共查询到18条相似文献，搜索用时 171 毫秒
1.
生物降解原油中吡咯氮化合物组成的变化 总被引：1，自引：0，他引：1
渤海海域地区近50个原油样品中性氮组分的GC／MS定量分析资料表明,油藏中的生物降解作用对原油的吡咯氮化合物含量和分布有明显影响。经与同源未降解原油比较,各种烷基咔唑和苯并咔唑在3。4级中轻度降解油中就出现明显降解迹象,随生物降解程度增高其含量逐渐减少,在6—8级严重降解油中它们的总含量降低到原有的五分之一左右。在3—4级中轻度降解油中,裸露型甲基咔唑异构体更容易被微生物侵袭而代谢,抗生物降解能力按1-甲基咔唑〉4-甲基咔唑〉2-、3-甲基咔唑顺序递减;当降解程度更高时,这些化合物降解速率相当,1-／4-MCA等比值相对稳定。低-中等降解阶段,不同类型二甲基咔唑异构体的抗生物降解能力也存在明显差异性,呈屏蔽型〉半屏蔽型〉裸露型降低;在生物降解水平进一步增高时,这些异构体之间的相对含量变化不大。生物降解作用对苯并咔唑系列化合物分布的影响具有不确定性,且随降解程度的增加变得更为显著,降解油中【a】／[c】苯并咔唑比值或增高或降低。生物降解原油中吡咯氮化合物的组成变化,使降解油的二次运移示踪面临新的问题。 相似文献
2.
生物降解作用对储层抽提物中多甲基取代萘分布的影响 总被引：5，自引：0，他引：5
对辽河盆地冷东油田冷43块沙三段油藏3口取心井岩心抽提物进行了详细的地球化学分析, 族组成和饱和烃生物标志物分布显示油藏遭受了不同程度生物降解作用的影响, 降解程度由油柱顶部向底部增大, 呈良好梯度变化特征.对比不同降解程度原油样品中三甲基萘、四甲基萘和五甲基萘含量和分布可以发现生物降解的明显控制作用, 根据甲基取代萘异构体在生物降解过程中相对含量的变化初步确定了三甲基萘、四甲基萘和五甲基萘单个异构体的生物降解顺序, 结果表明那些热力学稳定性高的异构体容易遭受微生物的攻击, 而热力学稳定性低的异构体却在生物降解过程中相对富集, 表明生物降解作用完全不同于热力学作用过程, 当原油遭受中等程度生物降解作用影响后, 根据热力学稳定性提出的成熟度参数不再能提供有效的成熟度信息, 易降解和难降解异构体间的比值却是衡量原油遭受生物降解作用程度的地球化学新指标. 相似文献
3.
塔里木盆地群4井原油吡咯类含氮化合物地球化学研究 总被引：27，自引：7，他引：27
在塔里木盆地群４井原油中成功地分离并检测出丰富的吡咯类含氮化合物-链基咔唑类，而链基苯并咔唑和链基二苯并咔唑则未被发现。链基咔唑中以二甲基咔唑、C3-咔唑和C4-咔唑为主。在甲基咔唑和二甲基咔唑中又鉴别出多个异构体。甲基咔唑中G2 G3含量相当，而二甲基咔唑中G3占优势。在我国，原油含氮化合物研究刚刚起步。实践证明，该类化合物是研究油气运移的可靠的、专属性强的标志化合物。通过本项研究，我们认为群４井原油已经历了长距离的运移。 相似文献
4.
对渤海湾盆地一系列生物降解原油的色谱-质谱分析结果表明,庙西凹陷PL15-8D与PL9-4井四个严重生物降解原油三环萜烷系列分布较为异常,主要表现为以C23为主峰的后峰型、C20与C23为主峰的微弱双峰型以及以C20与C24为主峰的双峰型分布模式。强烈的生物降解作用导致C19~C23三环萜烷优先于C24+三环萜烷被不同程度地侵蚀,是形成这一异常分布的根本原因。三环萜烷系列相对丰度与绝对浓度的变化规律表明,不同碳数三环萜烷的生物降解作用同时发生,但其降解速率有明显差别,即抗生物降解能力不同。三环萜烷系列化合物（除C20三环萜烷以外）的抗生物降解能力具有随碳数增加而增强的趋势,而C20三环萜烷抗降解能力似乎强于C21~C23三环萜烷。原油中未检测到脱甲基三环萜烷,表明三环萜烷的降解并非通过微生物的脱甲基化作用,推测其降解途径是微生物氧化三环萜烷C环支链末端的甲基,形成对应的羧酸化合物。四个原油样品甾烷、藿烷与三环萜烷被微生物严重侵蚀,不能用于油源对比研究,而三芳甾烷未受生物降解影响,可作为研究区严重生物降解原油油源对比的有效指标。 相似文献
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本文用GC-MS技术分析了美国南佛罗里达盆地Sunnliand原油和油源岩抽提物中的芳烃,以便探讨碳酸盐岩环境中芳烃的分布特征,并用来重建古环境.Sunnliand原油和油源岩中含较半富的萘、菲、二苯并噻吩和三芳甾烷等化合物,甲基二苯并噻吩异构体呈V型分布.芴、氧芴和硫芴三系列化合物的相对含量以及其他地球化学特征如:Pr/Ph<1、正烷烃在C22-C30范围内呈偶碳优势、无或很少有二环倍半萜、含丰富的含硫芳烃等,指示Sunnliand原油和油源岩形成于海相强还原高盐环境.Sunnliand原油和油源岩中检出的一些化合物如:D环芳构化8,14-断藿烷、长链烷基苯、长链烷基苯并噻吩以及很高的延伸藿烷(C31-C35)和C24、C26四环萜烷表明Sunniland有机质有细菌输入.成熟度参数指示Sunniland原油和油源岩属未成熟至低成熟. 相似文献
6.
高邮凹陷韦庄地区原油吡咯类含氮化合物运移分馏效应 总被引：4，自引：0，他引：4
高邮凹陷韦庄地区具有正常和轻微生物降解2类原油, 对油气运移方向一直存在争议.根据2类原油中含氮化合物浓度、屏蔽型含氮化合物的相对含量与反映原油生物降解的地化参数C21-/C22+、Pr/nC17等nC17物降解作用对该区原油中含氮化合物的相对含量及其分布影响不明显, 运移作用仍然是造成含氮化合物分馏的主要因素.自东向西、东北向西南方向, 韦X11井、韦6 - 2井、韦5 - 19井、韦8井原油中屏蔽型咔唑的相对含量依次增大, 分别为11.6 2 %, 10.6 6 %, 12.70 %, 13.88%;暴露型咔唑的相对含量则表现出相反的变化趋势, 分别为30.6 0 %, 2 8.5 6 %, 2 6.4 3%, 2 4.6 2 %.由此明确了本区油气自东、东北方向向西、西南方向注入, 深凹带和车逻鞍槽提供了主要油源. 相似文献
7.
对塔里木盆地台盆区未遭受生物降解的138个原油样品进行甾、萜烷定量分析,展示原油甾、萜烷浓度随成熟度变化特征。C23三环萜烷/(C23三环萜烷+C30藿烷)值与甾、萜烷浓度图版显示各类甾、萜烷具有不同的热稳定性。依据热稳定性的差异将甾、萜烷分为3类:第1类包括Tm、C29藿烷和C30藿烷等五环三萜烷,随成熟度增高,这类化合物浓度降低较快,具有相对较低的热稳定性;第2类既包括Ts、C29Ts和C30重排藿烷等五环三萜烷,也包括C27和C29规则甾烷各异构体,随成熟度增高,这类化合物浓度降低较慢,具有中等热稳定性;第3类包括C27重排甾烷、C21甾烷和C23三环萜烷,随成熟度增高,这类化合物浓度先增高、后降低,降低速率低于前2类化合物,表明其热稳定性相对较高。在常用的甾、萜烷成熟度指标中,Ts/(Ts+Tm)、C29Ts/(C29Ts+C29藿烷)和C30重排藿烷/(C 相似文献
8.
借助于定量GC—MS分析技术,系统分析了一组取自辽河油田生物降解程度不同的原油芳烃馏分中三芴系列的组成特征。结果表明在生物降解过程中三芴系列化合物很容易遭受生物降解。母体三芴化合物在原油轻微降解阶段抗降解能力相似,其相对组成保持基本稳定,仍可指示沉积环境的性质;但进入中等及以上程度降解作用后,抗生物降解能力出现差异,相对组成发生变异,失去其环境意义。在甲基三芴系列中,甲基硫芴的抗降解能力强于甲基芴和甲基氧芴,降解速率不一致,组成特征不断变化,使甲基三芴系列相对组成不能指示沉积环境的性质。“三芴系列”被细菌消耗的速率不同,整个生物降解过程中其相对组成都在发生变化,因此对生物降解原油而言,无论其降解程度如何,“三芴系列”相对组成特征均不能有效的指示沉积环境的性质。 相似文献
9.
利用芳烃化合物研究东濮凹陷西斜坡地区原油成熟度 总被引：13，自引：0，他引：13
采用GC-MS分析技术探讨了东濮凹陷西斜坡胡状集-庆祖集油田原油芳烃化合物成熟度参数,包括烷基二苯并噻吩系列、脱羟基维生素E和三芳甾烷系列化合物。分析结果表明,芳烃化合物分布特征、脱羟基维生素E的β/α异构体比值、4/1MDBT、2,4/1,4DMDBT比值、C20/(C20+C26)TAS以及三芳甾烷的相对含量均反映胡状集-庆祖集油田二台阶构造带内的原油为烃源岩低熟阶段的产物,而来自长垣断层断裂带和长垣断层下降盘的原油属于烃源岩成熟阶段的产物。 相似文献
10.
通过研究东道海子凹陷烃源岩抽提物及周边构造原油的地球化学特征,总结了研究区内三套主要烃源岩产物在稳定碳同位素、Pr/Ph、甾烷相对组成等方面存在的差别。油源对比结果表明:研究区原油碳同位素相对较轻,Pr/Ph普遍小于3,甾烷相对组成中以C29含量最高,C28含量次之,整体上符合二叠系平地泉组烃源岩产物的特征,并在滴南凸起的西部及中部存在石炭系烃源岩产物不同程度的少量混入。通过各项生物标志化合物成熟度参数及甲基菲指数分析了原油成熟度的差异,并借助前人研究成果将其换算为统一的成熟度参数Ro,从而得出了不同演化阶段生成原油的分布范围。平地泉组烃源岩生烃高峰期的产物未能大规模运移至构造高部位成藏,可能尚赋存于凹陷深部及斜坡区域,东道海子凹陷斜坡区域低幅度构造及岩性圈闭是寻获生烃高峰期产物的有利目标。 相似文献
11.
The effect of biodegradation on polycyclic aromatic hydrocarbons in reservoired oils from the Liaohe basin, NE China 总被引：3，自引：0，他引：3
Haiping Huang Bernard F.J. Bowler Thomas B.P. Oldenburg Steve R. Larter 《Organic Geochemistry》2004,35(11-12):1619
The occurrence and distribution of polycyclic aromatic hydrocarbons (PAHs) has been studied in oil columns from the Liaohe basin, NE China, characterized by varied degrees of biodegradation. The Es3 oil column has undergone light to moderate biodegradation – ranging from levels 2 to 5 on the [Peters, K.E., Moldowan, J.M., 1993. The Biomarker Guide: Interpreting Molecular Fossils in Petroleum and Ancient Sediments. Prentice Hall, Englewood Cliffs, NJ, p. 363] scale (abbreviated as ‘PM level’) – while the shallower Es1 column has undergone more severe biodegradation, ranging from PM level 5 to 8. Both columns show excellent vertical biodegradation gradients, with degree of biodegradation increasing with increasing depth toward the oil–water contact (OWC). The compositional gradients in the oil columns imply mass transport control on degradation rates, with degradation occurring primarily at the OWC. The diffusion of hydrocarbons to the OWC zone will be the ultimate control on the maximum degradation rate. The chemical composition and physical properties of the reservoired oils, and the ‘degradation sequence’ of chemical components are determined by mixing of fresh oil with biodegraded oil.The PAH concentrations and molecular distributions in the reservoired oils from these biodegraded columns show systematic changes with increasing degree of biodegradation. The C3+-alkylbenzenes are the first compounds to be depleted in the aromatic fraction. Concentrations of the C0–5-alkylnaphthalenes and the C0–3-alkylphenanthrenes decrease markedly during PM levels 3–5, while significant isomer variations occur at more advanced stages of biodegradation (>PM level 4).The degree of alkylation is a critical factor controlling the rate of biodegradation; in most cases the rate decreases with increasing number of alkyl substituents. However, we have observed that C3-naphthalenes concentrations decrease faster than those of C2-naphthalenes, and methylphenanthrenes concentrations decrease faster than that of phenanthrene. Demethylation of a substituted compound is inferred as a possible reaction in the biodegradation process.Differential degradation of specific alkylated isomers was observed in our sample set. The relative susceptibility of the individual dimethylnaphthalene, trimethylnaphthalene, tetramethylnaphthalene, pentamethylnaphthalene, methylphenanthrene, dimethylphenanthrene and trimethylphenanthrene isomers to biodegradation was determined. The C20 and C21 short side-chained triaromatic steroid hydrocarbons are degraded more readily than their C26–28 long side-chained counterparts. The C21–22-monoaromatic steroid hydrocarbons (MAS) appear to be more resistant to biodegradation than the C27–29-MAS.Interestingly, the most thermally stable PAH isomers are more susceptible to biodegradation than less thermally stable isomers, suggesting that selectivity during biodegradation is not solely controlled by thermodynamic stability and that susceptibility to biodegradation may be related to stereochemical structure. Many commonly used aromatic hydrocarbon maturity parameters are no longer valid after biodegradation to PM level 4 although some ratios change later than others. The distribution of PAHs coupled with knowledge of their biodegradation characteristics constitutes a useful probe for the study of biodegradation processes and can provide insight into the mechanisms of biodegradation of reservoired oil. 相似文献
12.
《Applied Geochemistry》2001,16(14):1611-1619
Biodegradation of polycyclic aromatic hydrocarbon (PAH) was investigated in the whole matrix and in the different aggregate size fractions of a sandy soil contaminated by a mixture of 8 PAHs and incubated at water holding capacity. The distribution of PAHs and of phenanthrene-degrading bacteria were determined in the bulk soil and in 4 size aggregate fractions corresponding to sand, coarse silt, fine silt and clay. The microbial communities able to degrade phenanthrene were detected at a similar level in the different aggregate fractions of the soil before contamination. After soil contamination and incubation, a significant growth of bacteria was observed and their distribution within aggregates was modified. Bacterial communities of phenanthrene-degraders were present in a higher density in the aggregates corresponding to sand (2000–50 μm) and clay (<2 μm). Chemical analysis show that remaining PAHs (low and high molecular weight) were much more concentrated in the fine soil fractions (fine silt and clay) and were present at a very low content in the larger aggregate size fractions. The interactions of well defined aggregates with PAHs and bacteria were also studied using phenanthrene as PAH model substrate and individual aggregates corresponding to sand and clay size fractions. Incubation of sand and clay aggregate fractions enriched with phenanthrene in the presence of a bacterial isolate NAH1 led to the simultaneous solubilization and biodegradation of phenanthrene. Differences in amounts of solubilized phenanthrene between sand and clay aggregate size fractions would be related to difference in adsorption capacities of phenanthrene by clay and sand aggregates. 相似文献
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14.
通过对取自MBR膜生物反应器中的活性污泥加入菲进行富集培养、驯化,分离、纯化出一株能以菲为唯一碳源和能源的短杆状革兰氏阴性菌J-1,细菌长2～5μm,宽1～3μm;研究了初始底物浓度、温度、pH对菌株J-1降解菲的影响,探讨了菌株J-1胞内酶对菲降解的底物抑制动力学。试验表明:菌株J-1在48h内能将不同浓度菲的水溶液中的菲完全降解;菲浓度增加,达到完全降解的时间延长。温度对细菌的降解能力影响较大,菌株J-1对菲降解的最佳温度为28℃。1.15mg·L-1的菲,28℃时48h内能完全降解,而相同时间内10℃时的降解率仅为36.65%。菌株J-1对pH的波动具有一定的适应性,pH在一定范围内(6.0～8.4)变化对菲降解的影响不大,降解反应的最佳pH为7.2。菌株J-1对菲的降解符合一级动力学反应方程。较高的底物浓度对酶促降解反应具有抑制作用,酶促反应的最大速率常数vm=1.17mg·L-1·h-1,米氏常数Km=61.70mg·L-1;底物抑制常数kS=49.60mg·L-1;最佳底物浓度[S]opt=55.32mg·L-1。 相似文献
15.
The biodegradation of crude oil by microorganisms from well Luo-801, China, was examined in cultures grown under conditions that promoted either methanogenesis or sulfate reduction, at 35 °C and 55 °C. Headspace gas and oil compositions were characterized at 180 d and 540 d. Alkylphenanthrenes are relatively recalcitrant to bacterial attack and the biodegradation of these compounds appeared to be insignificant after 180 d under both conditions, but is evident after 540 d. The depletion of alkylphenanthrenes was monitored through evaluation of the ratio of alkylphenanthrenes to the most bioresistant, analyzed component (C28 20R triaromatic steroid hydrocarbon) and isomer susceptibility also was evaluated by relative abundance comparison within the compound class. The influence of growth temperature varied. Only slight differences in alkylphenanthrene concentrations were observed after 180 d whereas the greater degrees of biodegradation were observed at 35 °C in the methanogenic culture and at 55 °C in the sulfate reducing culture. Overall, higher biodegradation rates occur under sulfate reducing condition, which is consistent with the conclusion that methanogens are generally less able to compete for substrates than sulfate reducers. The biodegradation susceptibility of alkylphenanthrenes decreases with increasing degree of alkylation, i.e., phenanthrene (P) and methylphenanthrenes (MPs) were more easily biodegradable than C2-alkylphenanthrenes (C2-Ps) and C3-alkylphenanthrenes (C3-Ps). Biodegradation selectivity for specific homologues is not striking for the limited time duration of the experiments. However, 3-MP seems slightly more vulnerable than other methylphenanthrene isomers and 1,7-DMP has slightly higher ability to resist biodegradation than the other C2-P isomers. The commonly used thermal maturity parameters derived from methylphenanthrene isomer ratios are altered insignificantly by biodegradation and remain valid for geochemical assessment. This information should be useful for assessing the limits of in situ crude oil biodegradation. 相似文献
16.
芳烃作为原油和烃源岩中可溶烃的一个重要组分,能提供烃源岩沉积环境、有机质来源、热演化程度和油源对比等多方面信息,并且其比饱和烃具有更强的抗生物降解作用的能力,因此广泛用于生物降解油的相关研究。生物降解油广泛分布于中国青藏高原羌塘盆地,为了有效开展羌塘盆地油源对比研究工作,本文对隆鄂尼地区油苗开展了系统的芳烃有机地球化学特征研究,样品中检测出的15类化合物系列中菲系列含量极高,其次为三芴系列,萘系列含量较低,但同样检测出一定量的源于陆源高等植物母质的化合物,如卡达烯、惹烯和海松烯等,这表明羌塘盆地生油母质以海相低等水生生物为主,同时有一定量陆源高等植物输入。芳烃成熟度参数研究表明,甲基萘指数由于受到混源影响而不能单独用于成熟度评价,而甲基菲指数和甲基二苯并噻吩指数是羌塘盆地原油成熟度研究的有效指标,综合各类成熟度指标研究表明,羌塘盆地原油属于成熟油。 相似文献
17.
LD湾JZ25-1地区沙河街组二段、三段原油,具有低硫、中高含蜡、凝析油～轻质油的特点。原油未受到生物降解作用的影响,正构烷烃有微弱奇偶优势。原油的甾萜烷特征表现出中等伽马蜡烷丰度、4-甲基甾烷含量高,甲藻甾烷丰富,规则甾烷C27、C28、C295α(H)、14α(H)、17α(H)指纹呈不对称的"V"型分布特点,甾烷异构化参数表明原油为成熟原油。原油主要来源于淡水～微咸水的还原环境,富沟鞭藻以水生生物为主混合型输入的有机相。JZ25-1地区沙河街组二段及三段,正常原油与LX凹陷沙三段有很好亲缘关系,其主要来源LX凹陷沙河街组三段烃源岩,也有少量来自沙河街组一段。沙河街组二段凝析油主要为LX凹陷沙河街组一段烃源岩产生的低熟凝析油,也有少量来源于LX凹陷沙河街组三段烃源岩。 相似文献
18.
George D. WardlawRobert K. Nelson Christopher M. ReddyDavid L. Valentine 《Organic Geochemistry》2011,42(6):630-639
Contamination of coastal marine sediments with polycyclic aromatic hydrocarbons is pervasive, with major sources including anthropogenic activity and natural seepage. Biodegradation serves as a major hydrocarbon sink with evaporation and dissolution responsible for the removal of low boiling range compounds and photo-oxidation acting on many multi-substituted aromatic compounds. In this work, first-order rate constants for aerobic biodegradation were quantified for naphthalene (N), benzothiophene (BT) and their alkylated congeners (1-4 carbon substituents (C1-C4)) in laboratory experiments with oil laden marine sediments from a natural seep. Rate constants were used as proxies for microbial preference, which follows the order: naphthalene > C1N > C2N > C1BT > C2BT > benzothiophene > C3BT > C3N > C4BT > C4N, with some overlap. The application of comprehensive two dimensional gas chromatography further enabled separation and quantification of multiple structural isomers for C2N-C4N and C2BT-C4BT, with 7-12 isomers resolved for each C2N-C4N and 4-7 isomers resolved for each C2BT-C4BT. A strong isomeric biodegradation preference was noted within each of these compound classes, with rate constants varying as much as a factor of 2 for structural isomers of the same compound class. Each isomer was consumed to a low, but non-zero concentration, suggesting that their residual load in sediment may be proportional to the number of structural isomers originally present, in addition to the pattern and the number of alkyl substitutions. The simultaneous first-order biodegradation rates observed for 52 aromatic hydrocarbons resolved in this study, along with reference compounds such as n-alkanes, lends support to the concept of broad scale metabolic specificity during aerobic biodegradation of petroleum. 相似文献