海相高过成熟页岩芳烃特征及页岩气意义

王保忠; 王传尚; 汪啸风; 彭中勤; 危凯

doi:10.3799/dqkx.2019.143

海相高过成熟页岩芳烃特征及页岩气意义

doi: 10.3799/dqkx.2019.143

王保忠^1,2, ,,
王传尚^1,2, ,,
汪啸风¹,
彭中勤¹,
危凯¹

1.
武汉地质调查中心地层古生物研究室, 湖北武汉 430205
2.
中国地质调查局古生物与生命-环境协同演化重点实验室, 湖北武汉 430205

基金项目:

中国地质调查项目 DD20160179

详细信息

作者简介:
王保忠(1980-), 男, 博士, 主要从事油气地质综合研究工作

通讯作者:
王传尚

中图分类号: P618
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出版历程
- 收稿日期: 2019-06-16
- 刊出日期: 2019-11-15

Characteristics of Aromatic Compounds in High-over Matured Marine Shale and Its Significance to Shale Gas

1.
Stratigraphic Paleontology Laboratory, Wuhan Center of China Geological Survey, Wuhan 430205, China
2.
Key Laboratory of Paleontology and Life-Environment Co-Evolution of China Geological Survey, Wuhan 430205, China

摘要

摘要: 为了合理评价我国南方下古生界页岩有机质热演化程度，研究其与页岩含气性关系；采用气相色谱-质谱联用仪对中扬子地区6口调查井、3个露头剖面的20件页岩样品的芳烃馏分进行了分析，并对代表不同区域的6件样品进行显微激光拉曼测试.分析结果显示拉曼D、G峰参数可以很好地计算过成熟至球粒石墨阶段高演化样品的有机质成熟度；拉曼D峰的子峰包含有芳烃含量的重要信息，随着有机质热演化程度的增加，与芳烃含量有关的D₄子峰强度不断降低.芳烃中菲系列化合物和二苯并噻吩系列化合物在_RmcR_o=2.73%~4.67%范围内的演化具有明显规律性；虽然甲基菲成熟度公式在该阶段已经不适用，但表征3-MP+2-MP相对含量的参数F1仍是很好的有机质成熟度指标；在有机质过成熟演化阶段，F1先随成熟度增加逐渐增加至0.74附近（R_o=3%附近），之后随成熟度增加逐渐减小.二苯并噻吩化合物参数2，4-/1，4-DMDBT和4，6-/1，4-DMDBT在过成熟阶段随成熟度增加而增大，两值分别增至2和4.5时对应页岩等效镜质体反射率为4%.页岩芳烃系列化合物在过成熟阶段随有机质热演化程度增加而发生的异构化作用和脱甲基作用与有机质的比表面积变化有较好的耦合作用，与页岩气调查井的气显情况也有较好的相关性；页岩芳烃特征对过成熟阶段页岩气的生成具有重要的指示意义，可以作为我国南方下古生界有机质过成熟地区页岩气勘探的有效指标.
- 芳香烃 /
- 菲系列 /
- 热成熟度 /
- 拉曼光谱 /
- 页岩气 /
- 油气地质
Abstract: In order to evaluate the thermal evolution degree of organic matter of Lower Paleozoic shale in South China and discuss its relationship with shale gas, gas chromatography-mass spectrometry analysis of aromatic compounds in 20 shale samples collected from 6 investigation wells and 3 outcrop profiles in the Central Yangtze region was made, and 6 samples representing different regions were determined by laser Raman spectroscopy. The results show that the parameters of Raman D and G bands can be used to calculate the maturity of organic matter from over-maturity to spheroidal graphite stage. The sub-bands of D band contain important information of aromatics content. The strength of D₄ sub-band, which is related to aromatics content, decreases with the increase of thermal evolution degree of organic matter. The evolution regularities of phenanthrene series compounds and dibenzothiophene series compounds are remarkable in the range of _RmcR_o=2.73%-4.67%. Although the formula for maturity of methylphenanthrene is no longer applicable in this stage, the parameter F₁ which characterizes the relative content of 3-MP+2-MP is still a good maturity index of organic matter. F1 gradually increases to about 0.74(R_o=3%) firstly, and then decreases with the increase of maturity at the over-maturity stage. The parameters of dibenzothiophene compounds, 2, 4-/1, 4-DMDBT and 4, 6-/1, 4-DMDBT, increase with maturity at the over-maturity stage. When the two ratios are 2 and 4.5 respectively, the Raman reflectance value of shale is _RmcR_o=4%. The isomerization and demethylation of aromatic hydrocarbon series compounds occur with the increase of thermal evolution degree of organic matter in the over-mature stage, which has a good coupling effect with the change of specific surface area of organic matter and a good correlation with analytical gas about investigation wells. The characteristics of aromatic hydrocarbon compounds have important indicative significance for shale gas generation at the over-mature stage, and can be used as an effective index for shale gas exploration in over-mature areas of Lower Paleozoic in South China.
- aromatic hydrocarbon /
- phenanthrene series /
- thermal maturity /
- Raman spectra /
- shale gas /
- petroleum geology

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图 1 样品位置分布

Fig. 1. Sample location map

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图 2 不同热演化程度页岩拉曼光谱图

Fig. 2. Raman spectra of shale with different thermal evolution degrees

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图 3 典型样品菲系列及二苯并噻吩系列图谱

Fig. 3. Chromatograms about phenanthrene series and dibenzothiophene series of typical samples

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图 4 菲系列化合物各参数关系

Fig. 4. Parameter diagrams of phenanthrene series compounds

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图 5 不同演化程度样品菲系列质量色谱图

Fig. 5. Chromatographic charts of phenanthrene series of samples with different evolution degrees

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图 6 样品二苯并噻吩系列相关参数关系

Fig. 6. Parameter relationships of dibenzothiophene series in samples

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图 7 中扬子地区主要调查井芳烃特征在孔隙演化序列中的位置

Fig. 7. The position of aromatic hydrocarbon characteristics in pore evolution sequence of main survey wells in Central Yangtze area

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表 1 样品的拉曼光谱参数及计算反射率

Table 1. Raman spectral parameters and calculated reflectance for samples

样品	拉曼峰	拉曼位移 (cm^-1)	峰高	半高宽	峰面积	峰间距 (G-D)	计算反射率（%）
LZ-C₁lz-1	D	1 339.72	25 907.80	166.830 0	1.80E+06	259.52	2.73
	G	1 599.24	39 319.10	55.610 0	926 298
	D′
YD5-∈₁sh-1	D	1 337.76	31 831.00	227.260 0	3 012 300	261.04	2.82
	G	1 598.80	44 359.00	61.420 0	1 160 220
	D′	/	/	/	/
YD4-∈₁n-1	D	1 331.62	29 028.00	165.830 0	2.02E+06	270.25	3.31
	G	1 601.87	38 762.00	49.140 0	812 297
	D′	/	/	/	/
XZD1-Z₂dy-1	D	1 334.69	45 475.00	135.124 0	2.59E+06	257.97	3.97*
	G	1 592.66	43 778.60	61.420 2	1.15E+06
	D′
XXD2-∈₁n-1	D	1 340.83	42 464.70	79.846 2	1.44E+06	245.68	4.67*
	G	1 586.51	25 881.40	79.846 2	878 014
	D′
XPN-∈₁n-1	D	1 346.97	40 254.40	55.278 1	9.48E+05	233.40
	G	1 580.37	26 715.40	49.136 0	5.60E+05
	D′	2 685.93	9 890.30	85.987 8	359 078
注：计算公式据Liu et al.（2012）；带*值采用_RmcR_o%=1.165 9h(Dh/Gh)+2.758 8计算（当D峰高大于G峰时），其余采用_RmcR_o%=0.053 7d(G-D)-11.21.

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表 2 样品菲系列、二苯并噻吩系列化合物主要参数

Table 2. Main parameters of phenanthrene series and dibenzothiophene series compounds for samples

样品编号	MPR-1	MPR-2	MPI-1	DMP	F1	R_c1	MDR	MDR-1	MDR-2，3	MDR-4	24/14	46/14	R_c2
LZ-C₁lz-4	2.40	0.67	0.75	0.54	0.62	1.85	5.97	0.28	0.94	1.66	1.36	2.80	1.38
LZ-C₁lz-3	3.11	0.83	1.25	0.67	0.69	1.55	13.38	0.18	1.42	2.35	1.19	2.26	1.59
LZ-C₁lz-2	3.83	0.74	2.04	0.76	0.72	1.08	19.43	0.32	3.66	6.15	1.55	2.41	1.69
LZ-C₁lz-1	4.07	0.70	2.11	0.74	0.73	1.03	19.76	0.30	3.83	5.98	1.68	2.56	1.70
YD1-S₁l-2	2.57	0.65	0.82	1.45	0.64	1.81	6.00	0.18	0.61	1.07	1.30	2.26	1.38
YD1-S₁l-1	2.77	0.85	1.15	1.64	0.69	1.61	8.05	0.22	1.16	1.78	1.37	2.73	1.46
YD5-∈₁sh-2	2.92	0.85	0.80	1.42	0.70	1.82	4.09	0.14	0.50	0.56	1.21	2.35	1.28
YD5-∈₁sh-1	3.33	0.86	0.81	1.65	0.72	1.81	3.77	0.11	0.40	0.40	1.45	2.16	1.26
YD2-∈₁sh-2	3.94	0.76	0.40	1.73	0.74	2.06	5.83	0.03	0.11	0.19	1.11	2.21	1.37
YD2-∈₁sh-1	3.54	0.90	0.75	1.56	0.74	1.85	12.07	0.07	0.46	0.84	1.64	3.18	1.57
YD4-∈₁n-1	2.75	0.94	0.39	1.40	0.70	2.06	3.91	0.22	0.40	0.86	0.97	1.91	1.27
YD4-Z₂l-1	2.02	0.76	0.50	1.26	0.60	2.00	8.70	0.14	0.63	1.25	1.21	2.65	1.48
XZD1-∈₁n-1	2.02	0.62	0.51	1.33	0.58	2.00	18.47	0.08	0.69	1.42	1.76	4.14	1.68
XZD1-Z₂dy-1	1.93	0.53	0.23	1.10	0.55	2.16	9.60	0.15	0.63	1.48	2.03	4.56	1.51
YL-Z₂l-2	1.58	0.87	0.96	1.28	0.55	1.72	2.48	1.13	1.79	2.80	1.09	2.19	1.15
YL-Z₂l-1	1.90	0.86	1.00	1.32	0.59	1.70	6.11	0.71	3.46	4.31	1.58	2.74	1.39
XXD2-∈₁n-2	1.32	0.75	0.45	1.25	0.50	2.03	14.22	0.11	0.73	1.62	2.83	6.73	1.61
XXD2-∈₁n-1	2.42	0.54	0.47	1.57	0.59	2.02	13.26	0.11	0.63	1.41	2.21	5.18	1.59
XPN-∈₁n-2	1.74	0.68	0.32	1.26	0.54	2.11	2.50	0.23	0.30	0.56	/	/	1.15
XPN-∈₁n-1	/	/	1.22	/	0.88	1.57	4.48	0.13	0.35	0.56	/	/	1.30
注：MPR-1=1-MP/P; MPR-2=2-MP/P; MPI-1=1.5× (3-MP+2-MP)/(P+1-MP+9-MP); DMP=[(3, 5+2, 6)-DMP+2, 7-DMP]/[(2, 10+1, 3+3, 10+3, 9)-DMP+(1, 6+2, 9+2, 5)]; F1=(3-MP+2-MP)/(3-MP+2-MP+9-MP+1-MP); MDR=4-DBT/1-DBT; R_c1=-0. 6×MPI-1+2.3；R_c2=-0. 266 3×ln(MDR)+0.903 4.

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