Application of multivariate statistical analysis in oil and source correlation: a case study of mixed-source oils from middle and shallow strata in coastal area of Qikou Sag, Bohai Bay Basin
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摘要: 渤海湾盆地歧口凹陷滨海地区是近年来大港油田增储上产的重要目标，该地区中—浅层系原油来源复杂，混合严重，次生变化明显。多元统计分析方法是一种高效率、便捷且具有高精度的数据处理手段。近年来，许多学者在不同地区的油气源对比中运用该方法取得了较为丰富的研究成果，但针对多元统计分析在混源油油源对比中的应用研究仍有待进一步加强。为此，以油气地质地球化学理论为指导，在揭示研究区中—浅层系原油(沙一段、东营组、馆陶组、明化镇组)和主力烃源岩(沙三段、沙一段、东三段)地球化学特征的基础上，应用聚类、主成分和判别分析方法，开展油源对比。结果表明，歧口凹陷滨海地区各层系烃源岩成熟度差异较小，沙一中、沙一下烃源岩品质更好；烃源岩生烃母质以混合来源为主，其中沙一中、沙一上和东三段形成于弱还原、淡水条件，沙三段、沙一下烃源岩形成于还原、淡水—微咸水条件。研究区的次生变化以生物降解作用为主，不同层系原油可分为两类：其中Ⅰ类原油分布在沙一段，具有低Pr/Ph值、高三环萜烷的特点，主要以沙三段、沙一下和沙一中烃源岩混合供烃；Ⅱ类原油分布在东营组、馆陶组和明化镇组，具有较高Pr/Ph值、低三环萜烷的特点，主要以沙一上和东三段烃源岩混合供烃。应用判别分析验证这两类油—源，获得初始验证率100%，交叉验证正确率90.0%，表明油源对比结果可靠。研究成果揭示了多元统计分析方法在混源油油源对比中的良好应用前景。Abstract: The coastal area of the Qikou Sag of Bohai Bay Basin has become an important target for increasing reserves and production in the Dagang Oilfield in recent years. In this area, crude oil from the middle and shallow strata of the region exhibited complex origins, severe mixing, and significant secondary alterations. Multivariate statistical analysis is an efficient, convenient, and accurate data processing method. In recent years, many researchers have applied this method to hydrocarbon source correlation in various regions, yielding fruitful research results. However, its application in source correlation of mixed-source oils requires further development. Guided by petroleum geology and geochemistry theory, this study characterized the geochemical characteristics of crude oils from the middle and shallow strata (the first member of the Shahejie Formation, Dongying Formation, Guantao Formation, and Minghuazhen Formation) and main source rocks (the third member of the Shahejie Formation, the first member of the Shahejie Formation, and the third member of the Dongying Formation). Then, cluster analysis, principal component analysis, and discriminant analysis were applied for oil and source correlation. The results demonstrated that the maturity of source rocks in different strata of the coastal area of the Qikou Sag was relatively similar, and the middle and lower units of the first member of the Shahejie Formation had better hydrocarbon quality. The precursor for hydrocarbon generation of these source rocks was mainly of mixed origin. The middle and upper units of the first member of the Shahejie Formation and the third member of the Dongying Formation source rocks were deposited under weakly reducing, freshwater conditions, while the third member of the Shahejie Formation and the lower unit of the first member of the Shahejie Formation source rocks were formed under reducing, fresh to brackish water conditions. The main secondary alteration in the study area was biodegradation. The crude oils from different strata could be classified into two types: Type Ⅰ crude oil, distributed in the first member of the Shahejie Formation, was characterized by low Pr/Ph values and high tricyclic terpane content. It mainly originated from a mixture of source rocks in the third member of the Shahejie Formation and the middle and lower units of the first member of the Shahejie Formation. Type Ⅱ crude oil was distributed in the Dongying Formation, Guantao Formation, and Minghuazhen Formation. It featured high Pr/Ph values and low tricyclic terpane content, and was mainly originated from mixed source rocks in the upper unit of the first member of the Shahejie Formation and the third member of the Dongying Formation. Discriminant analysis was applied to validate the oil and source correlation results, resulting in an initial classification accuracy of 100% and a cross-validation accuracy of 90.0%. These results indicated that the oil and source correlation results were reliable. The study reveals the promising application potential of multivariate statistical analysis method in source correlation for mixed-source oils.
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图 1 渤海湾盆地歧口凹陷构造单元(a)及地层综合柱状图(b)
Figure 1. Structural units (a) and stratigraphic composite column (b) of Qikou Sag, Bohai Bay Basin
图 2 渤海湾盆地歧口凹陷滨海地区烃源岩评价
Figure 2. Evaluation of source rocks in coastal area of Qikou Sag, Bohai Bay Basin
图 3 渤海湾盆地歧口凹陷滨海地区烃源岩饱和烃气相色谱、藿烷(m/z=191)、甾烷(m/z=217)质量色谱
Pr=姥鲛烷，Ph=植烷，Tri=三环萜烷，Tet=四环萜烷，Ts=18α(H)-22, 29, 30-三降藿烷，Tm=17α(H)-22, 29, 30-三降藿烷，C30H= C30藿烷，Ga=伽马蜡烷，Preg=孕甾烷，Homopreg=升孕甾烷，DiaC27=C27重排甾烷，C27-C28-C29=ααα20(R) 构型的C27-C28-C29规则甾烷。
Figure 3. Gas chromatograms of saturated hydrocarbons and mass chromatograms of hopanes (m/z=191) and steranes (m/z=217) in source rocks from coastal area of Qikou Sag, Bohai Bay Basin
图 4 渤海湾盆地歧口凹陷滨海地区原油饱和烃气相色谱、藿烷(m/z=191)、甾烷(m/z=217)质量色谱
Figure 4. Gas chromatograms of saturated hydrocarbons and mass chromatograms of hopanes (m/z=191) and steranes (m/z=217) in crude oils from coastal area of Qikou Sag, Bohai Bay Basin
图 5 渤海湾盆地歧口凹陷滨海地区不同降解程度原油饱和烃总离子流图(TIC)、藿烷(m/z=191)、甾烷(m/z=217)质量色谱
Figure 5. Total ion chromatograms (TIC) of saturated hydrocarbons and mass chromatograms of hopanes (m/z=191) and steranes (m/z=217) in crude oils with different biodegradation degrees from coastal area of Qikou Sag, Bohai Bay Basin
图 6 渤海湾盆地歧口凹陷滨海地区不同降解程度原油金刚烷(m/z=136)、甲基金刚烷(m/z=135)质量色谱
Figure 6. Mass chromatograms of adamantanes (m/z=136) and methyladamantanes (m/z=135) in crude oils with different biodegradation degrees from coastal area of Qikou Sag, Bohai Bay Basin
图 7 渤海湾盆地歧口凹陷滨海地区中浅层原油样品Pr/nC17、Ph/nC18与深度交汇图
Figure 7. Relationships between Pr/nC17 and Pr/nC18 ratios with depth for middle and shallow crude oil samples from coastal area of Qikou Sag, Bohai Bay Basin
图 8 渤海湾盆地歧口凹陷滨海地区中浅层原油、各层位烃源岩生标参数交汇图
a.甲基菲分布分数F1与F2关系，F1=[(2-MP)+(3-MP)]/[(1-MP)+(2-MP)+(3-MP)+(9-MP)]，F2=(2-MP)/[(1-MP)+(2-MP)+(3-MP)+(9-MP)]；b.C29ββ/(αα+ββ)与甾烷C2920S/(20S+20R)关系；c.伽马蜡烷指数(Ga/C30H)与Pr/Ph关系；d.C27-28-29(ααα20(R)C27/ααα20(R)(C27+C28+C29)、(ααα20(R)C28/ααα20(R)(C27+C28+C29)、(ααα20(R)C29/ααα20(R)(C27+C28+C29))三端元交汇图；e.生标参数折线图(Pr/Ph=姥鲛烷/植烷，Pr/nC17=姥鲛烷/正十七烷，Ph/nC18=植烷/正十八烷，TriC19/C21=三环萜烷C19/C21，TriC19/C23=三环萜烷C19/C23，Tri(19+20)/23=三环萜烷(C19+C20)/C23，TriC19-22/C23-26=三环萜烷C19-22/C23-26，TriC23/C30H×10=C23三环萜烷/C30藿烷×10，TriC26/C25=三环萜烷C26/C25，C31R/C30H=C31藿烷(22R)/C30藿烷，Ts/Tm=三降藿烷Ts/Tm，Ole指数×10=奥利烷/C30藿烷× 10，Ga指数×10=伽马蜡烷/C30藿烷×10，35/34-Hop=藿烷C35/C34，Ga/C31H22R=伽马蜡烷/C31藿烷(22R)，Ga/2×C29Hop=伽马蜡烷/2×C29藿烷，27/(27+ 28+29)=ααα20(R)C27/ααα20(R)(C27+C28+C29)甾烷，28/(27+28+29)=ααα20(R)C28/ααα20(R) (C27+C28+C29)甾烷，29/(27+28+29)=ααα20(R)C29/ααα20(R)(C27+C28+C29)甾烷。
Figure 8. Cross-plots of biomarker parameters for middle and shallow crude oils and source rocks from different strata in coastal area of Qikou Sag, Bohai Bay Basin
图 9 渤海湾盆地歧口凹陷滨海地区中浅层原油、各层位烃源岩聚类分析谱系图
Figure 9. Cluster analysis dendrogram of middle and shallow crude oils and source rocks from different strata in coastal area of Qikou Sag, Bohai Bay Basin
图 10 渤海湾盆地歧口凹陷滨海地区中浅层原油、各层位烃源岩主成分三维交汇图
Figure 10. 3D cross-plots of principal components for middle and shallow crude oils and source rocks from different strata in coastal area of Qikou Sag, Bohai Bay Basin
图 11 渤海湾盆地歧口凹陷滨海地区PC1、PC2、PC3主成分对应生标参数载荷分布直方图
Figure 11. Histogram of biomarker parameter loadings corresponding to principal components PC1, PC2, and PC3 in coastal area of Qikou Sag, Bohai Bay Basin
表 1 渤海湾盆地歧口凹陷滨海地区烃源岩地化特征
Table 1. Geochemical characteristics of source rocks in coastal area of Qikou Sag, Bohai Bay Basin
层位 ω(TOC)/% (S1+S2)/(mg/g) HI/(mg/g) Ro/% 沙三段 $\frac{{0.51 \sim 6.61}}{{1.21}} $ $\frac{{0.30 \sim 5.34}}{{2.14}} $ $\frac{{170.20 \sim 730.30}}{{323.56}} $ >1.00 沙一下亚段 $\frac{{0.50 \sim 11.07}}{{6.66}} $ $\frac{{0.80 \sim 32.04}}{{8.44}} $ $\frac{{183.72 \sim 685.28}}{{343.68}} $ 0.72~0.95 沙一中亚段 $\frac{{0.51 \sim 4.30}}{{1.56}} $ $\frac{{10.02 \sim 32.40}}{{13.99}} $ $\frac{{131.52 \sim 666.94}}{{474.91}} $ 0.78~1.37 沙一上亚段 $\frac{{0.55 \sim 3.50}}{{1.45}} $ $\frac{{1.82 \sim 23.42}}{{4.11}} $ $\frac{{174.19 \sim 960.00}}{{354.84}} $ 0.52~0.98 东三段 $\frac{{0.53 \sim 7.66}}{{1.54}} $ $\frac{{0.45 \sim 36.75}}{{5.81}} $ $\frac{{176.05 \sim 583.33}}{{355.64}} $ 0.55~0.65 注：表中公式含义为：$\frac{{最小值 \sim 最大值}}{{平均值}} $。 
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表 2 渤海湾盆地歧口凹陷滨海地区中浅层原油API度、沥青质、氮硫氧化合物、非烃数据
Table 2. API gravity, asphaltenes, NSO compounds, and non-hydrocarbon data of middle and shallow crude oils from coastal area of Qikou Sag, Bohai Bay Basin
井号 层位 深度/m API/(°) 沥青质与NSO化合物/% 非烃/% Q132 Nm 1 655 34 18.40 14.26 G8-23-1 Nm 1 221 13 40.71 29.30 G9-24-2 Nm 1 275 11 41.74 25.80 G6-24-1 Nm 1 514 23 22.59 16.48 B75 Nm 1 698 24 34.18 26.10 G516 Ng 1 972 31 18.57 11.72 G24 Ng 2 472 33 24.51 20.61 Q133-1 Ng 2 429 32 25.48 16.70 G71 Ng 1 780 23 37.85 29.13 G519 Ng 1 801 21 40.68 33.43 Z19-1 Ed1 2 886 30 20.71 16.97 Z20-30 Ed1 3 097 32 23.83 18.11 Z16 Ed2 3 153 33 19.61 15.47 G580 Ed2 1 611 20 32.44 23.65 GS27-1k Ed3 2 617 31 12.23 9.69 G561 Ed3 2 441 31 13.85 10.72 G556 Ed3 2 541 33 8.72 6.28 G528 Ed3 2 541 34 12.23 8.69 G508-12 Ed3 2 989 28 15.73 11.59 Z7 Ed3 3 020 33 23.27 18.53 MG1 Es1s 3 270 28 9.63 7.35 B1502 Es1z 3 020 29 12.33 9.19 B14-1 Es1x 3 551 35 15.77 13.43 GS33 Es1x 4 114 40 17.09 11.63 GS3 Es1x 3 502 34 17.39 14.11 GS3 Es1x 3 533 32 10.76 8.81 QN3 Es1x 3 324 30 23.31 18.12
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表 3 Fisher判别法分类结果
Table 3. Classification results by Fisher discriminant method
分类 预测的群组成员资格 总计/个 Ⅰ类 Ⅱ类 初始验证 计数/个 Ⅰ类 18.0 0.0 18.0 Ⅱ类 0.0 12.0 12.0 百分比/% Ⅰ类 100.0 0.0 100.0 Ⅱ类 0.0 100.0 100.0 交叉验证 计数/个 Ⅰ类 17.0 1.0 18.0 Ⅱ类 2.0 10.0 12.0 百分比/% Ⅰ类 94.4 5.6 100.0 Ⅱ类 16.7 83.3 100.0 初始验证：100.0 %的原始分组观察值已正确地分类。 交叉验证：90.0 %的交叉验证已分组观察值已正确地分类。
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