Characteristics and Geological Significance of Biomarker for the Upper Permian Dalong Formation Shale in Southern Anhui Province
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摘要: 为阐明下扬子皖南地区上二叠统大隆组页岩特征，通过对港地1井岩心进行取样，开展了大隆组页岩样品的有机地球化学测试、氩离子抛光—扫面电镜观察、矿物组成分析等工作.结果表明皖南地区大隆组页岩TOC含量为1.18%~4.35%，干酪根以Ⅰ型为主，少数为Ⅱ1型，Ro介于1.15%~1.29%，反映大隆组页岩整体处于成熟的生油气阶段.饱和烃气相色谱图呈典型的单峰型分布，正构烷烃主峰碳数分布在nC18~nC22之间，nC25+高碳数正构烷烃含量较低.规则甾烷的丰度整体上表现为C27≈C29>C28，属于V型分布，且高、低碳数的正构烷烃单体碳同位素δ13C相差较大（3.0‰~5.6‰），略高于单一来源的不同碳数正构烷烃的δ13C变化（一般小于1.6‰），反映大隆组页岩有机质主体来源于菌藻类等低等水生生物，局部存在陆源高等植物.TOC与TS的相关性、Pr/Ph比值、Pr/nC17-Ph/nC18图解共同指示皖南地区大隆组页岩形成于缺氧—贫氧环境，有利于有机质保存.Abstract: In order to elucidate shale characteristics of the Upper Permian Dalong Formation in southern Anhui Province in the Lower Yangtze, a total of 20 shale samples collected from Gangdi-1 Well were analyzed by conducting organic geochemical test, argon ion polishing-scanning electron microscopy (SEM) observation, and mineral composition analysis. Results show that total organic carbon (TOC) content for the Dalong Formation shale in southern Anhui Province is in the range of 1.18%-4.35%. The kerogen type is dominated by type Ⅰ and followed by type Ⅱ1. The vitrinite reflectance (Ro) is between 1.15% and 1.29%, demonstrating that the Dalong Formation shale is in a mature stage of hydrocarbon generation. Moreover, the Dalong Formation shale extracts display a full range of C11-C35 n-alkanes and acyclic isoprenoids. The chromatograms are characterized by a unimodal distribution of n-alkanes with carbon peak in the range of nC18-nC22 and low quantities of long-chain (nC25+) n-alkanes. Furthermore, the steranes are dominated by C27, C28, and C29 sterane homologs of regular steranes, with the following relative distributions: C27≈C29>C28 regular steranes, which belongs to the V-shaped distribution, indicating that the organic matters in Dalong Formation black shale are mainly originated from lower aquatic organisms (e.g., bacteria and algae) and followed by higher plants in a local area. This conclusion is also supported by the variations of the δ13C values of C13-C26 n-alkanes for the target samples being in the range of 3.0‰-5.6‰ offset, which is slightly higher than the corresponding value (1.6‰) of n-alkanes from a single source. In addition, the cross plot of TOC vs. TS as well as the Pr/Ph ratio and the Pr/nC17-Ph/nC18 diagram indicate that Dalong Formation black shale was mainly formed in a marine anoxic-dysoxic environment, which is beneficial to the preservation of organic matter.
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图 1 研究区范围及港地1井位置分布（据黄保家等，2013修改）
Fig. 1. The scope of the studied area and the location distribution of Gangdi-1 Well (modified from Huang et al., 2013)
图 2 港地1井上二叠统大隆组地层综合柱状图
Fig. 2. Stratigraphic column of the Upper Permian Dalong Formation according to Gangdi-1 Well
图 3 TOC与S2交汇图判别皖南地区上二叠统大隆组页岩品质
Fig. 3. Plot of TOC vs. S2 distinguishing the quality of the Upper Permian Dalong Formation shale in southern Anhui Province
图 4 皖南地区港地1井大隆组页岩矿物组成
a.全岩组成；b.黏土组成
Fig. 4. Mineral compositions of the Dalong Formation shale from Gangdi-1 Well in southern Anhui Province
图 5 港地1井大隆组页岩孔隙发育特征
a.有机孔大量发育，GD-1，984.9 m；b.有机孔，GD-6，971.7 m；c.图b局部放大，GD-6，971.7 m；d.有机孔大量发育，GD-7，967.5 m；e.有机孔和黏土矿物层间孔，GD-4，975.5 m；f.黏土矿物层间孔，GD-9，959.1 m；g.粒间孔，具纸房构造，GD-19，924.1 m；h.黏土矿物层间孔和有机质边缘收缩缝，GD-7，967.5 m；i.有机质边缘收缩缝，图h局部放大，GD-7，967.5 m
Fig. 5. Pore development characteristics of the Dalong Formation shale from Gangdi-1 Well
图 6 皖南地区港地1井上二叠统大隆组页岩饱和烃气相色谱图
Fig. 6. The m/z 85 mass fragmentograms of the saturated hydrocarbons for the Upper Permian Dalong Formation shale samples from Gangdi-1 Well in southern Anhui Province
图 7 港地1井上二叠统大隆组页岩饱和烃藿烷与甾烷气相色谱图
Fig. 7. Mass chromatograms of terpane (m/z 191) and sterane (m/z 217) in saturated hydrocarbon fractions of Dalong Formation shale samples from Gangdi-1 Well
图 8 皖南地区港地1井上二叠统页岩正构烷烃单体碳同位素分布曲线
Fig. 8. The δ13C values of individual C13-C26 n-alkanes in the selected samples from Gangdi-1 Well in southern Anhui Province
图 9 皖南地区上二叠统大隆组页岩Pr/nC17和Ph/nC18交汇图（底图据Rangel et al., 2017修改）
Fig. 9. Plot of Pr/nC17 versus Ph/nC18 of the Dalong Formation shale in southern Anhui Province (modified from Rangel et al., 2017)
图 10 皖南地区港地1井大隆组页岩规则甾烷C27-C28-C29三角图（底图据Hakimi et al., 2016修改）
Fig. 10. Ternary diagram of C27, C28 and C29 regular steranes of Dalong Formation rock samples from Gangdi-1 Well in southern Anhui Province (modified from Hakimi et al., 2016)
图 11 皖南地区港地1井上二叠统大隆组页岩TOC与TS交汇图
Fig. 11. Crossplot of TOC versus TS contents for Dalong Formation rock samples from Gangdi-1 Well in southern Anhui Province
表 1 皖南地区港地1井大隆组页岩有机地化参数
Table 1. Geochemical parameters of the Dalong Formation shale from Gangdi-1 Well in southern Anhui Province
样品编号 深度
(m)TOC
(%)TS
(%)Ro
(%)S1
(mg/g)S2
(mg/g)S3
(mg/g)Tmax
(℃)HI
(mg/g)S1+S2
(mg/g)PI GD-20 919.5 1.24 1.69 1.17 0.39 1.96 0.15 447 158.06 2.35 0.17 GD-19 924.1 1.18 2.74 1.24 0.35 1.35 0.18 448 114.41 1.70 0.21 GD-18 927.4 2.89 2.48 1.19 0.45 2.72 0.17 449 94.12 3.17 0.14 GD-17 930.5 2.18 2.67 1.16 0.33 1.42 0.18 452 65.14 1.75 0.19 GD-16 934.2 1.71 2.81 1.18 0.37 1.68 0.21 451 98.25 2.05 0.18 GD-15 937.8 1.70 2.84 1.21 0.47 1.73 0.21 450 101.76 2.20 0.21 GD-14 941.8 1.86 2.67 1.24 0.29 1.19 0.18 448 63.98 1.48 0.20 GD-13 945.9 2.81 1.65 1.15 0.51 2.00 0.22 453 71.17 2.51 0.20 GD-12 950.0 3.94 3.40 1.17 0.54 3.21 0.29 452 81.47 3.75 0.14 GD-11 953.5 2.05 2.82 1.25 0.41 1.52 0.16 450 74.15 1.93 0.21 GD-10 955.6 1.19 2.68 1.18 0.46 2.37 0.19 450 199.16 2.83 0.16 GD-9 959.1 3.52 2.63 1.20 0.58 3.72 0.24 453 105.68 4.30 0.13 GD-8 964.0 3.20 3.33 1.19 0.65 2.40 0.20 454 75.00 3.05 0.21 GD-7 967.5 3.68 3.02 1.24 0.22 0.81 0.27 455 22.01 1.03 0.21 GD-6 971.7 2.67 2.31 1.19 0.41 2.12 0.19 454 79.40 2.53 0.16 GD-5 973.7 3.05 2.94 1.17 0.61 2.67 0.25 452 87.54 3.28 0.19 GD-4 975.5 4.35 3.10 1.21 0.87 5.59 0.33 451 128.51 6.46 0.13 GD-3 979.3 2.02 1.19 1.20 0.37 1.61 0.14 455 79.70 1.98 0.19 GD-2 982.0 1.89 0.99 1.24 0.68 2.54 0.20 450 134.39 3.22 0.21 GD-1 984.9 3.54 1.80 1.29 0.90 4.33 0.28 453 122.32 5.23 0.17 平均值 2.53 2.49 1.20 0.49 2.35 0.21 451 97.81 2.84 0.18 
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表 2 皖南地区港地1井大隆组页岩样品干酪根显微组成
Table 2. Maceral compositions of the Dalong Formation shale samples from Gangdi-1 Well in southern Anhui Province
样品编号 组分含量(%) 类型指数 类型 腐泥组 壳质组 镜质组 惰质组 GD-20 90.7 1 7.5 0.8 84.8 Ⅰ GD-19 86.3 1 11.8 0.9 77.1 Ⅱ1 GD-18 88.4 0 10.4 1.2 79.4 Ⅱ1 GD-17 91.8 0 7.4 0.8 85.5 Ⅰ GD-16 89.6 1 8.3 1.1 82.8 Ⅰ GD-15 90.5 0 8.9 1.0 82.8 Ⅰ GD-14 90.2 0 8.4 1.4 82.5 Ⅰ GD-13 94.5 0 5.0 0.5 90.3 Ⅰ GD-12 91.2 0 8.1 0.7 84.4 Ⅰ GD-11 86.6 3 9.3 1.1 80.0 Ⅰ GD-10 89.7 1 8.5 0.8 83.0 Ⅰ GD-9 90.5 0 8.4 1.1 83.1 Ⅰ GD-8 89.4 0 9.4 1.2 81.2 Ⅰ GD-7 87.7 0 10.7 1.7 78.0 Ⅱ1 GD-6 89.9 0 8.9 1.2 82.0 Ⅰ GD-5 89.7 0 9.3 1.0 81.7 Ⅰ GD-4 88.9 0 10.3 0.8 80.4 Ⅰ GD-3 92.7 0 6.7 0.7 87.0 Ⅰ GD-2 81.5 0 16.7 1.8 67.2 Ⅱ1 GD-1 73.7 0 25.0 1.3 53.7 Ⅱ1 平均值 88.7 0.4 10.0 1.1 80.3
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表 3 皖南地区港地1井上二叠统大隆组页岩样品正构烷烃相关参数
Table 3. Biomarker parameters of normal alkanes (m/z 85) for the Upper Permian Dalong Formation shale samples from Gangdi-1 Well in southern Anhui Province
样品编号 主峰碳数 nC17/
nC31nC21-/
nC22+(nC21+nC22)/
(nC28+nC29)CPI OEP Pr/Ph Pr/nC17 Ph/nC18 GD-20 nC19 2.16 0.81 1.64 1.12 1.00 0.98 0.73 0.70 GD-19 nC19 2.24 0.83 1.52 1.09 1.01 1.06 0.80 0.72 GD-17 nC19 1.86 0.73 1.43 1.08 1.01 0.94 0.75 0.75 GD-15 nC20 2.33 0.79 1.52 1.09 1.00 0.92 0.67 0.68 GD-14 nC19 1.86 0.72 1.54 1.25 1.01 0.92 0.72 0.69 GD-13 nC20 2.74 0.93 1.68 1.14 1.00 1.06 0.76 0.68 GD-11 nC22 1.01 0.46 1.13 1.14 0.99 0.95 0.87 0.77 GD-10 nC19 1.89 0.64 1.69 1.13 1.01 0.88 0.62 0.59 GD-8 nC19 3.97 1.22 2.04 1.15 1.03 1.02 0.60 0.56 GD-7 nC21 1.17 0.55 1.39 1.15 1.01 0.83 0.54 0.52 GD-5 nC21 1.45 0.65 1.78 1.12 1.01 0.68 0.58 0.59 GD-3 nC19 1.71 0.68 1.52 1.09 1.01 0.86 0.64 0.63 GD-1 nC18 3.47 0.92 2.06 1.11 0.98 0.90 0.57 0.57 平均值 2.14 0.76 1.61 1.13 1.00 0.92 0.68 0.65
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表 4 皖南地区港地1井上二叠统大隆组页岩萜烷与甾烷类化合物相关参数
Table 4. Biomarker parameters of terpanes (m/z 191) and steranes (m/z 217) for the Upper Permian Dalong Formation shale from Gangdi-1 Well in southern Anhui Province
样品编号 C29/ C30H Tm/ Ts Ts/ (Ts+Tm) γ蜡烷/C30藿烷 三环萜烷/藿烷 规则甾烷(%) C27/ C29 C27 C28 C29 GD-20 0.32 0.52 0.68 0.20 0.85 39.05 26.37 34.58 1.13 GD-19 0.28 0.49 0.67 0.19 0.96 36.43 27.24 36.33 1.00 GD-17 0.31 0.60 0.63 0.21 1.05 37.37 25.32 37.31 1.00 GD-15 0.31 0.45 0.69 0.20 0.56 38.25 25.74 36.00 1.06 GD-14 0.37 0.42 0.70 0.20 0.42 37.87 25.98 36.15 1.05 GD-13 0.34 0.17 0.86 0.16 0.40 34.46 27.37 38.17 0.90 GD-11 0.30 0.37 0.73 0.20 0.37 35.42 26.65 37.93 0.93 GD-10 0.34 0.43 0.69 0.28 0.36 40.56 25.72 33.72 1.20 GD-8 0.40 0.18 0.85 0.18 0.45 38.61 26.90 34.48 1.12 GD-7 0.36 0.49 0.67 0.19 0.49 38.99 23.88 37.13 1.05 GD-5 0.35 0.76 0.57 0.20 0.64 42.36 24.99 32.65 1.30 GD-3 0.32 0.61 0.62 0.38 0.56 44.52 23.86 31.62 1.41 GD-1 0.33 0.76 0.57 0.47 0.52 39.31 24.19 36.50 1.08 平均值 0.33 0.48 0.69 0.24 0.59 38.68 25.65 35.67 1.09 注：C29为C29-降藿烷；C30H为C30-藿烷；Ts为C27 18α（H）-22，29，30-三降藿烷；Tm为C27 17α（H）-22，29，30-三降藿烷.
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表 5 皖南地区大隆组页岩与四川盆地典型页岩特征对比
Table 5. Comparison of the characteristics between Dalong Formation shale in southern Anhui Province and typical shales in Sichuan Basin
页岩层系 龙马溪组 大隆组 大隆组 区块或地区 焦石坝 长宁‒昭通 川东北 皖南 时代 奥陶系 奥陶系 二叠系 二叠系 典型钻井 焦页1HF 宁201-H1 乐坝1 港地1 沉积相 深水陆棚 深水陆棚、半深水陆棚 深水陆棚‒盆地相 深水陆棚、浅水陆棚 埋深(m) 2 250~3 500 2 300~3 200 2 500~6 000 800~2 500 优质页岩厚度TOC>2% (m) 38 37.8 15~40 12~35 TOC(%) 0.46~7.13/2.66 3.0~5.0/3.8 0.56~22.05/7.19 1.18~4.35/2.53 Ro(%) 2.42~2.80 2.14~2.87 1.49~2.99/2.15 1.15~1.29/1.20 有机质类型 Ⅰ-Ⅱ1 Ⅰ-Ⅱ1 Ⅰ-Ⅱ1 Ⅰ型为主，少数Ⅱ1型 孔隙度(%) 2.8~7.1/4.8 4.0~7.0/5.4 1.3~5.7/3.5 1.2~6.8/3.9 石英含量(%) 46.0~65.0/55.5 46.4 4.1~77.8/44.7 34.9~58.4/48.3 含气量(m3/t) 5.0~10.0/7.5 2.9~7.4/4.5 0.6~11.5/4.6 0.5~1.5 压力系数 1.6 1.2~2.0 1.4~1.7 / 天然裂缝发育程度 发育 不发育‒发育 一般 不发育 天然裂缝脉体类型 方解石脉和石英脉 方解石脉 方解石脉 方解石脉 改造强度 较弱 较弱 较强 强 注：“/”后为平均值；长宁‒昭通区块龙马溪组数据据梁兴等（2020）和马新华等（2020）汇编；川东北地区大隆组部分数据据王威等（2020）.
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