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1.
The thermodynamic stability of selected alkylated, dealkylated and rearranged 17α- and 17β-hopane isomers in the C27, C28, C29, C30 and C31 families were calculated using molecular mechanics (MM2) methods and, where possible, calculated equilibrium ratios of certain isomers were compared with observed ratios of isomers in thermally mature crude oil samples. Those calculated and observed ratios having similar values include: (1) the relative distributions among 17β(H)/17α(H) and 21β(H)/21α(H)-hopanes including the absence of the 17β(H),21β(H)- and 17α(H),21α(H)-hopanes; (2) the 22R/22S ratios in 30-methyl-17α-hopane and 30-methyl-17β-moretane; (3) the relative distributions among 17α(H)/17β(H)- and 21α(H)/21β(H)-28,30-bisnorhopanes and among 25,28,30-trisnorhopanes, including the relatively greater stability of 17β(H) isomers in contrast to the regular hopane series; and (4) the ratios of 28(18−17S)abeo hopanes with respect to their unrearranged counterparts including the C27 compounds, Ts/Tm.  相似文献   

2.
Series of α, β, ω and (ω-1) hydroxy fatty acids (FAOHs) were determined in several freshwater and brackish water lacustrine sediments in Japan. Analytical procedure used was digestion of the solvent-extracted sediment with HF/HCl followed by solvent and saponification extraction of the residue. Abundances of α/β and ω-FAOH determined by this procedure were 2–3 times higher than those obtained by single alkaline saponification and of the same order with those provided by HCl hydrolysis. Major portion of α/β-FAOH was obtained by solvent extraction of the acid-treated sediments, while subsequent alkaline saponification was needed for the majority of ω-FAOH to be recovered. Thus determined FAOHs comprised 33–61% (Av. = 42%) of the “bound” acid constituents in the lacustrine surface sediments. The α/β and ω-FAOH composition was principally the same among the samples examined, except for relative proportions of the iso to anteiso C15 and C17 ß(α)-FAOH, which showed significant variations in the ranges of 0.30–1.1 and 0.46–1.5, respectively. In the holomictic lakes, the ratios together with the same ratios of the “bound” branched monocarboxylic acids tended to decrease with increasing water depth of the lakes, suggesting that the ratios may indicate an extent of the early diagenetic alteration of the bacteria-derived lipids either in water column or in surface sediment.  相似文献   

3.
A series of tricyclic terpenoid carboxylic acids (C20–C40) was found in the acidic fraction of Tasmanian tasmanite bitumen, occurring as a mixture of stereoisomers with mainly the 13β(H), 14α(H)-and 13α(H),14α(H)-configurations. These dominant acidic tricyclic constituents have the same carbon skeleton as the ubiquitous tricyclic terpane biomarkers. A novel series of ring-C monoaromatic tricyclic terpenoid carboxylic acids was also characterized. The series ranges from C19 to C39 and is the acidic counterpart of the recently described series of monoaromatic tricyclic terpanes.  相似文献   

4.
The major steranes of the non-asphaltene fraction of Nigerian tar sand bitumen (maltene) are the c27-c29 diasteranes [13β(H),17α(H); 20R + S] and C28-C29 regular steranes [14β (H),17β (H); 20S]. The reducing metal reaction products of the corresponding asphaltenes (maltene-I) contain mainly C27-C29 regular steranes with the 14β(H),17β(H); 20R + S and 14α(H),17α(H); 20R + S configurations as well as the corresponding diasteranes having the 13β(H),17α(H); 20R + S configuration. These sterane distributions suggest that maltene-I corresponds to an unaltered oil whilst the maltene is equivalent to the product of severe biodegradation of maltene-I. This is consistent with maltene-I being the remnant of “original oil” trapped within the asphaltene matrix and protected from the effect of in-reservior biodégradation.Degradation of Nigerian asphaltenes by refluxing with ferric chloride-acetic anhydride or methanolic potassium hydroxide also releases soluble reaction products having the characteristics of unaltered oil such as the presence of n-alkanes having an unbiased distribution. These methods appear to be milder and more suitable than reducing metal reactions for releasing hydrocarbons occluded by asphaltenes.  相似文献   

5.
This work describes the origin, applications and limitations of a specific biomarker: 18α(H)-oleanane, which is a paleoenvironmental, organic matter type and age indicator for the assessment of oil–oil and oil–source rock correlations. Specific cases in which this compound has been detected in oils and source rocks in the two main Venezuelan petroleum basins are presented in this work, along with scenarios for future research.  相似文献   

6.
The local and geometrical structure around gold (III) e.g., Au3+ ions in aqueous solution with different OH−/Cl− molar ratios, has been investigated by X-ray absorption spectroscopy (XAS). X-ray absorption near-edge structure (XANES) spectra of [AuCln(OH)4−n]− solutions have been calculated and the multiple-scattering spectral features have been attributed to Cl d-states, axial water molecules and the replacement of Cl− ligands by OH− ligands. A square–planar geometry for [AuCln(OH)4−n]− with two axial water molecules has been identified. Moreover, a spectral correlation between XANES features and the type of planar atoms has been identified. By extended X-ray absorption fine structure spectra (EXAFS), the planar Au bond distances in the solutions have also been determined, e.g., 2.28 Å for Au–Cl and 1.98 Å for Au–O, respectively. The same EXAFS analysis provides evidence that the peak at about 4.0 Å in solutions with the lowest OH−/Cl− molar ratio arises from collinear Cl–Au–Cl multiple-scattering contributions. For the first time, a complete detailed reconstruction of the hydration structure of an Au ion at different pH values has been achieved.  相似文献   

7.
A quantitative sterane biomarker study was conducted on a series of paralic freshwater lacustrine shale samples ranging in maturity from immature to near oil window maturity taken from Section 3 of the Shahejie Formation (Es3) in the Liaohe Basin, N.E. China. Concentrations of 5α(H),14α(H),17α(H)-20S and 5α(H),14β(H),17β(H)-steranes remain nearly constant throughout the sample suite. However, the decrease in the absolute concentrations of the 20R-5α(H),14α(H),17α(H)-C29 steranes with increasing maturity results in an increase in the conventionally defined maturity parameters, 20S/(20S + 20R)-ααα and αββ/(ααα + αββ) sterane ratios. In addition, the data suggest that relatively early generation of 5α(H),14α(H),17α(H)-20S and 5α(H),14β(H),17β(H)-steranes has occurred in lacustrine sediments with a vitrinate reflectance 0.3% (Ro). The data provide strong support for the major importance of relative thermal stability of epimers, but do not exclude the possibility of isomerization as a viable mechanism for production.  相似文献   

8.
This study presents new data on major, trace and REE element concentration of groundwaters in Lastochka spa located in the northern part of Primorye, Far East of Russia. The studied area is characterized by two types of groundwaters issued from a spring and wells: fresh waters with low mineralization (Total Dissolved Solids is up to 400 mg/l) and high pCO2 waters with high mineralization (TDS is up to 4700 mg/l). New data and previous δ13C(TIC), oxygen (δ18O) and hydrogen (δ2H) isotope data indicate that these waters result from meteoric water infiltration in the Sikhote–Alin mountain, circulating at shallow depths in sedimentary rocks. CO2 in groundwater is of mantle origin.  相似文献   

9.
The extent of sterane isomerisation reactions and the moretane/hopane ratios of 234 crude oils, taken world wide, from a wide variety of source rocks of differing geological ages, have been measured.This data indicates that in 78 crude oils derived from Tertiary source rocks, sterane isomerisation reactions as determined by the 20S/(20S + 20R) ration of the C29 5α(H), 14α(H), 17α(H) normal-steranes and the C29 iso/(iso + normal) ratio [iso = 5α (H), 14β(H), 17β(H)] are mainly incomplete and sometimes considerably so. In addition, the same crude oils have 17β(H), 21α(H)-moretane/17α(H), 21β(H)-hopane ratios which are significantly greater (predominantly in the range 0.10–0.30) than those of crude oils derived from older, mature source rocks (mainly less than 0.1).This data, for crude oils, lends support to the hypothesis, proposed by Mackenzie and McKenzie (1983) for source rock extracts, that the time/temperature constraints of sterane isomerisation reactions are such that the time available for isomerisation in Tertiary sediments is generally insufficient, despite generation of crude oil at relatively high temperatures.An alternative hypothesis is that the incomplete sterane isomerisation of Tertiary crude oils may be due to generation of these crude oils from their deltaic, land plant-containing source rocks under low heating conditions.A third hypothesis proposes that the Tertiary crude oils may have picked up the incompletely isomerised steranes from immature sediments during migration. Although possible in particular instances, such a mechanism does not appear to be generally applicable since, in that case, the phenomenon would then appear to be restricted to the Tertiary.The higher moretane/hopane ratios of the Tertiary crude oils could suggest that constraints, similar to those applying in sterane isomerisation, also operate in the conversion of moretane to 17α(H)-hopane.  相似文献   

10.
We recently showed that silicon isotopic fractionation in banana (Musa acuminata Colla, cv Grande Naine) was related to phytolith production, and therefore to silica content in plant. The present study focuses on isotopic fractionation between the different plant parts. Silicon isotopic compositions were measured using a Nu plasma multicollector plasma source mass spectrometer (MC–ICP–MS) operating in dry plasma mode. The results are expressed as δ29Si relatively to the NBS28 standard, with an average precision and accuracy of ± 0.08‰ (± 2σ). On mature banana (Musa acuminata Colla, cv Grande Naine) from Cameroon, δ29Si ranged from + 0.13‰ in the petiole to + 0.49‰ in the lamina, yielding to a 0.36‰ change towards heavier isotopic composition in the upper parts of the plant. This strongly accords with results obtained on in vitro banana plantlets cultivated in hydroponics, where the δ29Si increase from pseudostems to lamina is 0.26‰. These preliminary results on in situ banana show a trend of intra-plant fractionation comparable with that of in vitro hydroponics banana plantlets and with previous data obtained on bamboo.  相似文献   

11.
Multi-equilibrium thermobarometry shows that low-grade metapelites (Cubito-Moura schists) from the Ossa–Morena Zone underwent HP–LT metamorphism from 340–370 °C at 1.0–0.9 GPa to 400–450 °C at 0.8–0.7 GPa. These HP–LT equilibriums were reached by parageneses including white K mica, chlorite and chloritoid, which define the earliest schistosity (S1) in these rocks. The main foliation in the schists is a crenulation cleavage (S2), which developed during decompression from 0.8–0.7 to 0.4–0.3 GPa at increasing temperatures from 400–450 °C to 440–465 °C. Fe3+ in chlorite decreased greatly during prograde metamorphism from molar fractions of 0.4 determined in syn-S1 chlorites down to 0.1 in syn-S2 chlorites. These new data add to previous findings of eclogites in the Moura schists indicating that a pile of allochtonous rocks situated next to the Beja-Acebuches oceanic amphibolites underwent HP–LT metamorphism during the Variscan orogeny. To cite this article: G. Booth-Rea et al., C. R. Geoscience 338 (2006).  相似文献   

12.
The kerogen of a sample of Estonian Kukersite (Ordovician) was examined by spectroscopic (solid state 13C NMR, FTIR) and pyrolytic (“off-line”, flash) methods. This revealed an important contribution of long, linear alkyl chains in Kukersite kerogen. The hydrocarbons formed upon pyrolysis are dominated by n-alkanes and n-alk-1-enes and probably reflect a major contribution of selectivity preserved, highly aliphatic, resistant biomacromolecules from the outer cell walls of Gloeocapsomorpha prisca. This is consistent with the abundant presence of this fossilized organism in Kukersite kerogen. In addition high amounts of phenolic compounds were identified in the pyrolysates. Series of non-methylated, mono-, di- and trimethylated 3-n-alkylphenols, 5-n-alkyl-1,3-benzenediols and n-alkylhydroxybenzofurans were identified. All series of phenolic compounds contain long (up to C19), linear alkyl side-chains. Kukersite kerogen is, therefore, an aliphatic type II/I kerogen, despite the abundance of free phenolic moieties. This study shows that phenol-derived moieties are not necessarily associated with higher plant-derived organic matter.The flash pyrolysate of Kukersite kerogen was also compared with that of the kerogen of the Guttenberg Oil Rock (Ordovician) which is also composed of accumulations of fossilized G. prisca. Similarities in the distributions of hydrocarbons and sulphur compounds were noted, especially for the C1–C6 alkylbenzene and alkylthiophene distributions. However, no phenolic compounds were detected in the flash pyrolysate of the Guttenberg kerogen. Possible explanations for the observed similarities and differences are discussed.  相似文献   

13.
The Karacadağ (Kulu-Konya) area is one of the main volcanic provinces in Central Anatolia. The Karacadağ volcanites are composed of large volumes of andesitic-dacitic lavas associated with pyroclastics and small volumes of alkali basalt, trachybasalt and trachyandesite lavas. Two groups of volcanic rocks can be distinguished: (1) calcalkaline rocks including andesites and dacites, and (2) alkaline rocks including basalts, trachybasalts and trachyandesites. 40Ar/39Ar ages show that the Karacadağ volcanites were erupted during Early Miocene (ca.18–19 Ma) and suggest that alkaline volcanites succeed shortly afterwards calcalkaline volcanites. Major oxides and trace elements plotted versus SiO2 suggest fractionation of hornblende, Fe–Ti oxide and apatite for calcalkaline volcanic rocks and olivine, clinopyroxene and Fe–Ti oxide for alkaline volcanic rocks in the magmatic evolution. The incompatible trace element patterns of the calcalkaline volcanites show enrichment of LILEs (Sr, K, Rb, Ba and Th) and negative HFSEs (Nb, Ta) anomalies suggesting an enriched lithospheric source by a subduction-related process. On the other hand, alkaline volcanites show enrichment of both LILEs and HFSEs suggesting an enriched lithospheric source by small volume melts from the asthenosphere. The rocks also have moderately fractionated REE patterns with (La/Lu)N ratios of 7–24 for calcalkaline and 6–17 for alkaline volcanites. Moreover, the volcanites have relatively low 87Sr/86Sr(t) ratios for between 0.703782 and 0.705129, and high εNd(t) values between +2.25 and +4.49. Generally, the Sr–Nd isotopic compositions of the rocks range from the mantle array to bulk earth. All of these observations and findings suggest that the calcalkaline volcanites were formed in a subduction modified orogenic setting, and the alkaline volcanites in a within-plate setting.  相似文献   

14.
This study describes the reduction of functionalised model compounds to their corresponding hydrocarbons by catalytic hydropyrolysis to provide information on the release of biomarkers from kerogens and asphaltenes covalently bound through the functional groups investigated. Five model compounds were investigated, the n-C18 carboxylic acids, stearic and oleic acids; the C24 steroidal acid, 5β-cholanic acid; and the saturated and unsaturated C27 sterols, 5α-cholestanol and cholesterol. The yield and distribution of the hydrocarbons generated were assessed for the model compounds adsorbed to silica and carbon substrates, and unsupported on a bed of catalyst. The n-C18 acids are shown to be reduced to the n-C18 alkane, with a selectivity of >95% for stearic acid, although due to its unsaturated structure, oleic acid is prone to cracking, with shorter chained n-alkanes also being formed. The conversion of these compounds, adsorbed to either silica or carbon is relatively low, even at hydropyrolysis temperatures significantly above their boiling point, suggesting that interactions between the acids and substrate leading to the formation of stable entities (Si–O–C linkages in the case of silica) significantly retard volatilisation. The yield can be increased by placing the compounds directly onto a bed of catalyst, but for low boiling compounds such as stearic acid this can result in volatilisation and cracking at temperatures below that of the activation point of the catalyst. This method produced improved yields of >95% pure product for higher boiling compounds such as 5β-cholanic acid. The presence of the functional group attached to the ring system of compounds such as 5α-cholestanol does not diminish the selectivity of the technique. The double bond in cholesterol resulted in more incomplete hydrogenation with sterenes being generated, and in addition to 5α and 5β-cholestane, diasteranes were also generated via migration of the double bond.  相似文献   

15.
Carotenoid pigments are ubiquitous components of the biosphere but have rarely been reported in geological samples. Oils from the Kelamayi oilfield of northwestern China have been shown by GC-MS analysis to contain abundant carotenoid-derived alkanes including β- and γ-carotanes, 1,1,3-trimethyl-2-alkylcyclohexanes and a compound tentatively identified as saturated lexene. In addition, a seepage oil contained a possible C40 alkene with a structure similar to that of β-carotane except for a carbon-carbon double bond in one of the cyclohexyl rings. The distributions of biomarker compounds in these oils are very similar to those observed in the few other reported samples that contain abundant carotenoid-derived compounds, indicating that the Kelamayi source rock was probably deposited under very specific environmental conditions. The distribution of carotenoid-derived compounds, particularly the ratio of γ-carotane to β-carotane, appears to be sensitive to both thermal maturation and biodégradation. This ratio increases with maturation and decreases with increasing biodegradation.  相似文献   

16.
New field, petrological, geochemical, and geochronological data (U–Pb and Sm–Nd) for Ordovician rock units in the southeastern Puna, NW Argentina, indicate two lithostratigraphic units at the eastern–northeastern border of salar Centenario: (1) a bimodal volcanosedimentary sequence affected by low- to medium-grade metamorphism, comprising metasediments associated with basic and felsic metavolcanic rocks, dated 485 ± 5 Ma, and (2) a plutonic unit composed of syenogranites to quartz-rich leucogranites with U–Pb zircon ages between 462 ± 7 and 475 ± 5 Ma. Felsic metavolcanic and plutonic rocks are peraluminous and show similar geochemical differentiation trends. They also have similar Sm–Nd isotopic compositions (TDM model ages of 1.54–1.78 Ga; εNd(T) values ranging from −3.2 to −7.5) that suggest a common origin and derivation of the original magmas from older (Meso-Paleoproterozoic?) continental crust. Mafic rocks show εNd(T) ranging from +2.3 to +2.5, indicating a depleted mantle source. The data presented here, combined with those in the literature, suggest Ordovician magmatism mainly recycles preexisting crust with minor additions of juvenile mantle-derived material.  相似文献   

17.
Mathematical models of hydrocarbon formation can be used to simulate the natural evolution of different types of organic matter and to make an overall calculation of the amounts of oil and/or gas produced during this evolution. However, such models do not provide any information on the composition of the hydrocarbons formed or on how they evolve during catagenesis.From the kinetic standpoint, the composition of the hydrocarbons formed can be considered to result from the effect of “primary cracking” reactions having a direct effect on kerogen during its evolution as well as from the effect of “secondary cracking” acting on the hydrocarbons formed.This report gives experimental results concerning the “primary cracking” of Types II and III kerogens and their modelling. For this, the hydrocarbons produced have been grouped into four classes (C1, C2–C5, C6–C15 and C15+). Experimental data corresponding to these different classes were obtained by the pyrolysis of kerogens with temperature programming of 4°C/min with continuous analysis, during heating, of the amount of hydrocarbons corresponding to each of these classes.The kinetic parameters of the model were optimized on the basis of the results obtained. This model represents the first step in the creation of a more sophisticated mathematical model to be capable of simulating the formation of different hydrocarbon classes during the thermal history of sediments. The second step being the adjustment of the kinetic parameters of “secondary cracking”.  相似文献   

18.
The behaviour of the ammonium ion in synthetic buddingtonite, N(D,H)4AlSi3O8, has been studied by infrared (IR) spectroscopy from 20 K to 298 K and by 2H NMR spectroscopy from 120 K to 298 K. IR spectra were collected from 500 to 3500 cm–1. Static 2H NMR spectra collected at 298 K and 120 K are very similar, consisting of a single sharp isotropic resonance, indicating complete averaging of quadrupolar interactions and implying that at these temperatures the ammonium ion is in rapid (<1 s) randomised motion within the M-site cavity of the feldspar framework. NMR spectroscopy indicates that the splitting of the internal modes of the ammonium ion observed by IR spectroscopy is not due to freezing in of the ammonium ion. This observation rules out the formation of a preferred N–H...O hydrogen bond, with precession of the ion about it, as proposed by Kimball and Megaw (1978), because any N–H...O hydrogen bond must be very weak and transient in nature. Contraction of the cavity site upon cooling imposes a distortion upon the ammonium ion that affects vibrational modes. This distortion does not affect the motion of the ammonium ion as observed on the NMR time-scale.  相似文献   

19.
The Semna gold deposit is one of several vein-type gold occurrences in the central Eastern Desert of Egypt, where gold-bearing quartz veins are confined to shear zones close to the boundaries of small granitoid stocks. The Semna gold deposit is related to a series of sub-parallel quartz veins along steeply dipping WNW-trending shear zones, which cut through tectonized metagabbro and granodiorite rocks. The orebodies exhibit a complex structure of massive and brecciated quartz consistent with a change of the paleostress field from tensional to simple shear regimes along the pre-existing fault segments. Textural, structural and mineralogical evidence, including open space structures, quartz stockwork and alteration assemblages, constrain on vein development during an active fault system. The ore mineral assemblage includes pyrite, chalcopyrite, subordinate arsenopyrite, galena, sphalerite and gold. Hydrothermal chlorite, carbonate, pyrite, chalcopyrite and kaolinite are dominant in the altered metaggabro; whereas, quartz, sericite, pyrite, kaolinite and alunite characterize the granodiorite rocks in the alteration zones. Mixtures of alunite, vuggy silica and disseminated sulfides occupy the interstitial open spaces, common at fracture intersections. Partial recrystallization has rendered the brecciation and open space textures suggesting that the auriferous quartz veins were formed at moderately shallow depths in the transition zone between mesothermal and epithermal veins.Petrographic and microthermometric studies aided recognition of CO2-rich, H2O-rich and mixed H2O–CO2 fluid inclusions in the gold-bearing quartz veins. The H2O–CO2 inclusions are dominant over the other two types and are characterized by variable vapor: liquid ratios. These inclusions are interpreted as products of partial mixing of two immiscible carbonic and aqueous fluids. The generally light δ34S of pyrite and chalcopyrite may suggest a magmatic source of sulfur. Spread in the final homogenization temperatures and bulk inclusion densities are likely due to trapping under pressure fluctuation through repeated fracture opening and sealing. Conditions of gold deposition are estimated on basis of the fluid inclusions and sulfur isotope data as 226–267 °C and 350–1100 bar, under conditions transitional between mesothermal and epithermal systems.The Semna gold deposit can be attributed to interplay of protracted volcanic activity (Dokhan Volcanics?), fluid mixing, wallrock sulfidation and a structural setting favoring gold deposition. Gold was transported as Au-bisulfide complexes under weak acid conditions concomitant with quartz–sericite–pyrite alteration, and precipitated through a decrease in gold solubility due to fluid cooling, mixing with meteoric waters and variations in pH and fO2.  相似文献   

20.
We have studied the paleomagnetism of the middle Cretaceous Iritono granite of the Abukuma massif in northeast Japan together with 40Ar–39Ar dating. Paleomagnetic samples were collected from ten sites of the Iritono granite (102 Ma 40Ar–39Ar age) and two sites of its associated gabbroic dikes. The samples were carefully subjected to alternating field and thermal demagnetizations and to rock magnetic analyses. Most of natural remanent magnetizations show mixtures of two components: (1) H component, high coercivity (Bc > 50–90 mT) or high blocking temperature (Tb > 350–560 °C) component and (2) L component, relatively low Bc or low Tb component. H component was obtained from all the 12 sites to give a mean direction of shallow inclination and northwesterly declination (I = 29.9°, D = 311.0°, α95 = 2.7°, N = 12). This direction is different from the geocentric axial dipole field at the present latitude (I = 56.5°) and the typical direction of the Cenozoic remagnetization in northeast Japan. Since rock magnetic properties indicate that the H component of the Iritono granite is carried mainly by magnetite inclusions in plagioclase, this component probably retains a primary one. Thus the shallow inclination indicates that the Abukuma massif was located at a low latitude (16.1 ± 1.6°N) about 100 Ma and then drifted northward by about 20° in latitude. The northwesterly deflection is attributed mostly to the counterclockwise rotation of northeast Japan due to Miocene opening of the Japan Sea. According to this model, the low-pressure and high-temperature (low-P/high-T) metamorphism of the Abukuma massif, which has been well known as a typical location, would have not occurred in the present location. On the other hand, the L component is carried mainly by pyrrhotite and its mean direction shows a moderate inclination and a northwesterly declination (I = 42.8°, D = 311.5°, α95 = 3.3°, N = 9). Since this direction is intermediate between the H component and early Cenozoic remagnetization in northeast Japan, some thermal event would have occurred at lower temperature than pyrrhotite Curie point ( 320 °C) during the middle Cretaceous to early Cenozoic time to have resulted in partial remagnetization.  相似文献   

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