温压实验液态产物中菲和蒽系列的演化特征EVOLUTIONAL CHARACTERISTICS OF THE PHENANTHRENE AND ANTHRACENE SERIES IN THE LIQUID PRODUCTS FROM THE TEMPERATURE-PRESSURE EXPERIMENTS
张婷,王作栋,钱宇,王永莉,李晓斌,宋红莎
ZHANG Ting,WANG Zuodong,QIAN Yu,WANG Yongli,LI Xiaobin,SONG Hongsha
摘要(Abstract):
对华北中元古界下马岭组低熟海相页岩进行温压(Ⅰ系列)和温控(Ⅱ系列)模拟实验,并对原始样品和实验过程中的液态产物进行GCMS分析。结果表明:样品含较高丰度的菲、艹屈、萘等系列化合物,液态产物中检出了实验过程中新产生的蒽、甲基蒽和苯并萘并噻吩;随着温度的升高,菲系列中丰度较高的9-甲基菲、1-甲基菲逐渐向热稳定性更好的3-甲基菲、2-甲基菲转化,菲的相对丰度先减小后增大;模拟实验样品中检出的蒽系列化合物与温度呈正相关,表明其来源与热演化过程有关;温压实验过程中检测出丰度较高的苯并萘并噻吩,而其他温度段几乎检测不到,说明该化合物的形成需要适当的温度和压力;压力增大会抑制菲的烷基化和抑制蒽系列化合物形成,但会促进9-甲基菲的转化和苯并萘并噻吩的形成。
Temperature-pressure experiments were conducted on the low-maturity marine shale of Mesoproterozoic Xiamaling Formation in North China,containing pressure controlled experiments( Series Ⅰ) and temperature controlled experiments( Series Ⅱ),and moreover the analyses on the original samples and the liquid products in the experiments were dealt with by GC-MS. The results show that the samples contain abundant phenanthrene,chrysene,naphthalene etc,and the newly produced anthracene,methylanthracene and naphthobenzothiophene were detected in the liquid products in the process of the experiments; with the increase of the temperature,the high-abundance 9-methylphenanthrene and 1-methylphenanthrene are transformed gradually to more stable 3-meth-ylphenanthrene and 2-methylphenanthrene,the relative abundance of the phenanthrene first decreases and then increases; the checked out anthracene series compounds in the simulating experiment samples are positively correlated with the temperature,these conditions indicate that the sources of the anthracene series compounds are related to the thermal evolution process; the high-abundance naphthobenzothiophene is detected in Series I,while it is undetectable in the other temperature intervals,these phenomena indicate that the compound formation needs proper temperature and pressure; the greater pressure will not only inhibit the alkylation of the phenanthrene and the generation of the anthracene series compounds,but also promote the conversion of 9-methylphenanthrene and the formation of the naphthobenzothiophene.
关键词(KeyWords):
下马岭组;低熟海相页岩;温压模拟实验;菲系列;蒽系列;苯并萘并噻吩
Xiamaling Formation;low-maturity marine shale;temperature-pressure simulating experiment;phenanthrene series;anthracene series;naphthobenzothiophene
基金项目(Foundation): 国家自然科学基金项目“氦气资源在天然气藏中的聚集规律研究”(416721);; 兰州油气资源研究中心“十三五”创新基金“地质条件下温度对甾烷形成和分布的影响研究”(135CCJJ20160523);; 甘肃省油气资源研究重点实验室开放课题基金“海相烃源岩热解产物及微量杂原子化合物色谱质谱定量分析方法研究”(SZDKFJJ20150605)
作者(Author):
张婷,王作栋,钱宇,王永莉,李晓斌,宋红莎
ZHANG Ting,WANG Zuodong,QIAN Yu,WANG Yongli,LI Xiaobin,SONG Hongsha
DOI: 10.19597/J.ISSN.1000-3754.201705031
参考文献(References):
- [1]Radke M,Welte D.The methylphenanthrene index(MPI):A maturity parameter based on aromatic hydrocarbons[J].Advances in Organic Geochemistry,1983,27(5):504-512.
- [2]陈琰,包建平,刘昭茜,等.甲基菲指数及甲基菲比值与有机质热演化关系:以柴达木盆地北缘地区为例[J].石油勘探与开发,2010,37(4):508-12.
- [3]宋长玉,金洪蕊,刘璇,等.烃源岩中甲基菲的分布及对成熟度参数的影响[J].石油实验地质,2007,29(2):183-187
- [4]Simoneit B R T,Grimalt J O,Wang T G,et al.Cyclic terpenoids of contemporary resinous plant detritus and of fossil woods,ambers and coals[J].Organic Geochemistry,1986,10(4-6):877-889.
- [5]Thomas B R.Organic geochemistry[M].Berlin:Springer,1969:599-618.
- [6]孟仟祥,张文正.松粉热降解芳烃生物标志物特征及其地球化学意义:残渣抽提物研究[J].沉积学报,1999,17(12):825-831.
- [7]张立平,黄第藩.某些海相烃源岩中多环芳烃的组成特征[J].石油勘探与开发,1997,24(2):10-14.
- [8]妥进才.柴达木盆地第三系芳烃的地球化学:二环芳烃与多环芳烃的关系[J].石油实验地质,1996,18(4):406-412.
- [9]马军,李水福,胡守志,等.芳烃化合物组成及其在油气地球化学中的应用[J].地质科技情报,2010,29(6):73-79.
- [10]王作栋,郑建京,李晓斌,等.华北中—上元古界下马岭组烃源岩分子指纹特征[J].天然气地球科学,2013,24(3):599-603.
- [11]曾花森,蔡郁文,霍秋立,等.烃源岩中有效有机质的类型评价及意义[J].大庆石油地质与开发,2013,32(3):8-14.
- [12]刘忆彤,刘忠生,李景坤,等.塔东地区奥陶系—寒武系烃源岩评价[J].大庆石油地质与开发,2015,34(5):18-24.
- [13]Luo Genming,Hallmann C,Xie Shucheng,et al.Comparative microbial diversity and redox environments of black shale and stromatolite facies in the Mesoproterozoic Xiamaling Formation[J].Geochimica&Cosmochimica Acta,2015,151(1):150-167.
- [14]刘庆.东营凹陷樊页1井沙河街组烃源岩元素地球化学特征及其地质意义[J].油气地质与采收率,2017,24(5):1-7.
- [15]高林志,张传恒,史晓颖,等.华北古陆下马岭组归属中元古界的锆石SHRIMP年龄新证据[J].科学通报,2008,53(21):2617-2623.
- [16]高林志,张传恒,史晓颖,等.华北青白口+系下马岭组凝灰岩锆石SHRIMP U-Pb定年[J].地质通报,2007,26(3):249-255.
- [17]王泽九,黄枝高,姚建新,等.中国地层表及说明书的特点与主要进展[J].地球学报,2014,35(3):271-276.
- [18]荆铁亚,杨光,林拓,等.中国中上元古界页岩气地质特征及有利区预测[J].特种油气藏,2015,22(6):5-9.
- [19]Rowl S J,Alexander R,Kagi R I,et al.Microbial degradation of aromatic components of crude oils:A comparison of laboratory and field observations[J].Organic Geochemistry,1986,9(4):153-161.
- [20]宋红莎,张晓宝,曹占元,等.隆鄂尼地区油砂地质及地球化学特征[J].大庆石油地质与开发,2017,36(1):43-49.
- [21]Killops S D,Readman J W.HPLC fractionation and GC-MS determination of aromatic hydrocarbons from oils and sediments[J].Organic Geochemistry,1985,8(4):247-257.
- [22]Garrigues P,Ewald M,Natural occurrence of 4-methyl-phenanthrene in petroleums and recent marine sediments:A new sensitive method to identify and quantify isomers in a series of alkyl—PAH:High resolution spectrofluorimetry at 15 K in n-alkane(Shpolskii effect)[J].Organic Geochemistry,1983,5(2):53-56.
- [23]谢春安.菲系列化合物的分布特征及其意义[J].科技资讯,2006(30):184.
- [24]Raymond R L,Jamison V W,Hudson J O.Microbial hydrocarbon co-oxidation I.Oxidation of mono-and dicyclic hydrocarbons by soil isolates of the genus Nocardia[J].Applied Microbiology,1967,15(4):857-865.
- [25]赵海舟.腐泥煤和腐植煤生物标志物色谱对比[J].中国煤田地质,2002,14(2):16-19.
- [26]王传远,杜建国,段毅,等.芳香烃地球化学特征及地质意义[J].新疆石油地质,2007,28(1):29-32.
- [27]Zhang H,Wang C,Zhao R,et al.New diagnostic ratios based on phenanthrenes and anthracenes for effective distinguishing heavy fuel oils from crude oils[J].Marine Pollution Bulletin,2016,106(1-2):58-61.
- [28]周世新,贾星亮,宋振响,等.塔里木盆地深层碳酸盐岩中不同赋存形式芳烃化合物组成[J].沉积学报,2008,26(2):330-339.
- [29]Fan Pu,Philip R P,Li Zhenxi,et al.Geochemical characteristics of aromatic hydrocarbons of crude oils and source rocks from different sedimentary environments[J].Organic Geochemistry,1990,16(1-3):427-435.
- [30]夏燕青,王春江.联苯系列化合物与苯并萘噻吩系列化合物的形成机制[J].中国科学D辑,1999,29(3):260-262.
- [31]林青,周明辉,魏志红,等.晚三叠世末期楚雄盆地云龙凹陷海相沉积的分子地球化学证据[J].石油勘探与开发,2004,31(4):29-31.
- [32]刘琼,何生.江汉盆地西南缘原油中含硫化合物的分布特征及其地球化学意义[J].地质科技情报,2008,27(2):56-62.
- [33]张敏,张俊.塔里木盆地原油噻吩类化合物的组成特征及地球化学意义[J].沉积学报,1999,17(1):121-126.
- 下马岭组
- 低熟海相页岩
- 温压模拟实验
- 菲系列
- 蒽系列
- 苯并萘并噻吩
Xiamaling Formation - low-maturity marine shale
- temperature-pressure simulating experiment
- phenanthrene series
- anthracene series
- naphthobenzothiophene