Crude oil type classification and source rock identification in Miaoxi area of Bohai Sea area based on stoichiometric method
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摘要: 渤海海域庙西地区原油类型复杂，油源及成因类型不清，多元统计分析可以综合考察多种关联数据间的交叉关系, 尤其适合于大规模数据收集的数据挖掘和区域性的油—油(源)分析。利用生物标志物指标参数体系，采用国际上常用的层次聚类分析(HCA)和主成分分析(PCA)，对渤海海域庙西地区多个层位的原油进行了油—油(源)对比。庙西地区存在3种类型原油：Ⅰ类原油成熟度较低，低的C23TT/C30H比值反映可能源自淡水湖泊，处于还原环境且有充足的陆源有机质输入，其与黄河口东洼沙一、二段烃源岩具有良好的相关性；Ⅱ类原油处于成熟阶段，C23TT/C30H和G/C30H比值低于Ⅰ类原油，但Pr/Ph、甾烷/藿烷、C19TT/C23TT比值略高于Ⅰ类原油，表明原油可能源自淡水湖泊环境，陆源有机质输入，推断其源于沙三段烃源岩，黄河口东洼与庙西南洼烃源岩对Ⅱ类原油均有贡献；Ⅲ类原油处于成熟阶段，ETR[(C28TT+C29TT)/(C28TT+C29TT+Ts)]、G/C30H、C23TT/C21TT、Pr/Ph和C23TT/C30H、C24Te/C26TT、规则甾烷C27/C29、4-甲基甾烷/C29规则甾烷参数分布范围较为广泛，反映出油源岩的沉积环境和有机质输入的类型具有较大的异向性，推断其可能为沙三段、沙四段烃源岩的混源油。利用交替最小二乘法计算显示，Ⅲ类原油主要来源于沙四段烃源岩，贡献率为85%~93%，沙三段的贡献率仅为7%~15%。Abstract: The crude oil types in the Miaoxi area of the Bohai Sea area are highly complex, and the source rocks and genetic types remain unclear. Using multivariate statistical analysis, researchers can comprehensively examine the interrelationships among multiple correlated variables, which is particularly suitable for large-scale data mining and regional oil-oil and oil-source analysis. In this study, based on the biomarker parameter index system, hierarchical cluster analysis (HCA) and principal component analysis (PCA), common methods in multivariate statistical analysis, were applied for oil-oil and oil-source correlation of crude oil from multiple layers in the Miaoxi area. Three types of crude oil were detected. Type Ⅰ crude oil are characterized by a low C23TT/C30H ratio with relatively low maturity. It may be derived from a freshwater lacustrine reducing environment with abundant input of terrigenous organic matter. This type of crude oil shows a strong correlation with the source rocks in the first and second members of the Shahejie Formation in the eastern sag of the Huanghekou Depression. Type Ⅱ crude oil is at a mature stage and features lower C23TT/C30H and G/C30H ratios compared to Type Ⅰ, but with slightly higher Pr/Ph, sterane/hopane, and C19TT/C23TT ratios. These features also indicate a freshwater lacustrine environment with terrestrial organic matter input. It is inferred that Type Ⅱ oil is mainly sourced from the third member of the Shahejie Formation, with contributions from source rocks in both the eastern sag of the Huanghekou Depression and the southern sag of the Miaoxi Depression. Type Ⅲ crude oil is at a mature stage, exhibiting a wide distribution range in multiple biomarker parameters, including ETR[(C28TT+C29TT)/(C28TT+C29TT+ Ts)], G/C30H, C23TT/C21TT, Pr/Ph, C23TT/C30H C24Te/C26TT, C27/C29 regular sterane, and 4-methyl sterane/ C29 regular sterane. These variations reflect heterogeneity in the depositional environment of oil source rocks and organic matter types. It can be concluded that type Ⅲ crude oil is mixed-source oil, likely derived from the third and fourth members of the Shahejie Formation. Alternating least squares analysis results indicated that Type Ⅲ crude oil is mainly derived from the source rocks in the fourth member of the Shahejie Formation, with a contribution rate of 85% to 93%, while the contribution from the third member is only 7% to 15%.
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图 2 渤海海域庙西地区原油族组分分布特征
Figure 2. Distribution characteristics of crude oil group components in Miaoxi area of Bohai Sea area
图 3 渤海海域庙西地区原油饱和烃质量色谱图
Pr为姥鲛烷；Ph为植烷；TT为三环萜烷；Te为四环萜烷；Ts为C27-18α(H)三降新霍烷；Tm为C27-17α(H)三降霍烷；H为藿烷；G为伽马蜡烷。
Figure 3. Mass chromatograms of saturated hydrocarbons of crude oil in Miaoxi area of Bohai Sea area
图 4 渤海海域庙西地区原油Pr/nC17—Ph/nC18交会图
Figure 4. Cross-plots of Pr/nC17-Ph/nC18 in crude oil from Miaoxi area of Bohai Sea area
图 5 渤海海域庙西地区原油C29ββ/(αα+ββ)—C2920S/(20S+20R)交会图以及MDBI—DBT交会图
Figure 5. Cross-plots of C29ββ/(αα+ββ)-C2920S/(20S+20R) and MDBI-DBT in crude oil from Miaoxi area of Bohai Sea area
图 6 渤海海域庙西地区原油样品聚类分析谱系图
Figure 6. Dendrogram of cluster analysis for crude oil samples in Miaoxi area of Bohai Sea area
图 7 渤海海域庙西地区原油主成分三维图
图中数值表示降维后得到的特征值。
Figure 7. Three-dimensional plots of principle components of crude oil in Miaoxi area of Bohai Sea area
图 8 渤海海域庙西地区原油生物标志化合物散点图
Figure 8. Scatter plots of biomarker compounds in crude oil from Miaoxi area of Bohai Sea area
图 9 渤海海域庙西地区烃源岩有机质丰度和类型
Figure 9. Cross-plots of organic matter abundance and types in source rocks from Miaoxi area of Bohai Sea area
图 10 渤海海域庙西地区部分烃源岩样品生物标志化合物特征
Figure 10. Characteristics of biomarker compounds in selected source rock samples from Miaoxi area, Bohai Sea area
图 11 渤海海域庙西地区原油与不同层位烃源岩生物标志化合物参数对比
Figure 11. Comparison diagrams of biomarker compound parameters between crude oil and source rocks at different layers of Miaoxi area, Bohai Sea area
表 1 渤海海域庙西地区油气地球化学分析数据
Table 1. Geochemical analysis data of oil and gas in Miaoxi area of Bohai Sea area
样品号 层位 密度/(g/cm3) 黏度/(mPa·s) 含蜡量/% 含硫量/% SA/‰ AR/‰ SAT/% ARO/% (NSO+ASP)/% CPI OEP Pr/nC17 Ph/nC18 Pr/Ph G/C30H PL15-2-8A Ng 0.95 490.94 1.86 0.84 -28.34 -24.18 44.23 31.35 20.58 0.25 0.09 0.96 0.33 0.70 0.77 PL15-2-8B Ng 0.93 1 716.96 2.15 0.51 -27.09 -25.82 41.11 28.86 24.20 0.77 0.37 3.53 0.36 1.93 0.76 PL15-2-8C Ng 0.93 208.69 3.38 0.77 -28.22 -26.43 39.02 28.29 22.93 0.55 0.17 0.61 0.17 0.93 0.61 PL15-2-A Ng 0.99 272.20 1.52 0.57 -29.87 -25.06 38.82 27.03 25.61 1.14 1.22 1.78 2.22 0.92 0.13 PL15-2-C Ng 0.88 497.03 1.66 0.86 -27.71 -23.89 49.53 25.71 21.23 0.57 0.52 1.01 0.13 3.23 0.13 PL15-2-B Ng 0.89 2 088.10 2.62 0.93 -26.71 -24.02 39.78 26.58 29.93 0.87 1.37 7.32 1.37 0.86 0.11 PL25-6-A Ng 0.93 595.11 0.93 0.44 -28.33 -24.37 46.88 20.57 27.08 0.97 1.43 24.55 0.06 1.37 0.11 PL25-6-B Ng 0.99 848.17 3.15 0.21 -26.57 -25.64 42.27 31.08 21.56 0.35 0.98 0.57 0.50 1.06 0.41 PL25-6-C Ng 0.98 81.15 4.45 1.63 -26.69 -25.68 44.34 29.49 22.46 0.53 0.40 1.07 0.18 1.91 0.22 PL25-6-D Ng 0.98 212.36 4.88 0.95 -26.10 -25.27 43.51 30.52 24.24 1.55 1.75 0.28 0.45 0.62 0.14 PL20-3-A Ng 0.95 288.99 7.93 0.64 -27.17 -23.96 43.91 27.16 23.35 0.72 1.58 0.09 0.04 2.50 0.44 BZ35-2-A Ng 0.89 287.64 2.95 0.85 -25.74 -25.81 41.75 24.50 32.25 1.47 1.64 2.25 1.72 1.17 0.08 BZ35-2-B Ng 0.88 706.10 3.81 1.33 -25.36 -24.02 65.15 16.92 22.22 1.08 1.04 0.41 0.33 1.25 0.09 BZ35-2-C Ng 0.94 469.97 7.79 0.51 -26.70 -26.85 58.53 24.04 13.76 1.09 1.04 0.61 0.48 1.30 0.07 KL6-1-A Es1 0.96 522.87 5.19 1.37 -25.94 -25.22 57.58 26.26 12.08 1.11 1.30 3.66 2.82 1.09 0.17 KL6-4-C Ed3 0.88 948.66 7.06 1.27 -25.71 -23.35 60.00 20.26 13.33 1.22 1.10 0.61 0.58 1.12 0.08 KL6-4-A Ed3 0.89 378.04 7.34 2.96 -28.78 -25.96 57.35 20.41 16.94 1.26 1.24 0.77 0.71 1.24 0.05 KL6-4-B Ed3 0.89 2 291.31 12.30 1.19 -27.27 -26.06 56.30 21.75 19.11 1.25 1.24 0.74 0.68 1.22 0.06 PL31-3S-A Ng 0.88 83.78 3.38 0.34 -26.31 -25.93 46.10 30.50 15.96 1.47 1.83 17.47 8.69 0.91 0.13 PL31-3S-B Ng 0.98 196.00 4.24 0.36 -25.84 -26.47 43.62 36.38 17.23 1.88 2.41 0.35 0.71 0.49 0.12 BZ36-1-A Ng 0.99 610.69 7.03 1.03 -25.44 -25.59 32.38 37.14 23.81 1.19 1.45 1.21 0.99 1.22 0.23 BZ36-1-B Ng 0.95 1 046.41 7.40 1.13 -25.57 -26.72 37.17 34.87 22.70 1.22 1.42 9.76 7.48 0.85 0.21 注：SA和AR分别为原油饱和烃和芳烃碳同位素；SAT、ARO和NSO+ASP分别为原油饱和烃、芳烃和非烃+沥青质含量；CPI为碳优势指数；OEP为奇偶优势指数；G/C30H为伽马蜡烷/C30藿烷；Pr/Ph为姥鲛烷/植烷。CPI、OEP由m/z 85计算，Pr/nC17、Ph/nC18、Pr/Ph数据来自于饱和烃色谱数据。 
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表 2 渤海海域庙西地区原油地球化学参数
Table 2. Geochemical parameters of crude oil in Miaoxi area of Bohai Sea area
样品地区 样品号 层位 化学计量学计算选用参数(HCA和PCA) 沉积环境 成熟度 母质类型 R1 R2 R3 R4 R5 R6 R7 R8 R9 R10 R11 R12 R13 R14 R15 R16 R17 黄河口东洼 BZ35-2-A Ng 1.17 0.86 0.08 0.70 0.06 0.25 0.33 0.34 0.37 0.44 1.77 0.10 0.25 1.77 0.71 0.43 2.02 BZ35-2-B Ng 1.25 1.95 0.09 0.72 0.10 0.22 0.26 0.62 0.53 0.44 3.20 0.07 0.20 3.20 0.81 0.36 2.00 BZ35-2-C Ng 1.30 0.95 0.07 0.68 0.07 0.24 0.33 0.46 0.39 0.45 2.47 0.15 0.23 2.47 0.75 0.37 1.40 BZ36-1-A Ng 1.12 0.85 0.23 0.72 0.10 0.16 0.29 0.42 0.38 0.42 3.51 0.08 0.57 3.51 0.70 0.27 1.97 BZ36-1-B Ng 0.85 0.56 0.21 0.80 0.07 0.08 0.30 0.41 0.35 0.38 1.92 0.07 0.45 1.92 0.71 0.31 2.17 KL6-4-A Ed3 1.24 1.65 0.05 0.83 0.04 0.18 0.58 0.35 0.30 0.35 1.70 0.03 0.24 2.31 0.70 0.25 1.70 KL6-4-B Ed3 1.22 1.56 0.06 0.86 0.04 0.24 0.49 0.36 0.32 0.36 1.59 0.09 0.26 1.70 0.67 0.30 1.46 KL6-4-C Ed3 1.12 1.46 0.08 0.78 0.05 0.17 0.14 0.40 0.32 0.37 2.31 0.38 0.27 1.59 0.81 0.37 1.38 KL6-1-A Es1 1.09 1.51 0.17 0.87 0.24 0.22 0.35 0.58 0.47 0.41 4.15 0.06 0.27 2.14 0.85 0.36 2.09 庙西南洼 PL31-3S-A Ng 0.91 1.37 0.13 0.76 0.07 0.26 0.10 0.49 0.37 0.42 2.14 0.14 0.31 0.36 0.79 0.48 2.20 PL31-3S-B Ng 0.49 1.39 0.12 0.78 0.11 0.21 0.36 0.55 0.40 0.45 0.36 0.09 0.34 3.51 0.82 0.40 2.07 PL25-6-A Ng 0.92 1.93 0.13 0.85 0.06 0.38 0.48 0.35 0.31 0.33 1.49 0.03 0.31 1.92 0.74 0.25 1.81 PL25-6-B Ng 3.23 1.5 0.13 0.77 0.24 0.31 0.46 0.45 0.44 0.36 3.30 0.03 0.57 1.80 0.80 0.24 1.77 PL25-6-C Ng 0.86 1.18 0.11 0.82 0.15 0.23 0.38 0.42 0.39 0.43 2.59 0.07 0.41 1.93 0.79 0.31 1.58 PL25-6-D Ng 1.37 0.99 0.11 0.76 0.13 0.32 0.24 0.40 0.38 0.41 2.69 0.03 0.40 2.11 0.77 0.37 2.16 PL15-2-A Ng 1.91 1.12 0.22 0.65 0.27 0.29 0.11 0.56 0.42 0.51 2.05 0.20 0.32 2.05 0.83 0.42 1.99 PL15-2-B Ng 2.50 1.30 0.44 0.81 0.30 0.21 0.11 0.49 0.47 0.44 2.49 0.34 0.23 4.05 0.88 0.35 1.53 PL15-2-C Ng 0.62 1.32 0.14 0.73 0.15 0.29 0.30 0.55 0.45 0.50 4.05 0.07 0.28 2.49 0.91 0.26 1.94 PL20-3-A Ng 1.06 1.59 0.41 0.78 1.00 0.44 0.42 0.50 0.34 0.52 1.80 0.06 0.32 1.80 0.85 0.27 1.65 PL15-2-8A Ng 0.70 1.58 0.77 0.51 0.79 0.54 0.20 0.56 0.39 0.43 1.30 1.07 0.12 1.30 0.31 0.31 1.87 PL15-2-8B Ng 1.93 1.37 0.76 0.58 1.30 0.59 0.14 0.41 0.44 0.49 0.88 1.10 0.25 0.88 0.57 0.31 1.71 PL15-2-8C Ng 0.93 0.90 0.61 0.71 1.01 0.31 0.33 0.48 0.35 0.33 0.89 1.20 0.20 0.89 0.35 0.26 1.62 注：R1为Pr/Ph；R2为C26/C25TT；R3为G/C30H；R4为C35H/C34H；R5为TT/H=∑C19~30TT/∑C29~35H；R6为ETR=(C28TT+C29TT)/(C28TT+C29TT+Ts)；R7为4-甲基甾烷/C29规则甾烷；R8为Ts/(Ts+Tm)；R9为C29ββ/(ββ+αα)；R10为C2920S/(20S+20R)；R11为DBT；R12为(孕甾烷+升孕甾烷)/C29规则甾烷；R13为S/H=∑C27~29甾烷/∑C29~35H；R14为4-/1DBT；R15为C21/C23TT；R16为C19TT/C23TT；R17为C24Te/C26TT。
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表 3 渤海海域庙西地区沙河街组烃源岩地球化学参数
Table 3. Geochemical parameters of source rocks in Shahejie Formation of Miaoxi area, Bohai Sea area
样品地区 层位 样品号 R1 R2 R3 R4 R5 R6 R7 R8 R9 R10 R11 R12 R13 R14 R15 R16 R17 黄河口东洼 沙一、二段 BZ36-3-A 1.61 0.18 0.12 0.79 0.13 0.17 0.33 0.28 0.23 0.17 2.34 0.08 0.18 1.42 0.90 0.20 4.74 BZ36-3-B 0.40 2.61 0.58 0.40 0.31 0.34 0.31 0.50 0.27 0.08 3.51 0.03 0.45 2.18 1.25 0.21 1.12 BZ36-3-A 0.82 1.11 0.08 0.50 0.29 0.28 0.32 0.91 0.38 0.35 1.07 0.25 0.36 1.87 0.71 0.15 1.13 沙三段 BZ36-1-A 0.72 1.90 0.04 0.67 0.30 0.11 0.02 0.75 0.33 0.13 2.63 0.08 0.39 1.66 1.03 0.37 1.20 BZ36-1-B 0.70 1.78 0.05 0.78 0.36 0.09 0.13 0.58 0.30 0.10 3.00 0.03 0.44 1.76 0.94 0.45 1.95 BZ36-2-A 0.73 1.60 0.04 0.56 0.22 0.09 0.12 0.27 0.21 0.30 0.70 0.02 0.27 0.34 0.87 0.16 3.06 BZ36-4-A 0.31 2.18 0.01 0.58 0.22 0.04 0.14 0.20 0.21 0.08 2.44 0.01 0.28 1.95 1.07 0.20 4.80 BZ36-4-B 0.33 1.38 0.18 0.98 0.77 0.11 0.19 0.22 0.20 0.11 1.84 0.01 0.99 1.36 0.76 0.18 2.29 庙西南洼 沙一、二段 LK31-1-A 0.83 4.77 0.04 0.67 1.33 0.12 0.00 0.27 0.21 0.01 2.19 0.01 1.33 0.89 0.72 0.00 6.99 LK31-1-B 1.08 1.33 0.05 0.89 0.88 0.22 0.00 0.35 0.22 0.03 0.30 0.02 0.89 1.41 0.98 0.34 2.35 LK31-1-C 0.21 1.18 0.24 0.78 0.92 0.14 0.18 0.00 0.19 0.04 0.19 0.01 1.05 1.28 0.93 0.33 1.48 PL25-3S-A 0.88 1.29 0.07 0.62 0.45 0.15 0.24 0.55 0.25 0.19 1.31 0.04 0.32 0.67 0.78 0.55 3.12 PL25-3S-B 0.95 0.52 0.03 0.44 0.20 0.28 0.22 0.56 0.24 0.19 1.17 0.04 0.19 1.25 0.85 0.20 3.70 沙三段 LK31-1-A 1.00 0.45 0.25 0.59 0.46 0.11 0.00 0.28 0.22 0.13 0.23 0.01 0.53 1.39 0.63 0.25 0.89 LK31-1-B 1.03 0.56 0.20 0.58 0.43 0.08 0.82 0.48 0.12 0.17 0.12 0.00 0.57 1.59 0.50 0.56 0.93 LK31-1-C 0.94 1.24 0.06 0.74 0.33 0.06 0.18 0.52 0.22 0.12 0.16 0.02 0.31 2.04 0.68 0.10 4.78 PL25-3S-A 1.02 1.08 0.04 0.52 0.27 0.04 0.15 0.59 0.22 0.16 0.23 0.04 0.25 2.13 1.05 0.45 5.13 PL25-3S-B 0.28 1.97 0.07 0.52 0.34 0.11 0.20 0.61 0.20 0.11 0.18 0.02 0.31 3.12 1.02 0.08 3.46 沙四段 PL25-3S-C 0.70 1.28 0.12 0.47 0.35 0.12 0.19 0.47 0.21 0.14 0.06 0.02 0.33 2.24 0.92 0.26 3.56 PL25-3S-D 0.70 1.31 0.11 0.42 0.40 0.22 0.19 0.48 0.23 0.17 0.18 0.03 0.38 1.63 0.94 0.24 3.69 PL25-3S-E 0.24 1.21 0.13 0.53 0.42 0.20 0.19 0.42 0.21 0.16 3.19 0.04 0.40 3.10 0.91 0.16 3.52 PL25-3S-F 0.58 1.48 0.14 0.60 0.34 0.15 0.22 0.42 0.23 0.16 3.09 0.02 0.33 2.18 0.64 0.09 3.46 注：R1为Pr/Ph；R2为C26/C25TT；R3为G/C30H；R4为C35H/C34H；R5为TT/H=∑C19~30TT/∑C29~35H；R6为ETR=(C28TT+C29TT)/(C28TT+C29TT+Ts)；R7为4-甲基甾烷/C29规则甾烷；R8为Ts/(Ts+Tm)；R9为C29ββ/(ββ+αα)；R10为C2920S/(20S+20R)；R11为DBT；R12为(孕甾烷+升孕甾烷)/C29规则甾烷；R13为S/H=∑C27~29甾烷/∑C29~35H；R14为4-/1DBT；R15为C21/C23TT；R16为C19TT/C23TT；R17为C24Te/C26TT。
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表 4 渤海海域庙西地区原油样品主成分分析的初始特征值与累计贡献量
Table 4. Initial eigenvalues and cumulative contribution for principal component analysis of crude oil samples in Miaoxi area of Bohai Sea area
成分 初始特征值 累计贡献量/% 总计 方差/% PC1 6.54 50.32 50.32 PC2 1.73 13.28 63.60 PC3 1.34 10.32 73.92 PC4 1.10 8.48 82.39 注：提取方法为主成分分析法，提取了4个成分。
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