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    用高分辨率质谱揭示塔中4油田原油成因机制

    李素梅 史权 张宝收 张海祖 潘娜 赵明 孟祥兵

    李素梅, 史权, 张宝收, 张海祖, 潘娜, 赵明, 孟祥兵, 2013. 用高分辨率质谱揭示塔中4油田原油成因机制. 地球科学, 38(1): 94-104. doi: 10.3799/dqkx.2013.009
    引用本文: 李素梅, 史权, 张宝收, 张海祖, 潘娜, 赵明, 孟祥兵, 2013. 用高分辨率质谱揭示塔中4油田原油成因机制. 地球科学, 38(1): 94-104. doi: 10.3799/dqkx.2013.009
    LI Su-mei, SHI Quan, ZHANG Bao-shou, ZHANG Hai-zhu, PAN Na, ZHAO Ming, MENG Xiang-bing, 2013. Formation Mechanism of the Oils in Tazhong-4 Oilfield Analyzed by High Resolution Mass Spectrum. Earth Science, 38(1): 94-104. doi: 10.3799/dqkx.2013.009
    Citation: LI Su-mei, SHI Quan, ZHANG Bao-shou, ZHANG Hai-zhu, PAN Na, ZHAO Ming, MENG Xiang-bing, 2013. Formation Mechanism of the Oils in Tazhong-4 Oilfield Analyzed by High Resolution Mass Spectrum. Earth Science, 38(1): 94-104. doi: 10.3799/dqkx.2013.009

    用高分辨率质谱揭示塔中4油田原油成因机制

    doi: 10.3799/dqkx.2013.009
    基金项目: 

    国家自然科学基金 40973031

    国家自然科学基金 41173061

    中国石油大学资源与探测国家重点实验室项目 PRPJC2008-02

    中国石油大学资源与探测国家重点实验室项目 PRP/indep-1-1101

    国家"973"项目 2011CB201102

    详细信息
      作者简介:

      李素梅(1968-), 女, 教授, 博士, 主要从事油气地质地球化学研究.E-mail: smli8888@yahoo.com.cn

    • 中图分类号: P618

    Formation Mechanism of the Oils in Tazhong-4 Oilfield Analyzed by High Resolution Mass Spectrum

    • 摘要: 塔里木盆地塔中4油田位于塔中构造较高部位, 具有显著不同于周边原油的特征.采用高分辨率质谱、色谱-质谱等对原油成因进行了调查.GC/MS分析表明, 塔中4油田石炭系原油中链烷烃(指示未降解-轻度降解)极其发育, 同时检测到丰富的降解三环萜烷及25-降藿烷系列(指示强烈生物降解), 反映该区油气具有多期充注特征.高分辨率质谱分析显示, 塔中4油田原油中硫化物分布正常, 低等效双键数(DBE)硫化物不太发育, 天然气组成与碳同位素也未显示异常, 反映石炭系原油可能未受TSR作用影响.观察到塔中4油田原油中硫化物组成与分布特征多数与下奥陶统原油相近, 指示两者可能有一定成因联系.混源模拟实验显示, 下奥陶统原油混入可导致塔中4油田原油出现高芳香硫特征.地质地球化学综合研究认为, 塔中4油田原油中芳香硫异常与深源油气混合有关, 与TSR作用关系不明显.

       

    • 图  1  塔中4油田构造位置与油藏剖面

      图a中说明:①I号断裂构造带;②TZ47-15井区;③TZ4油田/井区;④TZ16井区;⑤TZ1-6井区

      Fig.  1.  Tectonic location and profile of the Tazhong 4 oil pool

      图  2  塔中4油田及邻区代表性原油中链烷烃与降解萜烷系列分布特征

      空心圆为降解三环萜烷,实心圆为25-降解藿烷系列

      Fig.  2.  Distribution characteristics of the n-alkanes and biodegraded terpanes in the representative Tazhong-4 and the adjacent oils

      图  3  塔中4井区部分石炭系原油的芳烃总离子流图显示含超高丰度的二苯并噻吩系列

      图中MN、DMN、TMN、TEMN分别为甲基、二甲基、三甲基和四甲基萘;DBT、MDBT、DMDBT、TMDBT分别为二苯并噻吩、甲基、二甲基、三甲基二苯并噻吩

      Fig.  3.  Total ion chromatography of aromatic hydrocarbons in the Carboniferous oils illustrating significant high relative abundance of DBTs

      图  4  塔中4油田石炭系等原油中DBTs分布特征对比

      Fig.  4.  Correlation of the DBTs in the Carboniferous oils with the others in the Tazhong Uplift

      图  5  塔中4油田石炭系等原油中S1系列化合物碳数、DBE及其强度关系(x轴包含一个衍生甲基碳,泡点图大小代表不同DBE的S1化合物的强度)

      Fig.  5.  Plots of DBE versus the carbon number for the S1 class species in methylated oils from the positiveion ESI FT-ICR MS

      图  6  塔中4油田石炭系等原油中不同DBE系列的S1化合物分布特征

      Fig.  6.  Distribution characteristics of the S1 compounds with different DBE values for the Carboniferous oils etc

      图  7  芳烃馏分中二苯并噻吩、全油中DBE=9(DBE9)系列S1化合物相对丰度与饱/芳比关系(非石炭系数据源自Li et al., 2011b)

      Fig.  7.  Relative abundance of DBTs in aromatic fractions and DBE=9 compounds among S1 versus saturated hydrocarbons/aromatics ratio

      表  1  塔中4油田石炭系原油基本特征

      Table  1.   Basic characteristics of the Carboniferous oils from the Tazhong-4 oilfield

      井号 井段(m) 层位 密度(20 ℃)(g/cm3) 粘度(50 ℃)(mm2/s) 凝固点(℃) 硫醇(μg/mL) 饱和烃(%) 芳烃(%) 非烃(%) 沥青质(%) αααS/R DBT(μg/g) DBT(%) DBT/P
      TZ406 3 646.92~3 693.26 C 0.91 3.85 - - 23.1 32.7 11.5 32.7 0.53 861 42.1 0.94
      TZ404 3 619.47~3 681.81 CⅡ-Ⅲ - - - - 55.5 28.2 11.8 4.5 0.51 3 790 46.2 2.59
      TZ4 3 532~3 548 C 0.85 3.12 -25.0 - 74.8 19.5 5.7 0 0.47 4 230 29.8 1.52
      TZ4 3 712~3 720 C 0.92 51.19 10.5 - 58.0 25.7 12.7 3.6 0.53 4132 51.7 2.53
      TZ408 3 631.5~3 632.5 CⅢ 0.85 3.76 < -30.0 - 58.9 26.3 12.1 2.7 0.53 3 923 45.2 2.52
      TZ402 3 510~3 535 C 0.83 2.56 -34.0 55.9 30.5 13.6 0 0.52 4 058 44.6 2.66
      TZ402 3 613~3 628 C 0.84 2.81 -19.0 1.63 55.7 28.6 11.4 4.3 0.53 4 168 44.5 2.68
      TZ402 3 705.5~3 708 C 0.92 72.05 -21.5 36.0 24.6 10.3 29.1 0.55 2 670 42.7 2.59
      TZ421 3 221.0~3 223.5 C 0.82 4.75 -36.0 52.6 25.3 10.5 11.6 0.53 2 685 41.8 2.16
      TZ421 3 478~3 494.5 C 0.75 0.91 -45.0 1.60 86.4 10.2 3.4 0 0.49 3 419 19.6 1.12
      TZ421 3 570.5~3 575.0 C 0.84 2.85 -16.0 - 57.8 30.4 11.8 0 0.52 4 190 40.0 2.17
      TZ421 3 700.5~3 702.5 C - - - 1.63 59.3 22.9 8.5 9.3 0.51 2 820 11.3 0.34
      TZ422 3 604.0~3 624.0 C - - - - 54.3 32.6 10.1 2.9 0.54 3 809 45.8 2.76
      TZ75 3 701.00~3 715 C 0.86 6.25 -14.0 - 46.5 32.6 11.6 9.3 0.51 4 590 44.8 2.96
      TZ401 3 685~3 703 C 0.90 11.93 -5.0 - 40.4 31.7 15.4 12.5 0.53 6 243 54.1 4.56
      TZ411 3 263~3 450 C - - - 52.1 27.6 9.8 10.4 0.52 2 938 41.9 1.76
      TZ411 3 227.5~3 328 C 0.86 7.81 -18.0 36.4 38.6 14.8 10.2 0.52 3 320 40.6 2.24
      TZ411 3 439~3 450 C 0.83 4.37 -10.0 48.7 31.1 11.8 8.4 0.53 3 131 42.2 1.93
      TZ411 3 720~3 723 C 0.87 9.9 -12.5 - 60.9 25.4 6.5 7.1 0.54 4 711 53.8 4.75
      注:表中αααS/R.C29甾烷ααα20S/(S+R);DBT/P.二苯并噻吩/菲;DBT(μg/g).二苯并噻吩在原油中的绝对丰度;DBT.二苯并噻吩在可定性芳烃中的百分含量.
      下载: 导出CSV

      表  2  常规GC/MS、FT-ICR MS检测的塔中83井原油(O1)中的含硫化合物对比

      Table  2.   Correlation of the sulfur compounds from the TZ83 (O1) oil detected by GC-MS and FT-ICR MS

      含硫化合物类型 检测途径
      硫化合物中的杂原子类型及数量 化合物名称 等价双键数DBE GC/MS(可检测碳数) FT-ICR MS(可检测碳数)
      S1 硫醚 0 - + C11~C40
      环硫醚(四氢化噻吩) 1 + C10~C30 + C8~C46
      2 - + C11~C45
      噻吩 3 - + C9~C45
      4 - + C12~C43
      5 - + C11~C43
      苯并噻吩 6 - + C9~C44
      7 - + C9~C43
      8 - + C14~C43
      二苯并噻吩 9 + C12~C15 + C10~C47
      10~11 - + C12~C44
      12 - + C14~C44
      13 - + C14~C41
      14 - + C16~C44
      15 - + C18~C42
      16 - + C19~C41
      17 - + C20~C41
      18 - + C23~C40
      19 - + C25~C40
      O1S1 0~14 C8~C40*
      O1S2 4~9 - + C7~C29*
      O2S1 1~10 - + C11~C37*
      O3S1 2~7 C5~C28*
      S2 8~10 - + C13~C46*
      S3 7 C23~C48
      注:“-”.未能检测;“+”.可检测;“*”.因化合物的DBE值而异.
      下载: 导出CSV

      表  3  三元混合模拟实验参数

      Table  3.   Parameters for the binary and ternary oil mixing experiment

      混合类型 端元素油 与配比类型 DBTs(μg/g) 芳烃(μg/g) DBT*(%) 饱和烃(%) 芳烃(%) 饱/芳
      A(TZ15, S) 646.31 4 854 13.31 36.1 30.9 1.17
      端元油 B(TZ4, C) 4 230.00 14 179 29.83 74.8 19.5 3.84
      C(ZG5, O1) 2 021.00 3 585 56.37 96.36 2.18 44.17
      A∶B∶C=0.5∶0.5∶9 206 271.55 417 815 49.37 92.269 4.482 20.59
      三元 配比油 A∶B∶C=1∶1∶8 210 443.10 477 130 44.11 88.178 6.784 13.00
      A∶B∶C=1.5∶1.5∶7 214 614.65 536 445 40.01 84.087 9.086 9.25
      A∶C=1∶9 1 883.531 3 684.9 51.11 90.3 5.1 17.88
      二元 配比油 A∶C=2∶8 1 746.062 3 784.8 46.13 84.3 7.9 10.64
      A∶C=3∶7 1 608.593 3 884.7 41.41 78.3 10.8 7.25
      注:*.相对于GC/MS检测的芳烃馏分中可定性芳烃化合物总和.
      下载: 导出CSV
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    • 收稿日期:  2012-07-20
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