraphic zones of the Parachute Creek Member of the Green River Formation for analysis. All samples were analyzed for total elemental concentrations, mineralogy, and Fischer assay oil yield. The results of these analyses demonstrated that the Mahogany zone shales contain significantly greater trace element concentrations (antimony, arsenic, cadmium, chromium, copper, lead, lithium, mercury, molybdenum, nickel, selenium, silver, and vanadium) than the other three shale zones. These high trace element concentrations have been identified within well-defined interbedded tuff deposits in the Mahogany zone. In addition, all trace elements evaluated, except boron, show either increasing or decreasing concentrations as oil yield increases within all oil shale zones. With an increased number of analyses of existing oil shale cores, oil yield data will be correlated to specific stratigraphic units containing high trace element concentrations.  相似文献   

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