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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.  相似文献   

2.
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   

3.
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   

4.
Two comparative simulation experiments(a normal atmospheric-pressure opening system and a 20 MPa closed system)were conducted to study the geochemical evolution of n-alkane,sterane,and terpane biomarkers in the process of oil cracking into gas under different pressures.With an initial experimental temperature set at 300°C,the temperature was increased to 650°C at a heating rate of 30°C/h.The products were tested every 50°C starting at 300°C,and a pressure of 20 MPa was achieved using a water column.The low-maturity crude oil sample was from the Paleogene system in the Dongying sag in eastern China.The threshold temperature obtained for the primary oil cracking process in both pressure systems was 450°C.Before the oil was cracked into gas,some components,including macromolecular n-alkanes,were cracked into medium-or small-sized n-alkanes.The secondary oil cracking of heavy hydrocarbon gases of C2–5to methane mainly occurred between 550°C to 650°C,and the parameters Ln(C1/C2)and Ln(C1/C3),as well as the dry coefficients,increased.Overpressure inhibited the oil cracking process.In the 20 MPa system,the oil conversion rate decreased,the temperature threshold for gas generation rose,and oil cracking was inhibited.Compared with the normal pressure system,high-carbon n-alkanes and other compounds in the 20 MPa pressure system were reserved.Furthermore,the parameters∑C21-/∑22+,Ln(C1/C2),and Ln(C1/C3),as well as the dry coefficients,decreased within the main temperature range.During secondary oil cracking(550°C to 600°C),the Ph/nC18and Pr/nC17decreased.High pressure influenced the evolution of the biomarkers Ts and Tm,C31homohopane,C29sterane,and their related maturity parameters to different extents during oil cracking under different temperature ranges.  相似文献   

5.
By the aid of GC-MS technique, a series of sequentially biodegraded oils from Liaohe Basin have been analyzed. The results show that the concentrations and relative compositions of various aromatic compounds in the biodegraded crude oils will change with increasing biodegradation degree. The concentrations of alkyl naphthalenes, alkyl phenanthrenes, alkyl dibenzothiophene are decreased, and the concentration of triaromatic steroids will increase with increasing biodegradation degree in biodegraded oils. Those phenomena indicate that various aromatic compounds are more easily biodegraded by bacteria like other kinds of hydrocarbons such as alkanes, but different series of aromatic compounds have a varied ability to resistant to biodegradation. The ratios of dibenzothiophene to phenenthrene (DBTH/P) and methyl dibenzothiophene to methyl phenanthrene (MDBTH/MP) are related to the features of depositional environment for source rocks such as redox and ancient salinity. However, in biodegraded oils, the two ratios increase quickly with the increase of the biodegradation degree, indicating that they have lost their geochemical significance. In this case, they could not be used to evaluate the features of depositional environment. Methyl phenanthrene index, methyl phenanthrene ratio and methyl dibenzoyhiophene ratio are useful aromatic maturity indicators for the crude oils and the source rocks without vitrinite. But for biodegraded oils, those aromatic maturity indicators will be affected by biodegradation and decrease with the increase of the biodegradation degree. Therefore, those aromatic molecular maturity indicators could not be used for biodegraded oils.  相似文献   

6.
Source rock extracts and crude oils from the Songliao Basin were analyzed by high-temperature gas chromatography (HTGC), gas chromatography-mass spectrometry (HTGC-MS) and gas chromatography-isotope ratio-mass spectrometry (GC-IRMS), for high molecular-weight alkanes. The distributions of n-alkanes in the Nenjiang Formation extracts are in the C14―C63 range; a bimodal distribution occurs in the C-21 and C21―40 regions. The C30―C37 n-alkanes are accompanied by C29―C35 hopanes, whereas the high molecular-weight C45―C47 n-alkanes co-occur with abundant isoalkanes, alkylcyclohexanes and alkylcyclopentanes. The high δ 13C values of the n-alkanes and the microscopic maceral compositions indicate a highly diversified organic source input for the Nenjiang Formation source rocks, ranging from aquatic plants, blue alge-bacteria, to land plant material. In contrast, n-alkanes in the rock extracts of the Qingshankou Formation are characterized by a single modal distribution, with relatively low abundances of C29―C35 hopanes, but high molecular-weight isoalkanes, alkylcyclohexanes and alkylcyclopentanes. The relatively low δ 13C values of C22―C44 n-alkanes and organic material compositions indicate that the source rocks in the Qingshankou Formation contain dominantly type I algal organic matter. The relative abundance of C 40 compounds in source rocks changes little at low maturity stage, but decreases drastically at higher maturity levels, with a concurrent reduction in the odd/even carbon predominance. In crude oils, in contrast, the relative abundance of C 40 compounds appears to relate closely with the oil source and oil viscosity.  相似文献   

7.
Oils, condensates and natural gases in the Kekeya Field, southeast depression of the Tarim Basin were studied for their geochemical characteristics. According to the distribution analysis of the C2/C3 values with C1/C2 values, C2/C3 values with C1/C3 values, as well as C2/C3 values with dryness index, there are two different types of natural gases in the studied field, which are spatially regularly distributed. One is the oil cracking gas, located on shallow reservoirs over X 5 2 reservoir, namely Upper oil legs; the other is kerogen cracking gas, located on X 7 2 reservoirs, X8 reservoirs and E2 k reservoirs, namely Lower oil legs. In addition, the distribution patterns of molar concentration of oils and condensates with different carbon numbers of the n-alkanes in the Kekeya Field indicate that the crude oils have experienced several kinds of secondary alterations, which were closely related to the charging of gaseous hydrocarbons after petroleum accumulation. These results indicate that, based on the research of δ 13C values of individual hydrocarbons, heptane values and isoheptane values of light hydrocarbons and aromatic maturity parameters for oils, condensates and natural gases, oils and gases were charged at different geological time in the Kekeya Field.  相似文献   

8.

Oils, condensates and natural gases in the Kekeya Field, southeast depression of the Tarim Basin were studied for their geochemical characteristics. According to the distribution analysis of the C2/C3 values with C1/C2 values, C2/C3 values with C1/C3 values, as well as C2/C3 values with dryness index, there are two different types of natural gases in the studied field, which are spatially regularly distributed. One is the oil cracking gas, located on shallow reservoirs over X 25 reservoir, namely Upper oil legs; the other is kerogen cracking gas, located on X 27 reservoirs, X8 reservoirs and E2 k reservoirs, namely Lower oil legs. In addition, the distribution patterns of molar concentration of oils and condensates with different carbon numbers of the n-alkanes in the Kekeya Field indicate that the crude oils have experienced several kinds of secondary alterations, which were closely related to the charging of gaseous hydrocarbons after petroleum accumulation. These results indicate that, based on the research of δ 13C values of individual hydrocarbons, heptane values and isoheptane values of light hydrocarbons and aromatic maturity parameters for oils, condensates and natural gases, oils and gases were charged at different geological time in the Kekeya Field.

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9.
Study of Late Cretaceous lacustrine sedimentary strata in the eastern Songliao Basin, China revealed that the paleoclimate was relatively arid and hot during sedimentation of the upper Santonian of the Yaojia Formation, but became relatively humid and warm during deposition of the lower Campanian Nenjiang Formation. The upper Yaojia Formation was deposited in a freshwater lake environment, while the lower Nenjiang Formation was deposited in a slightly brackish to brackish environment. The average total organic carbon content in the upper Yaojia Formation is 0.15%, while the hydrogen index is 36 mgHC/gTOC, implying poor source rock for oil generation and the organic matter comprised of a mixture of woody and herbaceous organic matter. In contrast, the hydrogen index of oil shale and black shale of the lower Nenjiang Formation is 619 mgHC/gTOC, and total organic carbon content on average is 3.37%, indicating a mixed algae and herbaceous source of kerogen and an increase in aquatic bioproductivity. The black shale and oil shale have low Pristane/Phytane and C29 5α,14α,17α(H) ? stigmastane 20R/(20R + 20S) ratios, with maximum concentration of n‐alkanes at n‐C23, implying an anoxic depositional environment with algae, bacteria and higher plants providing most of the organic matter. Relatively abundant gammacerane and a higher Sr/Ba ratio in the oil shales suggest the presence of brackish water and development of salinity stratification in the lake. During sedimentation of the upper Yaojia through the lower Nenjiang Formations, the level of Songliao lake increased and a deep‐lake environment was formed with bottom waters being oxygen depleted. Concomitantly, as the lake deepened bottom conditions were changing from oxic to anoxic, and the input of organic matter changed from predominantly higher plants to a mixture of bacteria, algae and higher plants providing favorable conditions for oil source rock accumulation.  相似文献   

10.
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   

11.
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   

12.
In the processes of discrimination between oil-cracked gases and kerogen-cracked gases, Behar and Pinzgofer et al.’s results were adopted in the former researches, in which the ratio of C2/C3 is basically a constant while the ratio of C1/C2 gradually increases in the course of primary cracking of kerogen. Otherwise in the course of secondary cracking of oil, the ratio of C2/C3 increases rapidly while C1/C2 keeps relatively stable. Our study on analogue experiment shows that, whether it is oil or kerogen, in its process of gas generating by cracking, the ratios of C2/C3, C1/C2 or C1/C3 will all be increased with the growth of thermal conditions. In comparison, the ratio of C2/C3, which is affected by genetic type to some comparatively less extent, mainly responds to the maturity of gases, while the value of C2/C3 is about 2, and that of C2/iC4 is about 10, and the corresponding value of R o is about 1.5%–1.6%. The influence of gas source on C2/C3 is less than that of gas maturity, otherwise C1/C2 (or C1/C3) is obviously affected by cracking matrices. The ratios of C1/C2, C1/C3 of oil-cracked gases are less than that of kerogen-cracked gases, under the condition that the ratios of C2/C3 are similar in value, so are the value of dryness indexes. There exists wide diffidence between this view and the former discrimination method in theory. The analysis of the spot sample indicates that we can apply the above basic view to dealing efficiently with the problem of the discrimination between oil-cracked gas and kerogen-cracked gas.  相似文献   

13.
Ken  Sawada 《Island Arc》2006,15(4):517-536
Abstract Organic petrological observations of kerogen macerals and organic geochemical analyses of carbon isotopes of kerogen macerals and biomarkers were conducted on Neogene neritic sediments of the Takafu syncline area of central Japan. The Senmi, Sakainomiya and Lower Shigarami Formations in that area were deposited at the neritic provinces on the southern edge of the paleo‐Japan Sea during the Late Miocene to Early Pliocene. Sedimentary organic matter in these formations was almost terrigenous in origin. Changes in kerogen maceral compositions reflect sedimentological and tectonic histories evaluated in previous studies from sedimentary facies and paleontology. It was found that carbon isotope ratios (δ13C) of kerogen macerals increased from ?28‰ to ?25‰ from the Sakainomiya to the lower part of the Lower Shigarami Formations. The cause of that increase was presumably the expansion of C4 plants into southwest Japan. The timing was concordant with that of the expansion of C4 plant grasslands in East Asia. The oxicity (oxic to anoxic) conditions of sea bottoms evaluated from pristane/phytane ratios varied. Particularly, in the lower part of the Senmi Formation, layers in which no steroid biomarkers could be detected were found, and had presumably formed under oxic conditions when strong biodegradation had occurred. Concentrations of regular (C27–C29) steranes and dinosteranes were higher in the Sakainomiya and Lower Shigarami Formations. This indicates that dinoflagellates‐dominant primary productions were higher at those stages. In addition, concentrations of diatomaceous biomarkers such as C26 norsterane increased from the Lower Shigarami Formation, thus adding diatoms to the major producers. Furthermore, similar associations between the increases of δ13C values of kerogen macerals and concentrations of diatomaceous biomarkers were observed in the Takafu syncline area. Thus, the expansion of C4 plants was possibly associated with the high production of diatom in the shallow‐marine areas of the paleo‐Japan Sea during the Neogene Period.  相似文献   

14.
With the increasing demand for and consumption of crude oils, oil spill accidents happen frequently during the transportation of crude oils and oil products, and the environmental hazard they pose has become increasingly serious in China. The exact identification of the source of spilled oil can act as forensic evidence in the investigation and handling of oil spill accidents. In this study, a weathering simulation experiment demonstrates that the mass loss of crude oils caused by short-term weathering mainly occurs within the first 24h after a spill, and is dominated by the depletion of low-molecular weight hydrocarbons (相似文献   

15.
In the saturate fractions of crude oils from the Zhu1 and Zhu2 depressions of the Pearl River Mouth Basin,two novel C_(15) sesquiterpanes have been detected except for drimanes and rearranged drimanes.By comparison with spectra and retention times in previous studies,they have been identified as 2,2,4α,7,8-pentamethyl-trans-decalin and 2,2,4α,7,8-pentamethyl-cis-decalin,respectively,which are related to the D/Eringsof18α(H)-and18β(H)-oleanane.ResultsshowthatthenovelC15sesquiterpanesarerelativelyabundantincondensateoilsthathavehighPr/PhratiosandarerichinterrigenoustriterpanessuchasoleananeandbicadinanesfromtheZhu2depression,butevidentlylowinlacustrineoilsthathavelowPr/Phratiosandarerichin4-methylsteranesfromtheZhu1depression.ThissuggeststhatthenovelC15sesquiterpanescouldberelatedtoterrigenousorganicmatterinoriginandcanhelpdistinguishtheoriginandsourceofcrudeoilsinthestudyarea.Inaddition,thereexistcompletelydifferentcorrelationsbetweentherelativeabundancesofdifferentC15sesquiterpanesthathavedifferentsourcesandthePr/Phratio,whichindicatesredoxconditionsinthecrudeoils.Forexample,thenovelC15sesquiterpanesandcadinanethatindicateterrigenousinputarepositivelycorrelatedwiththePr/Phratio,butdrimanesandrearrangeddrimaneshavingmicrobialoriginarenegativelycorrelatedwiththePr/Phratio.ThisimpliesthattheformationofthenovelC15sesquiterpanesrequiresrelativelyoxicconditions.ThenovelC15sesquiterpanesaremuchmoreabundantincarbonaceousmudstone(Pr/Ph=7.39)thanindarkmudstone(Pr/Ph=2.19)fromtheEnpingformation,althoughtheirorganicmatterishumic.However,theyarenotcommoninsapropeliclacustrinesourcerocks(Pr/Ph=2.29)fromtheWenchangFormation.Thissuggeststhatterrigenousorganicmatterisonlyasufficientcondition,butanoxicenvironmentduringdepositionanddiagenesismaybeaprerequisitefortheformationofnovelC15sesquiterpanes.  相似文献   

16.
Since the discovery of the Tahe oilfield, it has been controversial on whether the main source rock is in the Cambrian or Middle-Upper Ordovician strata. In this paper, it is assumed that the crude oil from the Wells YM 2 and TD 2 was derived from the Middle-Upper Ordovician and Cambrian source rocks, respectively. We analyzed the biomarkers of the crude oil, asphalt-adsorbed hydrocarbon and saturated hydrocarbon in bitumen inclusions from the Lunnan and Hade areas in the North Uplift of the Tarim Basin. Results show that the ratios of tricyclic terpane C21/C23 in the crude oil, asphalt-adsorbed hydrocarbon and saturated hydrocarbon in bitumen inclusions are less than 1.0, indicating that they might be from Upper Ordovician source rocks; the ratios of C28/(C27+C28+C29) steranes in the saturated hydrocarbon from reservoir bitumen and bitumen inclusions are higher than 25, suggesting that they might come from the Cambrian source rocks, however, the ratios of C28/(C27+C28+C29) steranes in oil from the North Uplift are less than 25, suggesting that they might be sourced from the Upper Ordovician source rocks. These findings demonstrate that the sources of crude oil in the Tarim Basin are complicated. The chemical composition and carbon isotopes of Ordovician reservoired oil in the Tarim Basin indicated that the crude oil in the North Uplift (including the Tahe oilfield) and Tazhong Depression was within mixture areas of crude oil from the Wells YM 2 and TD 2 as the end members of the Cambrian and Middle-Upper Ordovician sourced oils, respectively. This observation suggests that the crude oil in the Ordovician strata is a mixture of oils from the Cambrian and Ordovician source rocks, with increasing contribution from the Cambrian source rocks from the southern slope of the North Uplift to northern slope of the Central Uplift of the Tarim Basin. Considering the lithology and sedimentary facies data, the spatial distribution of the Cambrian, Middle-Lower Ordovician and Upper Ordovician source rocks was reconstructed on the basis of seismic reflection characteristics, and high-quality source rocks were revealed to be mainly located in the slope belt of the basin and were longitudinally developed over the maximum flooding surface during the progressive-regressive cycle. Affected by the transformation of the tectonic framework in the basin, the overlays of source rocks in different regions are different and the distribution of oil and gas was determined by the initial basin sedimentary structure and later reformation process. The northern slope of the Central Uplift-Shuntuo-Gucheng areas would be a recent important target for oil and gas exploration, since they have been near the slope area for a long time.  相似文献   

17.
Biodegradation of polycyclic aromatic hydrocarbons (PAHs) in contaminated sediment is an attractive remediation technique and its success depends on biodegradation kinetics, and the optimal condition for the PAH-degrading isolates; however, information on this aspect is still scarce. The effects of multi-factors on biodegradation of phenanthrene, a 3-ring model PAH, in contaminated sediment slurry by Sphingomonas sp. a bacterial strain isolated from surface mangrove sediment, were investigated using the orthogonal experimental design (form L16(45)). The most significant factors were salinity and inoculum size, while the effects of phenanthrene concentrations, nutrient addition and temperatures were insignificant. The optimal biodegradation condition in contaminated mangrove sediment slurry was 30 °C, 15 ppt salinity, a carbon/nitrogen ratio of 100:1 (the background ratio in sediment) and an inoculum size of 106 most probable number g−1 sediment. The phenanthrene biodegradation could be best described by the first order rate model, C = C0e−kt, where k (the rate constant) is equaled to 0.1185, under the optimal condition. The kinetic model was verified and its validity in predicting biodegradation by Sphingomonas sp. at various phenanthrene concentrations was proved by experimental data.  相似文献   

18.
《Marine pollution bulletin》2009,58(6-12):895-898
Experimentally, a feasibility study for adsorption and catalytic pyrolysis of spill oils on Cu/ZSM-5 for recycling of light oils has been conducted in the present work. The adsorption and pyrolysis of model compounds such as heptane, toluene, and diesel (to stimulate the spill oils) on Cu/ZSM-5 have been investigated on a continuous fixed-bed reactor. By component fitted X-ray absorption near edge structural (XANES) spectroscopy, catalytic active species such as metallic copper (Cu) (77–84%) and Cu2O (6–7%) are found in the channels of ZSM-5 during pyrolysis of heptane or toluene. Pyrolysis of diesel effected by Cu/ZSM-5 yields gas (C1–C5) (32%) and light oil (68%) that can be used as auxiliary fuels.  相似文献   

19.
Yang  Chun  Luo  Xia  Li  Jian  Li  ZhiSheng  Liu  QuanYou  Wang  YuLin 《中国科学:地球科学(英文版)》2008,51(1):140-147

The Xushen gas field, located in the north of Songliao Basin, is a potential giant gas area for China in the future. Its proved reserves have exceeded 1000×108 m3 by the end of 2005. But, the origin of natural gases from the deep strata is still in debating. Epimetamorphic rocks as a potential gas source are widely spreading in the northern basement of Songliao Basin. According to pyrolysis experiments for these rocks in the semi-confined system, gas production and geochemistry of alkane gases are discussed in this paper. The Carboniferous-Permian epimetamorphic rocks were heated from 300°C to 550°C, with temperature interval of 50°C. The gas production was quantified and measured for chemical and carbon isotopic compositions. Results show that δ 13C1 is less than −20‰, carbon isotope trend of alkane gas is δ 13C1<δ 13C2<δ 13C3 or δ 13C1<δ 13C2>δ 13C3, these features suggest that the gas would be coal-type gas at high-over maturity, not be inorganic gas with reversal trend of gaseous alkanes (δ 13C1>δ 13C2>δ 13C3). These characteristics of carbon isotopes are similar with the natural gas from the basin basement, but disagree with gas from the Xingcheng reservoir. Thus, the mixing gases from the pyrolysis gas with coal-typed gases at high-over maturity or oil-typed gases do not cause the reversal trend of carbon isotopes. The gas generation intensity for epimetamorphic rocks is 3.0×108–23.8×108 m3/km2, corresponding to R o from 2.0% to 3.5% for organic matter.

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20.
Revealing of the sources and distributions of sedimentary organic matter in the East China Sea (ECS) is important for understanding its carbon cycle, which has significant temporal and spatial variability due to the influences of recent climate changes and anthropogenic activities. In this study, we report the contents of both terrestrial and marine biomarkers including ∑C27+C29+C31n-alkanes (38.6-580 ng/g), C37 alkenones (5.6-124.6 ng/g), brassicasterol (98-913 ng/g) and dinosterol (125-1521 ng/g) from the surface sediments in the Changjiang River Estuary (CRE) and shelf areas of the ECS. Several indices based on biomarker contents and ratios are calculated to assess the spatial distributions of both terrestrial and marine organic matter in the ECS surface sediments, and these results are compared with organic matter distribution patterns revealed by the δ13C (−20.1‰ to −22.7‰) and C/N ratio (5-7.5) of total organic matter. The contents of terrestrial biomarkers in the ECS surface sediments decrease seaward, controlled mostly by Changjiang River (CR) inputs and surface currents; while higher contents of the two marine biomarkers (brassicasterol and dinosterol) occur in upwelling areas outside the CRE and in the Zhejiang-Fujian coastal zone, controlled mostly by marine productivity. Four proxies, fTerr(δ13C) (the fraction of terrestrial organic matter in TOC estimated by TOC δ13C), odd-alkanes (∑C27+C29+C31n-alkanes), 1/Pmar-aq ((C23+C25+C29+C31)/(C23+C25) n-alkanes) and TMBR (terrestrial and marine biomarker ratio) (C27+C29+C31n-alkanes)/((C27+C29+C31) n-alkanes+(brassicasterol+dinosterol+alkenones)), reveal a consistent pattern showing the relative contribution of terrestrial organic matter (TOM) is higher in the CRE and along the Zhejiang-Fujian coastline, controlled mostly by CR inputs and currents, but the TOM contribution decreases seaward, as the influences of the CR discharge decrease.  相似文献   

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