首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 15 毫秒
1.
详细研究了吉林伊通地堑下第三系生油岩和原油中的芳烃生物标志物,包括常规的多环芳烃,以及丰富的来源于高等植物的芳香二萜和芳构化的五环三萜。目前,原油中芳构化五环三萜类生物类生物标志物国内外均尚报道极少。还详细讨论了利用原油中最新发现的芳构化五环三萜在解决本区生物输入,油源对比以及石油成因等方面的重要意义。  相似文献   

2.
The molecular distributions of homologous aliphatic lipid compounds (n-alkanes, n-alkanoic acids, n-alkanols, n-alkanals and n-alkan-2-ones) were investigated in sediments of Lake Bera, Malaysia as well as in plant waxes from the vicinity using gas chromatography-mass spectrometry. In addition, triterpenoids of the oleanane, ursane, lupane and friedelane series, and their diagenetic products were also identified. Using the aquatic proxy Paq, it was found that the n-alkanes present in surface sediments S1, S5 and S6 correspond to an input from emergent macrophytes, whereas in sediments collected from open water (S2, S3 and S4) they correspond to input from submerged/floating macrophytes. The presence of n-alkan-2-ols, a commonly found homologous series in the sediments as well as in the plant wax, is novel here. In addition, the presence of 24-methylcycloart-22-enol and 24-ethylcycloart-22-enol in sediments as well as the plant wax of Pandanus helicopus, a dominant reed around the lake, also supports the input of plant biomarkers to the sediments. The occurrence of 5-membered ring triterpenoid derivatives as major diagenetic products of the triterpenoids identified (e.g. friedelan-2,3-dione) shows that the degradation of the organic matter in the sediments occurs mainly under oxic conditions. Also, the presence of ring-A degraded triterpenoids (dihydroputranjivic acid, 3-nor-2,4-seco-friedelane, 4α- and 4β-3-norfriedelanes, A-norfriedel-10-one, and A-norfriedel-8-en-10-one) and the aromatized triterpenoid hydrocarbons (mono- and triaromatic derivatives) as minor diagenetic products indicates photochemical and microorganism-mediated alteration reactions of natural products in the sediments. Additional novel polyfunctional friedelane derivatives, namely friedelane-2,3-dione, friedelane-1,3-diol-2-one and friedel-1(10)-ene-1,3-diol-2-one were identified for the first time in this study. These novel polyfunctional triterpenoids were inferred to derive from the oxidation of the triterpenoids from higher plants in this oxic tropical environment. For future reference purposes, the mass spectra of the identified polar triterpenoids are also presented here. This study provides important data on the biogeochemistry of organic matter in a tropical lake of SE Asia.  相似文献   

3.
Surface sediments from the Outer Continental Shelf of Alaska were analyzed for hydrocarbons as part of an environmental survey sponsored by NOAA/BLM. Sediments were collected from the proposed oil lease areas of Beaufort Sea, southeastern Bering Sea, Norton Sound, Navarin Basin, Gulf of Alaska, Kodiak Shelf and lower Cook Inlet. Data on normal and branched alkanes and di- and triterpenoids from capillary gas chromatography (GC) and gas chromatography-mass spectrometry (GC/ MS) indicate that the area displays little evidence of petroleum hydrocarbons (i.e., seeps) except at a few isolated stations. Beaufort Sea sediments have the highest hydrocarbon budget, whereas Kodiak Shelf sediments have the lowest. The molecular markers of the hydrocarbons are of a mixed marine autochthonous and terrestrial allochthonous origin. Norton Sound and Cook Inlet sediments contain the highest levels of terrigenous lipids and Kodiak Shelf the lowest. The abundance of alkenes implies that relatively low oxidizing conditions exist in some of the depositional areas studied, suggesting that extraneous petroleum hydrocarbons introduced into these sediments would be expected to have a relatively long residence time. The distribution of polynuclear aromatic hydrocarbons (PAH) is complex and shows a pyrolytic origin. The data on perylene strongly favor the hypothesis that it is “performed” from terrigenous precursors and transported into the marine environment with no apparent in situ generation. Polynuclear aromatic hydrocarbons of diagenetic origin are probably dominant in Gulf of Alaska and Kodiak Shelf sediments.Two stations, north of Kalgin Island, in lower Cook Inlet and one in southeastern Bering Sea show typical weathered petroleum distribution of n-alkanes and triterpenoids. Probable pathways of transport and fate of petroleum hydrocarbons in case of an oil spill are also briefly discussed.  相似文献   

4.
Analysis of the tri- and tetraaromatic hydrocarbon fractions of a brown coal sample from the Latrobe Valley, Victoria, Australia indicate the predominance of pentacyclic hydroaromatic components. Many of these have not been previously reported in the literature, but are obviously diagenetically related to triterpenoids naturally occurring in the biosphere. The components whose molecular structures have been confirmed, together with those for which tentative structural assignments are given, offer strong support for a theory of progressive diagenetic aromatization of C-3 oxygenated triterpenoids, commencing from ring A. Other compounds present in smaller amounts suggest that 1,2-methyl shift reactions also occur prior to or during aromatization. There is a notable absence of polycyclic aromatic hydrocarbons (PAH's) which can be diagenetically related to the steroid or extended-side-chain hopane skeletons.  相似文献   

5.
Analysis of aromatic hydrocarbon fractions of selected coal and shale samples reveals the predominance of two specific polyalkylnaphthalenes which have been identified as 1,2,5-trimethylnaphthalene and 1,2,5,6-tetramethylnaphthalene. The maturity of the samples is such that the source effect on the formation of individual molecules from biological precursors is expected to be recognisable. These alkylnaphthalenes are thought to be diagenetically derived from pentacyclic triterpenoids via 8,14-seco-triterpenoids, which are also detectable in some of the samples investigated. It is proposed that 1,2,5,6-tetramethylnaphthalene, in the coal samples, is formed by cleavage and methyl shift reactions from geminal C-4-methylated triterpenoids which contain a leaving group in position 3. For the shale samples, degradation of monoaromatic secohopanoids must be considered as an alternative pathway.  相似文献   

6.
《Applied Geochemistry》2006,21(6):919-940
Smoke particulate matter from grasses (Gramineae, temperate, tropical and arctic) subjected to controlled burning, both under smoldering and flaming conditions, was sampled by high volume air filtration on pre-cleaned quartz fiber filters. The filtered particles were extracted with dichloromethane/methanol and the crude extracts were methylated for separation by thin layer chromatography into hydrocarbon, carbonyl, carboxylic acid ester and polar fractions. Then, the total extract and individual fractions were analyzed by GC–MS. The major organic components directly emitted in grass smoke particles were the homologous series of n-alkanoic acids from plant lipids, n-alkanes from epicuticular wax, and sterols and triterpenols. The major natural products altered by combustion included pyrolysis products from cellulose and lignin biopolymers, and oxidation products from triterpenoids and sterols. Polycyclic aromatic hydrocarbons (PAH) were also present; however, only as minor components. Although the concentrations of organic compounds in smoke aerosols are highly variable and dependent on combustion temperature, the biomarkers and their combustion alteration products are in these cases source specific. The major components are adsorbed on or trapped in smoke particulate matter and thus may be utilized as molecular tracers in the atmosphere for determining fuel type and source contributions from grass burning.  相似文献   

7.
Shales of very low metamorphic grade from the 2.78 to 2.45 billion-year-old (Ga) Mount Bruce Supergroup, Pilbara Craton, Western Australia, were analyzed for solvent extractable hydrocarbons. Samples were collected from ten drill cores and two mines in a sampling area centered in the Hamersley Basin near Wittenoom and ranging 200 km to the southeast, 100 km to the southwest and 70 km to the northwest. Almost all analyzed kerogenous sedimentary rocks yielded solvent extractable organic matter. Concentrations of total saturated hydrocarbons were commonly in the range of 1 to 20 ppm (μg/g rock) but reached maximum values of 1000 ppm. The abundance of aromatic hydrocarbons was ∼1 to 30 ppm. Analysis of the extracts by gas chromatography-mass spectrometry (GC-MS) and GC-MS metastable reaction monitoring (MRM) revealed the presence of n-alkanes, mid- and end-branched monomethylalkanes, ω-cyclohexylalkanes, acyclic isoprenoids, diamondoids, tri- to pentacyclic terpanes, steranes, aromatic steroids and polyaromatic hydrocarbons. Neither plant biomarkers nor hydrocarbon distributions indicative of Phanerozoic contamination were detected. The host kerogens of the hydrocarbons were depleted in 13C by 2 to 21‰ relative to n-alkanes, a pattern typical of, although more extreme than, other Precambrian samples. Acyclic isoprenoids showed carbon isotopic depletion relative to n-alkanes and concentrations of 2α-methylhopanes were relatively high, features rarely observed in the Phanerozoic but characteristic of many other Precambrian bitumens. Molecular parameters, including sterane and hopane ratios at their apparent thermal maxima, condensate-like alkane profiles, high mono- and triaromatic steroid maturity parameters, high methyladamantane and methyldiamantane indices and high methylphenanthrene maturity ratios, indicate thermal maturities in the wet-gas generation zone. Additionally, extracts from shales associated with iron ore deposits at Tom Price and Newman have unusual polyaromatic hydrocarbon patterns indicative of pyrolytic dealkylation.The saturated hydrocarbons and biomarkers in bitumens from the Fortescue and Hamersley Groups are characterized as ‘probably syngenetic with their Archean host rock’ based on their typical Precambrian molecular and isotopic composition, extreme maturities that appear consistent with the thermal history of the host sediments, the absence of biomarkers diagnostic of Phanerozoic age, the absence of younger petroleum source rocks in the basin and the wide geographic distribution of the samples. Aromatic hydrocarbons detected in shales associated with iron ore deposits at Mt Tom Price and Mt Whaleback are characterized as ‘clearly Archean’ based on their hypermature composition and covalent bonding to kerogen.  相似文献   

8.
A benzene-methanol extract of an Australian Permo-Carboniferous torbanite from New South Wales was analyzed by a computerized gas chromatographic-mass spectrometric system. Acidic and neutral fractions of the extract contained C12_C27 straight chain, saturated acids; C13-C29 straight chain hydrocarbons; cyclohexyl alkanes; pentacyclic triterpanes; naphthalene, anthracene, biphenyl, benzanthracene, terphenyl, and perylene, and many methyl substituted analogs of these polycyclic aromatic systems. It is concluded that nearly all of these compounds were derived from Botryococcus braunii, a major contributor to the biomass of Australian torbanite.  相似文献   

9.
A preliminary study of newly discovered sphagnum brown coal from the Jingsuo Basin, Yunnan Province, China, which is quite rich in montan wax, indicates the predominance of highern-alkane homologues and aromatized triterpenoid components. Aromatic hydrocarbons are composed mainly of pentacyclic and tetracyclic di-, tri- and tetra-aromatic components, which are obviously diagenetically related to higher plant-derived triterpenoids naturally occurring in the biosphere. Because the sphagnum brown coal still remains in the highly immature stage, it seems that the progressive diagenetic aromatization of the higher plant-derived triterpenoids may start at a very early stage.  相似文献   

10.
Several samples of peat from 6 bogs located in southern Poland were investigated for occurrence and distribution types of biomarkers present in their extractable organic matter fraction. It was found that there are inputs from two different sources of organic compounds differing in their characteristics and origin: (1) recent immature peat organic matter deposited in situ which is the source of all polar functionalized compounds, most of n-alkanes, and acyclic isoprenoids, and (2) mature fossil fuels, most probably bituminous coals from the Upper Silesia Coal Basin of vitrinite reflectance equivalent values of 0.9–1.1%. The latter compounds were most probably transported with fly ash to bogs from nearby settlements utilizing such fuel in domestic ovens. This group includes pentacyclic triterpenoids (hopanes and moretanes), minor amounts of n-alkanes, and numerous alkyl naphthalenes and alkyl phenanthrenes. All these compounds show distributions and values of geochemical ratios characteristic for mature organic matter confirming there ex situ origin.  相似文献   

11.
Concentration of aliphatic, aromatic, and chlorinated hydrocarbons were determined from 33 surface-sediment samples taken from the Tidal Basin, Washington Ship Channel, and the Anacostia and Potomac rivers in Washington, D.C. In conjunction with these samples, selected storm sewers and outfalls also were sampled to help elucidate general sources of contamination to the area. All of the sediments contained detectable concentrations of aliphatic and aromatic hydrocarbons, DDT (total dichlorodiphenyltrichloroethane), DDE (dichlorodiphenyldichloroethene), DDD (dichlorodiphenyldichloroethane), PCBs (total polychlorinated biphenyls) and total chlordanes (oxy-, α-, and γ-chlordane and cis + trans-nonachlor). Sediment concentrations of most contaminants were highest in the Anacostia River just downstream of the Washington Navy Yard, except for total chlordane, which appeared to have upstream sources in addition to storm and combined sewer runoff. This area has the highest number of storm and combined sewer outfalls in the river. Potomac River stations had lower concentrations than other stations. Total hydrocarbons (THC), normalized to the fine-grain fraction (clay + silt, < 63 μm), ranged from 120 μg g?1 to, 1,900 μg g?1 fine-grain sediment. The hydrocarbons were dominated by the unresolved complex mixture (UCM), with total polycyclic aromatic hydrocarbons (PAHs) concentrations ranging from 4 μg g?1 to 33 μg g?1 fine-grain sediment. Alkyl-substituted compounds (e.g., C1 to C4 methyl groups) of naphthalene, fluorene, phenanthrere + anthracene, and chrysene series dominated the polycyclic aromatic hydrocarbons (PAHs). Polycyclic aromatic hydrocarbons, saturated hydrocarbons, and the unresolved complex mixture (UCM) distributions reflect mixtures of combustion products (i.e., pyrogenic sources) and direct discharges of petroleum products. Total PCB concentrations ranged from 0.075 μg g?1 to 2.6 μg g?1 fine-grain sediment, with highest concentrations in the Anacostia River. Four to six C1-substituted biphenyls were the most-prevalent PCBs. Variability in the PCB distribution was observed in different sampling areas, reflecting, differing proportion of Arochlor inputs and degradation. The concentration of all contaminants was generally higher in sediments closer to known sewer outfalls, with concentrations of total hydrocarbon, PAHs, and PCBs as high as 6,900 μg g?1, 620 μg g?1, and 20 μg g?1 fine-grain sediment, respectively. Highest PCB concentrations were found in two outfalls that drain into the Tidal Basin. Concentrations of organic contaminants from sewers draining to the Washington Ship Channel and Anacostia River had higher concentrations than sediments of the mid-channel or river. Sources of PCBs appear to be related to specific outfalls, while hydrocarbon inputs, especially PAHs, are diffuse, and may be related to street runoff. Whereas most point-source contaninant inputs have been regulated, the importance of nonpoint source inputs must be assessed for their potential addition of contaminants to aquatic ecosystems. This study indicates that in large urban areas, nonpoint sources deliver substantial amounts of contaminants to ecosystems through storm and combined sewer systems, and control of these inputs must be addressed.  相似文献   

12.
Four typical distribution patterns of pentacyclic triterpenoid hydrocarbons (types A-D) are distinguished in the low-mature source rocks from eastern China. Type A has a relatively high content of pentacyclic triterpenes. It exists in immature sediments and the distribution and abundance of triterpenes vary with the maturity of the sediments. An unknown C30 triterpene (UCT2) has also been detected in very shallow sediments. This compound is very unstable and disappears rapidly with the increase of depth. Type B is characterized by a relatively high amount of 17α(H), 21β(H)-30-homohopane. This kind of distribution pattern is common in coals and terrestrial sediments of low maturity. Type C has a relatively high content of diahopane and neohopane series. The analysis shows that this distribution pattern may have an indirect relationship with the input of higher plants despite its microbial source. There are C30-unconfirmed triterpane (UCT2) and a relatively high content of C35 hopane in type D. The dist  相似文献   

13.
The existence of polycyclic aromatic hydrocarbons in the various environments has aroused great environmental concerns due to their potential hazards to human health. The presence of polycyclic aromatic hydrocarbons in aquifer is particularly sensitive where groundwater is used as a source of potable water. Anaerobic biodegradation of polycyclic aromatic hydrocarbons is an attractive option for remediation of contaminated aquifer sediment. Bacterial and archaeal community structures of phenanthrene-degrading aquifer sediment under methanogenic condition were investigated using clone library analysis in combination with microcosm study. The bacterial members were all affiliated with ??-Proteobacteria. Phylum Euryarchaeota was the predominant archaeal group, represented by genera Methanosarcina, Methanobacterium and Thermogymnomonas. Both bacteria (genera Citrobacter and Pseudomonas) and archaea (genus Methanosarcina) might have links to phenanthrene degradation process. This work might provide some new insights into developing strategies for the isolation of the putative polycyclic aromatic hydrocarbons degraders under methanogenic condition and bioremediating polycyclic aromatic hydrocarbons in leachate-contaminated aquifer sediment.  相似文献   

14.
This study aimed to evaluate the total concentration of polycyclic aromatic hydrocarbons in sediments of Iguassu River in Southern Brazil. Alongside the concentration, the amount of such compounds bioavailable was also evaluated. This is accomplished by comparing its total amount present in sediments and the amount extracted by n-butanol. The results showed that the total concentration of polycyclic aromatic hydrocarbons presented in sediment ranged from 4.49 to 58.75???g/g. The total amount of polycyclic aromatic hydrocarbons extracted by n-butanol ranged from 1.22 to 17.07???g/g. The use of n-butanol represents the mimetic conditions that hydrocarbons, derived from oil, could be taken up by organisms. Most of the hydrocarbons extracted by n-butanol were those with lower octanol?Cwater partition constant, usually those with three and four rings. Compounds with more than four rings were extracted in lower or insignificant amounts. Even the hydrocarbons with lower molecular weight available may be degraded or eliminated by organisms, when accumulated. Estimating bioavailability of hydrocarbons represents what specific hydrocarbons could be available to be taken up by organisms.  相似文献   

15.
Volatile organic compounds with volatilities ranging between those of n-hexane and n-pentadecane were identified in open ocean and coastal marine surface water samples taken in the north central part of the Gulf of Mexico. Approximately 40 organic compounds were found. The types and concentrations of the compounds found depended upon the extent of anthropogenic and terrestrial influences. Open ocean samples consisted mostly of aromatic hydrocarbons, whereas coastal samples included alkanes, cycloalkanes, cycloalkenes, aromatic hydrocarbons, aldehydes and chlorinated hydrocarbons. Unpolluted open ocean and coastal water samples had individual concentrations rarely exceeding 5 ng/kg; some aromatic hydrocarbons approached 15 ng/kg. n-Pentadecane dominated the hydrocarbons in these samples (50–100 ng/kg). The most polluted coastal water samples had individual volatile organic concentrations as great as 150 ng/kg with total concentrations approaching 1000 ng/kg. The terpene, limonene, was found extensively in the coastal samples (up to 40 ng/kg). Photooxidization of hydrocarbons in industrial/urban atmospheres was considered as a possible source of aldehydes present in coastal water. The dynamic headspace stripping/Tenax-GC adsorption method coupled with packed column gas chromatography, and gas chromatography-mass spectrometry were used for volatile organic analysis.  相似文献   

16.
A solvent–water extraction method was proposed as an assessment tool to estimate the bioavailability of polycyclic aromatic hydrocarbons in coal–tar-contaminated soils. The approach taken was to measure the percent of polycyclic aromatic hydrocarbons extracted by a solvent–water mixture and comparing the results with the percent of polycyclic aromatic hydrocarbons degraded in a soil slurry reactor. Five soil samples from three former manufactured gas plant sites and a coal–tar disposal site which were operated between 1880 and 1947, and 1945 and 1950, respectively, in Iowa, USA were used in this study. Extraction experiments were conducted using acetone–water or ethanol–water mixtures with solvent volume fractions ranging from 1.0 to 0.4 (v/v). The percent of polycyclic aromatic hydrocarbons extracted from the various soils decreased as the volume fraction of the solvent in the solvent–water mixture was reduced. An acetone–water mixture of 0.6 was found to be appropriate in correlating the percent of polycyclic aromatic hydrocarbons degraded to the percent of polycyclic aromatic hydrocarbons extracted. For the first correlation, the percent extracted and the percent biodegraded were modified by using the molecular weights and log K ow of polycyclic aromatic hydrocarbons, respectively. For the second correlation, the equation relating the percent extracted and the percent biodegraded was modified using soil properties such as organic carbon content and percent of clay and silt. Although the experiments were conducted for a limited number of soils, the extraction method appeared to be a good starting point in estimating the bioavailability of polycyclic aromatic hydrocarbons in coal–tar-contaminated soils.  相似文献   

17.
Polycyclic aromatic hydrocarbons and polychlorinated biphenyls were investigated in sediment of bitumen deposit impacted area of Agbabu, Nigeria, to determine the present level of contamination with these toxic compounds prior to exploitation. Samples were collected during the dry season (March) and the wet season (August) of year 2008. Analysis was carried out with gas chromatography using mass spectrometry detector for polycyclic aromatic hydrocarbons and flame ionization detector for polychlorinated biphenyls. In the dry season sum of concentration of PAHs ranged from zero to 0.12 ± 0.06 ppm, while in the wet season the minimum was 0.18 ± 0.07 ppm and the maximum was 1.04 ± 0.16 ppm. Most of these values were higher than sum of polycyclic aromatic hydrocarbons concentrations of 1–10 μg/kg indicating that they were likely to come from anthropogenic sources. Average concentrations of PAHs such as naphthalene and benzo (a) pyrene obtained in sediment in the wet season in some of the stations were higher than recommended limits. The linear regression analysis between sum of concentrations and percentage organic carbon showed no significant correlation in sediment in the dry season (r2 = 0.0025) and in the wet season (r2 = 0.1345). The predominance of 4–6 ringed polycyclic aromatic hydrocarbons and the ratios between pairs of individual polycyclic aromatic hydrocarbons showed that they are likely to have come from pyrolytic sources. No polychlorinated biphenyl congener was detected in the samples.  相似文献   

18.
分子有机地球化学与古气候、古环境研究   总被引:30,自引:5,他引:30  
分子有机地球化学可以从分子级水平研究地质体中有机分子化合物的演化规律。本文报道了应用生物标志化合物指标探讨古气候和古环境,例如探讨古生物(含古植物)的输入,淡水、半咸水和高盐度水古环境的判识以及大气飘尘的来源和成因等。  相似文献   

19.
20.
In situ biotransformation of oil to methane was investigated in a reservoir in Dagang, China using chemical fingerprinting, isotopic analyzes and molecular and biological methods. The reservoir is highly methanogenic despite chemical indications of advanced oil degradation, such as depletion of n-alkanes, alkylbenzenes and light polycyclic aromatic hydrocarbon (PAH) fractions or changes in the distribution of several alkylated polycyclic aromatic hydrocarbons. The degree of degradation strongly varied between different parts of the reservoir, ranging from severely degraded to nearly undegraded oil compositions. Geochemical data from oil, water and gas samples taken from the reservoir are consistent with in situ biogenic methane production linked to aliphatic and aromatic hydrocarbon degradation. Microcosms were inoculated with production and injection waters in order to characterize these processes in vitro. Subsequent degradation experiments revealed that autochthonous microbiota are capable of producing methane from 13C labelled n-hexadecane or 2-methylnaphthalene and suggest that further methanogenesis may occur from the aromatic and polyaromatic fractions of Dagang reservoir fluids. The microbial communities from produced oil–water samples were composed of high numbers of microorganisms (on the order to 107), including methane producing Archaea within the same order of magnitude. In summary, the investigated sections of the Dagang reservoir may have significant potential for testing the viability of in situ conversion of oil to methane as an enhanced recovery method and biodegradation of the aromatic fractions of the oil may be an important methane source.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号