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1.

By aid of gas chromatogram/mass spectrometry (GC-MS), the distributions and the compositions of biomarkers in a set of sequentially biodegraded oils from Liaohe Basin, China, have been quantitatively analyzed, and it has been found that during the biodegradation process of crude oils, the molecular maturity parameters such as Ts/Tm, homohopane C31 22S/(22S+22R) and sterane C29 20S/(20S+20R) ratios will be affected to different extent. The results show that except homohopane C31 22S/(22S+22R) ratio, Ts/Tm ratio will decrease with increasing biodegradation, but for C29 20S/(20S+20R) ratio, it will almost remain constant in slightly and moderately biodegraded oils, and then will increase quickly in severely biodegraded oils. The main reason is that there are some differences in the ability of resistant biodegradation for different isomer of biomarkers with different stereo configuration, resulting in the fact that destroying rate by bacteria for those biomarkers with weak ability will be higher than those with strong ability in resistant biodegradation. For example, 18α(H)-22,29,30-trisnorhopanes (Ts) will be destroyed more quickly than 17α(H)-22,29,30-trisnorshopanres (Tm), and 20R isomer is more quickly than 20S isomer for C29 sterane, resulting in the relative ratios changed with increasing biodegradation. Therefore, much more attention should be paid to the biodegradation extent of crude oils and the type of biomarker maturity indicators, when the distributions and the compositions of biomarkers in biodegraded oils are used to determine the maturity of biodegraded oils.

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2.
By aid of gas chromatogram/mass spectrometry (GC-MS), the distributions and the compositions of biomarkers in a set of sequentially biodegraded oils from Liaohe Basin, China, have been quantitatively analyzed, and it has been found that during the biodegradation process of crude oils, the molecular maturity parameters such as Ts/Tm, homohopane C31 22S/(22S+22R) and sterane C29 20S/(20S+20R) ratios will be affected to different extent. The results show that except homohopane C31 22S/(22S+22R) ratio, Ts/Tm ratio will decrease with increasing biodegradation, but for C29 20S/(20S+20R) ratio, it will almost remain constant in slightly and moderately biodegraded oils, and then will increase quickly in severely biodegraded oils. The main reason is that there are some differences in the ability of resistant biodegradation for different isomer of biomarkers with different stereo configuration, resulting in the fact that destroying rate by bacteria for those biomarkers with weak ability will be higher than those with strong ability in resistant biodegradation. For example, 18α(H)-22,29,30-trisnorhopanes (Ts) will be destroyed more quickly than 17α(H)-22,29,30-trisnorshopanres (Tm), and 20R isomer is more quickly than 20S isomer for C29 sterane, resulting in the relative ratios changed with increasing biodegradation. Therefore, much more attention should be paid to the biodegradation extent of crude oils and the type of biomarker maturity indicators, when the distributions and the compositions of biomarkers in biodegraded oils are used to determine the maturity of biodegraded oils.  相似文献   

3.
A suite of crude oil samples,that had not been previously characterized geochemically,was collected from two oil fields in the southwest Niger Delta Nigeria.The saturate biomarkers were used to evaluate geochemical characteristics such as depositional environments,sources of organic matter and extent of biodegradation using gas chromatography-flame ionization detector and gas chromatography-mass spectrometry.Distribution of n-alkanes(Pr/Ph,and isoprenoide/n-alkanes ratios),the abundance of hopanes,oleanane skeleton and C27-C29 steranes in the oils indicate that they were formed from mixed sources(marine and terrestrial kerogen) deposited in an oxic paleoenvironment with no particular maturity trend.These parameters also permit the source grouping of the oils into two families.  相似文献   

4.
Crude oil hydrocarbon composition characteristics and oil viscosity prediction are important bases in petroleum exploration.A total of 54 oil/heavy-oil samples and 17 oil sands were analyzed and quantified using both comprehensive 2D gas chromatography(GC×GC)and comprehensive 2D gas chromatography/time-of-flight mass spectrometry(GC×GC/TOFMS).The results show that crude oil in the West slope is mainly heavy oil and its hydrocarbon composition is characterized overall by paraffinsmono-aromaticsnaphthenesnon-hydrocarbonsdi-aromaticstri-aromaticstetra-aromatics.Aromatics are most abundant and non-hydrocarbons are least abundant,whilst content differences among paraffins,naphthenes,aromatics,and non-hydrocarbons are less than 15%.There are two types of heavy oil,secondary type and mixing type.Biodegradation is the main formation mechanism of heavy oil.Biodegradation levels cover light biodegradation,moderate biodegradation,and severe biodegradation.With increasing biodegradation,paraffin content decreases while contents of aromatics and nonhydrocarbons increase.In contrast,naphthene content increases first and then decreases with increasing biodegradation.In severe biodegradation stage,naphthenes decrease more quickly than aromatics and non-hydrocarbons.This provides a new method for studying oil/heavy-oil biodegradation mechanism and biodegradation resistance of different hydrocarbons at different biodegradation stages.In the Longhupao-Daan terrace and Qijia-Gulong depression,most crude oil is conventional oil.Its composition is dominated by paraffins with the lowest content of aromatics.In some casual oil wells from the Longhupao-Daan terrace,crude oil from Saertu oil reservoirs is moderately biodegraded whereas crude oil from Putaohua oil reservoir is lightly biodegraded.Chemical parameters using saturate hydrocarbons and aromatics are usually not suitable for determining organic type and thermal maturity of biodegraded oil,especially of moderately or severely biodegraded oil,whilst Ts/(Ts+Tm)ratio can be used to determine thermal maturity of both conventional crude oil and heavy oil.  相似文献   

5.
The distribution, the relative composition, and their variation of methylated chromans (MTTC) with maturation of organic matter in the source rocks from Mingjia 1 well, Jianghan hypersaline basin, have been analyzed and studied. There is a close relationship between the distribution of methylatd chromans and paleosalinity of depositional environment. In the Eq 1–Eq 3 source rocks deposited under hypersaline environment with lower Pr/Ph ratio, higher gammacerane index and abundant organic sulfur-containing compounds, methyl MTTC and dimethyl MTTC are main components, but in the Eq 4 source rocks deposited non-hypersaline environment with relatively higher Pr/Ph ratio, lower gammacerane index and organic sulfur-containing compounds, trimethyl MTTC is a major compound in methylate chromans. Obviously, the distributions and the compositions of methylated chromans in the source rocks are in harmony with biomarker indicators indicating the paleaosalinity and redox of depositional environment. The relationship between the ratio of 5,8-dimethyl MTTC to 7,8-dimethyl MTTC (dimethyl MTTC ratio) and the maturity of organic matter in the source rocks from Mingjia 1 well has been discussed. The results show that dimethyl MTTC ratio increased with the burial depth and the maturation of organic matter in the source rocks, especially in immature level. It is noteworthy that this ratio is very susceptible to small variation in the maturity of organic matter in the source rocks when vitrinite reflectance R o is less than 0.65%. It may imply that this ratio is a good and susceptible aromatic maturity indicator for the relative maturity of organic matter in immature source rocks.  相似文献   

6.
Aromatic hydrocarbons are generally main distillation of crude oil and organic extract of source rocks. Bicyclic and tricyclic aromatic hydrocarbons can be purified by two-step method of chromatography on alumina. Carbon isotopic composition of individual aromatic hydrocarbons is affected not only by thermal maturity, but also by organic matter input, depositional environment, and hydrocarbon generation process based on the GC-IRMS analysis of Upper Ordovician, Lower Ordovician, and Cambrian source rocks in different areas in the Tarim Basin, western China. The subgroups of aromatic hydrocarbons as well as individual aromatic compound, such as 1-MP, 9-MP, and 2,6-DMP from Cambrian-Lower Ordovician section show more depleted 13 C distribution. The 13 C value difference between Cambrian-Lower Ordovician section and Upper Ordovician source rocks is up to 16.1‰ for subgroups and 14‰ for individual compounds. It can provide strong evidence for oil source correlation by combing the 13 C value and biomarker distribution of different oil and source rocks from different strata in the Tarim Basin. Most oils from Tazhong area have geochemical characteristics such as more negative 13C9-MP value, poor gammacerane, and abundant homohopanes, which indicate that Upper Ordovician source rock is the main source rock. In contrast, oils from Tadong area and some oils from Tazhong area have geochemical characteristics such as high 13C9-MP value, abundant gammacerane, and poor homohopanes, which suggest that the major contributor is Cambrian-Lower Ordovician source rock.  相似文献   

7.
It is a challenge to determine the source and genetic relationship of condensate, waxy and heavy oils in one given complicated petroliferous area, where developed multiple sets of source rocks with different maturity and various chemical features.The central part of southern margin of Junggar Basin, NW China is such an example where there are condensates, light oils, normal density oils, heavy crude oils and natural gases. The formation mechanism of condensates has been seriously debated for long time;however, no study has integrated it with genetic types of waxy and heavy oils. Taking the central part of southern margin of Junggar Basin as a case, this study employs geological and geochemical methods to determine the formation mechanism of condensates,waxy and heavy oils in a complicated petroliferous area, and reveals the causes and geochemical processes of the co-occurrence of different types of crude oils in this region. Based on detailed geochemical analyses of more than 40 normal crude oils, light oils,condensates and heavy oils, it is found that the condensates are dominated by low carbon number n-alkanes and enriched in light naphthenics and aromatic hydrocarbons. Heptane values of these condensates range from 19% to 21%, isoheptane values from1.9 to 2.1, and toluene/n-heptane ratios from 1.5 to 2.0. The distribution of n-alkanes in the condensates presents a mirror image with high density waxy crude oils and heavy oils. Combined with the oil and gas-source correlations of the crude oils, condensates and natural gas, it is found that the condensates are product of evaporative fractionation and/or phase-controlled fractionation of reservoir crude oils which were derived from mature Cretaceous lacustrine source rocks in the relatively early stage. The waxy oils are the intermediate products of evaporative fractionation and/or phase-controlled fractionation of reservoir crude oils, while the heavy oils are in-situ residuals. Therefore, evaporative fractionation and/or phase-controlled fractionation would account for the formation of the condensate, light oil, waxy oil and heavy oil in the central part of southern margin of Junggar Basin, resulting in a great change of the content in terms of light alkanes, naphthenics and aromatics in condensates, followed by great uncertainties of toluene/n-heptane ratios due to migration and re-accumulation. The results suggest that the origin of the condensate cannot be simply concluded by its ratios of toluene/n-heptane and n-heptane/methylcyclohexane on the Thompson's cross-plot, it should be comprehensively determined by the aspects of geological background, thermal history of source rocks and petroleum generation,physical and chemical features of various crude oils and natural gas, vertical and lateral distribution of various crude oils in the study area.  相似文献   

8.
Organosulfur compounds of crude oils and light oils (condensates), collected from ten Chinese petroleumbearing basins and representing different sedimentary environments, were analyzed and identified using a newly-developed GC-AED technique. The results show that the distributions of organosulfur compounds of crude oils from different sedimentary environments are of obvious difference. The crude oils from marine carbonates are rich in organosulfur compounds and those from the source rocks in an ocean-land interchanging facies and a littoral facies have a high abundance of organosulfur compounds, while no or less organosulfur compounds of crude oils from a fresh-water lacustrine facies and a swamp facies were detected in the detectable abundance range of the instrument. This analysis gives a new effective method for oil-source correlation. We also tried to relate the various parameters of benzothiophenic compounds of crude oils with the methane carbon isotope of associated natural gases to discuss the thermoevolutionary degree of crude oils and natural gases.  相似文献   

9.
The spatial distribution and fate of petrogenic and pyrogenic hydrocarbons in coastal sediments following the Aegean Sea oil spill (Galicia, NW Spain) was investigated through a detailed study of chemical markers. Alkanes and acyclic isoprenoid hydrocarbons were degraded within six months of the accident, but triterpane and sterane distributions were still detectable and were useful in monitoring, respectively, the oil source and weathering. Aromatic steranes were also useful source indicators, and oil degradation was clear from the decrease of certain alkyl dibenzothiophene and phenanthrene isomers. The pyrogenic polycyclic aromatic hydrocarbons produced in the tanker wreck were found more persistent than the petrogenic ones. However, the presence of the oil in the sediments was recognized even one year after the accident and was found particularly preserved in the subsurface layers.  相似文献   

10.
Oils from two lacustrine rift basins in east China are thoroughly investigated using geochemical method to understand controls on alkylphenol occurrence and distribution in oils. Oils in the Lujiapu Depression, Kailu Basin are derived from the Cretaceous source rocks, and those in the Dongying De- pression, Bohai Bay Basin, from the Tertiary source rocks. All oils are experienced relatively short distance of migration and have similar maturity in each basin. Differences in homologue distributions from different oilfields are most likely caused by organic facies variation of source rocks. The oils in the Lujiapu Depression are characterized by high proportion of C3 alkylphenols (prefixes refer to the number of alkylcarbons joined to the aromatic ring of the phenol molecule) and low proportion of cre- sols and C2 alkylphenols compared to oils from the Dongying Depression. Alkylphenol isomer distri- bution is possibly affected by depositional environment especially for C3 alkylphenols. Dysoxic fresh- water environment is favorable for the formation of propyl or isopropyl substituted C3 alkylphenols, while highly reducing saline water is more suitable for trimethyl substituted C3 alkylphenols. Variations in alkylphenol concentrations within a petroleum system are controlled mainly by secondary migration processes with alkylphenol concentrations decreasing along migration direction. Interestingly, coupled with geological factors, a subtle change of alkylphenol concentrations can be applied to differentiate carrier systems. When oil migrates through sandy beds, concentrations of total alkylphenols decrease dramatically with migration distance, while such change is less significant when oil migrates vertically along faults. However, most isomer ratios potentially related to migration distance are not as effective as those alkylcarbazoles in migration diagnosis due to complicated affecting factors.  相似文献   

11.
Hydrocarbon distributions in sediment from the Severn Estuary can be explained mainly in terms of a pollutant origin. The aliphatic hydrocarbon distribution is similar to that found in biodegraded crude oils. The distribution of polycyclic aromatic hydrocarbons, including the carcinogen benzo(a)pyrene, is similar to that derived from the pyrolysis of fossil fuels, especially petroleum.  相似文献   

12.
Elevated concentrations of polycyclic aromatic hydrocarbons (PAHs) have been found in mangrove sediments due to anthropogenic pollution, and microbial degradation has been suggested as the best way to remove PAHs from contaminated sediments. The degradation of phenanthrene, a model PAH compound by bacteria, either the enriched mixed culture or individual isolate isolated from surface mangrove sediments was examined. The effects of salinity, initial phenanthrene concentrations and the addition of glucose on biodegradation potential were also investigated. Results show that surface sediments collected from four mangrove swamps in Hong Kong had different degree of PAH contamination and had different indigenous phenanthrene-degrading bacterial consortia. The enriched bacteria could use phenanthrene as the sole carbon source for growth and degrade this PAH compound accordingly. A significant positive relationship was found between bacterial growth and percentages of phenanthrene degradation. The phenanthrene biodegradation ability of the enriched mixed bacterial culture was not related to the degree of PAH contamination in surface sediments. The growth and biodegradation percentages of the enriched mixed culture were not higher than that of the individual isolate especially at low salinity (0 and 10 ppt). High salinity (35 ppt) inhibited growth and biodegradation of phenanthrene of a bacterial isolate but less inhibitory effect was found on the mixed culture. The inhibitory effects of salinity could be reduced with the addition of glucose.  相似文献   

13.
Wang C  Du J  Gao X  Duan Y  Sheng Y 《Marine pollution bulletin》2011,62(11):2469-2475
With its close proximity to Shengli Oilfield, China’s second largest oilfield, the Yellow River Delta is at high risk for crude oil contamination. The massive oil discharge in oilfield may offer a chance for a natural experiment to investigate compositional changes of oil residues and study the stability of source- and weathering-dependent molecular parameters in oil residues after spills. The results demonstrate that the conventional diagnostic ratios, such as C2920S/(20S + 20R), C29/C30H, C30βα/αβ, C3122S/(22S + 22R), C2-DBTs/C2-PHENs, C3-DBTs/C3-PHENs, DBT/MCHRY, CHRY/PHENs, are also valid for oil source identification even after extensive weathering of spilled oils in terrestrial environment, although some exceptions were encountered for extensively weathered sample. Moreover, the ratios of selected specific biomarkers (the oleanane index, the gammacerane index) have been developed and assessed as source indicators. Finally, we find that some maturity parameters based on alkyl naphthalenes and methyl phenanthrenes in petroleum geochemistry, such as the methylnaphthalene ratios (TMNr, TeMNr, PMNr), the methylphenanthrene ratios (MPI-1, MPDF), can be applied for the source identification and correlation at their lightly to moderately weathered stage.  相似文献   

14.
Svetlana  Yessalina  Noriyuki  Suzuki  Hiroyuki  Saito 《Island Arc》2006,15(3):292-303
Abstract   The Sagara oil field is located in the Neogene Kakegawa Basin, close to the Izu collision zone at the junction between the main Japanese Islands and the Izu–Bonin Arc. The Sagara oil field is one of the few oil fields situated in a forearc basin on the Pacific side of Japan and is present in a sedimentary basin with poor oil-generating potential. Several crude oils from Sagara oil field were investigated to infer their origin. Organic geochemical characteristics of Sagara oils showed the influences of light biodegradation, migration-contamination, and migration-fractionation. The maturity levels of Sagara oils evaluated based on abundant alkylnaphthalenes corresponded to 0.9–1.2% vitrinite reflectance. Sagara oils were characterized by significant amounts of higher plant biomarkers, a high pristane/phytane ratio and an absence of organic sulphur compounds, suggesting a siliciclastic source rock deposited under nearshore to fluvial–deltaic environments. Numerous faults and fractures in the active forearc basin provided excellent conduits and facilitated upward migration of light hydrocarbons generated at greater depth in the Kakegawa Basin.  相似文献   

15.
Our study examined the effects of Corexit 9500 and sediment on microbial mineralization of specific aliphatic and aromatic hydrocarbons found in crude oil. We also measured gross mineralization of crude oil, dispersed crude oil and dispersant by a marine microbial consortium in the absence of sediment. When provided as carbon sources, our consortium mineralized Corexit 9500 the most rapidly, followed by fresh oil, and finally weathered oil or dispersed oil. However, mineralization in short term assays favored particular components of crude oil (2-methyl-naphthalene > dodecane > phenanthrene > hexadecane > pyrene) and was not affected by addition of nutrients or sediment (high sand, low organic carbon). Adding dispersant inhibited hexadecane and phenanthrene mineralization but did not affect dodecane and 2-methyl-naphthalene mineralization. Thus, the effect of dispersant on biodegradation of a specific hydrocarbon was not predictable by class. The results were consistent for both high and low oiling experiments and for both fresh and weathered oil. Overall, our results indicate that environmental use of Corexit 9500 could result in either increases or decreases in the toxicity of residual oil through selective microbial mineralization of hydrocarbons.  相似文献   

16.
Routine GC/MS analysis may apply to the volatilized Low-Molecular-Weight compounds in saturate and aromatic hydrocarbon fractions;thus,relative studies using this technique inevitably bring about some limitations on distribution of miscellaneous sulfur atom.In this article,Fourier Transform Ion Cyclotron Resonance Mass Spectrometry(FT-ICR MS)with high resolution is employed to investigate the distribution of organic sulfur compounds(OSCs)in the crude oil typically derived from the Eogene carbonate-evaporite sediments with further chemical compositional characterization in molecular level by miscellaneous atomic type,carbon number,and double bond equivalent(DBE).A variety of miscellaneous atomic types with S1,S2,S3,OS,OS2,O2S,O2S2,NS,and NOS etc.(S1 means those OSCs with one sulfur atom in a molecule)were identified in OSCs in these oil samples.High levels of alkyl thioether series compounds with one ring structure were presented mainly in the crude oil in the Jianghan Basin whereas high amounts of benzothiophene,dibenzothiophene etc.compounds with higher values in DBE and carbon number range occurred in the sulfur-rich heavy oil in the Jinxian Sag.Although carbonate-evaporite sediments deposited in the saline lacustrine facies in the Eogene basin both occurred in the Jinxian Sag and Jianghan Basin,obviously,they possess different chemical diagenetic pathway of sulfur under various microbial reactions,leading to diverse distributional characteristics on biomarkers,OSCs,and even different hydrocarbon generation mechanism of immature crude oil.  相似文献   

17.
The formation mechanisms of biphenyl series and benzonaphthothiophene series are investigated by means of simulation experiment. Biphenyl series are likely formed in two ways: one is the aromatization of the chain compounds containing conjugated C== C double bonds or the compounds with such a kind of sidechains, and the other is the reaction of sulfur with ordinary chain compounds, in which sulphur acts on ordinary sidechain compounds by seizing some hydrogens and forming (H2S and) the intermediates with conjugated C== C double bonds first, and then the intermediates are aromatized. One of the basic precursors of benzonaphthothiophenes is likely the phenylnaphthalenes which may originate from the chain compounds containing conjugated C== C double bonds, the compounds with such sidechains and saturate or unsaturate chain compounds. Thermal stability of biphenyls is high, but they can become dibenzothiophenes and polycyclic aromatic hydrocarbons or dibenzofurans and polycyclic aromatic hydrocarbons respectively in the presence of sulphur or oxygen. The ratio of biphenyl and m-biphenyl to biphenyls may be employed to indicate the depositional environment in the mild to medium maturation, of which the higher value indicates a fresh water depositional environment and the lower indicates a saline depositional environment. The relative high content of benzonaphthothiophenes in the crude oil indicates that the crude oil has undergone an intense sulfurization in the source rock or reservoir.  相似文献   

18.
Aromatic hydrocarbon fractions isolated from sediments polluted with crude oil, from sampling stations in and around Sullom Voe, Shetland Islands, were found to exhibit, as the major feature in their gas chromatograms, an unresolved complex mixture or ‘hump’. This feature was absent from the gas chromatograms of the aromatic hydrocarbon fractions isolated from corresponding unpolluted sediments in the region. The observed aromatic hump had little resemblance to the distribution of aromatic hydrocarbons in a typical North Sea crude oil. Incubation studies, however, showed that such a hump was appearing when oil-spiked sediments were aerobically biodegraded. From these incubation studies it was also evident that alkylaromatic hydrocarbons in the crude oil were biodegraded before any change in the normal alkanes was apparent. Therefore, the presence of an unresolved complex mixture in the gas chromatograms of aromatic hydrocarbon fractions from recent sediments can act as a marker to recognize contamination by crude oil.  相似文献   

19.
The crude oils typically from the CambrianLower Ordovician source rocks of Tarim Basin, NW"China, such as TD2 and TZ62S, are13C-enriched with the stable carbon isotopic ratios(VPDB) approaching-28 %.In this paper, the main research viewpoints on this issue are summarized, and combined with results from organic and inorganic carbon isotope stratum curves of the outcrop at the Ya'erdang Mountain in Tarim Basin. In addition, more alternative interpretations are discussed. On one hand, the inverse fractionation features of stable carbon and hydrogen isotopes of these crude oils may imply their protogenous nature. On the other hand, the anisotropy of source rocks and contribution from older stratum source rocks need verifying as well. For the sake of the final resolution of this issue, some further study topics are recommended.  相似文献   

20.
Crude oil bioremediation field experiment in the Sea of Japan   总被引：4，自引：0，他引：4  
Experimental bioremediation of crude oil was conducted for approximately 3 months in the intertidal zone of the Sea of Japan, Hyogo Prefecture. Artificial mixtures of weathered Arabian light crude oil and sand taken from the experimental site were wrapped in polyester net envelopes. The envelopes were placed in drum-shaped acrylic vessels with perforated sides to facilitate seawater exchange. The vessels were laid in the intertidal area. Slow release nitrogen and phosphorus synthetic fertilizer granules were added to the oil-sand mixtures in three different amounts. Some oil-sand mixtures were unfertilized controls. The oil-sand mixtures were periodically sampled and changes in the composition of the residual oils were monitored. Oil samples were subjected to gas chromatography coupled with mass spectrometry for analysis of some representative semi-volatile aliphatic and aromatic compounds. All values for each analyte were normalized against that of hopane to evaluate the extent of oil biodegradation. Significant increases in the concentrations of both nitrogen and phosphorus were found in the fertilized sections in accordance with the amounts of added fertilizers. Although significant natural attenuation of oil was observed in the unfertilized sections, fertilization stimulated the degradation rate of the oil in the early stage of the experimental term. The extent of the oil biodegradation increased as the amount of added fertilizer increased. However, the final degradation efficiencies for each oil component in the fertilized sections were not significantly different from those in the unfertilized sections, and the degradation of each oil component had almost ceased after 6 weeks. We conclude that excessive amounts of macronutrients are required to accelerate oil biodegradation and that fertilization is only effective in the early stages.  相似文献   

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