海相页岩芳烃演化规律及成熟度指示意义——来自西加拿大盆地二白斑组自然演化与热模拟样品的对比研究

葛祝时; 左兆喜; 肖七林; 郑伦举; 黄海平

doi:10.11781/sysydz202403590

海相页岩芳烃演化规律及成熟度指示意义——来自西加拿大盆地二白斑组自然演化与热模拟样品的对比研究

doi: 10.11781/sysydz202403590

1.
长江大学资源与环境学院, 武汉 430100
2.
中国石化石油勘探开发研究院无锡石油地质研究所, 江苏无锡 214126
3.
中国地质大学(北京) 能源学院, 北京 100083

基金项目:

国家自然科学基金企业创新发展联合基金“海相深层油气富集机理与关键工程技术基础研究” U19B6003

详细信息

作者简介:
葛祝时(1998—)，男，硕士生，地质学专业。E-mail：1469389687@qq.com

中图分类号: TE122.113
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出版历程
- 收稿日期: 2023-08-08
- 修回日期: 2024-04-10
- 刊出日期: 2024-05-28

Aromatic hydrocarbon evolution patterns and maturity indication significance of marine shale: a comparative study of naturally evolved and thermally simulated samples from the Second White Specks Formation of Cretaceous Colorado Group, Western Canada Basin

1.
College of Resources and Environment, Yangtze University, Wuhan, Hubei 430100, China
2.
Wuxi Research Institute of Petroleum Geology, SINOPEC, Wuxi, Jiangsu 214126, China
3.
School of Energy Resources, China University of Geosciences (Beijing), Beijing 100083, China

摘要

摘要: 选取西加拿大盆地白垩系科罗拉多群二白斑组低成熟海相页岩进行地层孔隙热解生烃模拟实验，利用GC-MS对自然演化系列样品和热模拟系列样品内的芳烃进行了定量分析，系统对比自然演化与热模拟样品芳烃地球化学特征。结果表明：(1)自然系列页岩三甲基萘和四甲基萘、菲和甲基菲绝对含量相对较高，且随着演化程度的增加而增加；热模拟系列页岩内菲和甲基菲绝对含量和变化趋势在较高的热演化程度下依然保持与自然系列相同，而三甲基萘和四甲基萘绝对含量相对较低且变化趋势不同，随成熟度增加表现为先增加后减少。(2)自然系列页岩三甲基萘指数(TMNR)值随埋深增加逐渐增大，而热模拟系列页岩TMNR值表现为先减小后增大；自然系列和热模拟系列页岩四甲基萘指数(TeMNR)值、甲基菲指数(MPI)值变化具有协同性，TeMNR值随成熟度的增加呈先减小后增大，MPI值随成熟度的增加而增加，表明菲系列化合物可有效指示热模拟和自然演化条件下页岩的成熟度。(3)热模拟实验在一定温度内能够较好地反演芳烃热演化历程，即：350 ℃之前热模拟页岩TMNR值与自然演化页岩的规律不同，350 ℃之后相同；425 ℃之前烷基菲相关参数与自然演化页岩的规律相同，超过425 ℃后与自然演化不同，这主要受温度达到临界值而导致芳烃演化机理改变以及升温速率和有机质赋存状态等因素的影响。
- 芳烃演化 /
- 成熟度 /
- 热模拟 /
- 海相页岩 /
- 白垩系 /
- 西加拿大盆地
Abstract: A pyrolysis hydrocarbon generation experiment was conducted on low-maturity marine shale from the Second White Specks (2WS) Formation of the Cretaceous Colorado Group in the Western Canada Basin. Using GC-MS, quantitative analysis of aromatics in naturally evolved and thermally simulated samples was performed to systematically compare the geochemical characteristics of aromatics in both sets of samples. The results indicated that: (1) In the naturally evolved series of 2WS shale, the absolute contents of trimethylnaphthalene (TMN), tetramethylnaphthalene (TeMN), phenanthrene (P) and methylphenanthrene (MP) were relatively higher andincreased with the degree of evolution. In the thermally simulated series, the absolute contents and trends of P and MP remained consistent with those of naturally evolved series at higher thermal evolution levels, whereas the absolute contents of TMN and TeMN were relatively lower and showed different trends, increasing initially and then decreasing with maturity. (2) The trimethylnaphthalene ratio (TMNR) values of the naturally evolved series increased gradually with burial depth, while the TMNR values of the thermally simulated series decreased initially and then increased. The tetramethylnaphthalene ratio (TeMNR) and methylphenanthrene index (MPI) values of both series showed a consistent pattern: TeMNR values decreased initially and then increased with maturity, while MPI values increased with maturity, suggesting that phenanthrene series compounds effectively indicated shale maturity under both thermal simulation and natural evolution conditions. (3) The thermal simulation experiment was capable of effectively replicating the thermal evolution process of aromatics within a certain temperature range. Specifically, TMNR values of the simulated shale deviated from the naturally evolved shale before 350 ℃ but became consistent after 350 ℃. Similarly, alkyl phenanthrenes-related parameters aligned with those of the naturally evolved shale before 425 ℃ but diverged significantly beyond 425 ℃. This divergence was primarily influenced by the change in aromatic evolution mechanisms when the temperature reached a critical value, as well as by factors such as heating rate and the state of organic matter.
- aromatic hydrocarbon evolution /
- maturity /
- thermal simulation /
- marine shale /
- Cretaceous /
- Western Canada Basin
注释:

利益冲突声明/Conflict of Interests

所有作者声明不存在利益冲突。

All authors disclose no relevant conflict of interests.

作者贡献/Authors’Contributions

郑伦举、黄海平参与实验设计；葛祝时、左兆喜完成实验操作；葛祝时、肖七林、左兆喜参与论文写作和修改。所有作者均阅读并同意最终稿件的提交。

The study was designed by ZHENG Lunju and HUANG Haiping. The experimental operation was completed by GE Zhushi and ZUO Zhaoxi. The manuscript was drafted and revised by GE Zhushi, Xiao Qilin and ZUO Zhaoxi. All authors have read the last version of the paper and consented to its submission.

HTML全文

图 1 西加拿大盆地上白垩统科罗拉多群二白斑组采样位置

据SYNNOTT等修改^[17]。

Figure 1. Sampling locations of Second White Specks Formation of Cretaceous Colorado Group, Western Canada Basin

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图 2 西加拿大盆地自然演化与热模拟页岩样品R_o随成熟度变化

Figure 2. Variations of R_o with maturity of naturally evolved and thermally simulated shale samples from Western Canada Basin

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图 3 西加拿大盆地自然演化和热模拟页岩样品质量色质图(m/z 170和m/z 184)

Figure 3. Mass chromatogram (m/z=170 and m/z=184) of naturally evolved and thermally simulated shale samples from Western Canada Basin

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图 4 西加拿大盆地自然演化(a)与热模拟(b)页岩样品质量色质图(m/z 192)

Figure 4. Mass chromatogram (m/z=192) of naturally evolved and thermally simulated shale samples from Western Canada Basin

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图 5 西加拿大盆地自然演化与热模拟页岩样品中萘系列化合物绝对含量变化

Figure 5. Variations in absolute content of naphthalene series in naturally evolved and thermally simulated shale samples from Western Canada Basin

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图 6 西加拿大盆地自然演化与热模拟页岩样品菲系列化合物绝对含量变化

Figure 6. Variations in absolute content of phenanthrene series in naturally evolved and thermally simulated shale samples from Western Canada Basin

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图 7 西加拿大盆地自然演化与热模拟页岩样品甲基萘系列参数变化

Figure 7. Variations of methyl naphthalene series parameters in naturally evolved and thermally simulated shale samples from Western Canada Basin

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图 8 西加拿大盆地自然演化与热模拟页岩样品甲基菲相对含量和MPI₁指数变化

Figure 8. Variations of relative abundance and MPI-1 of various isomers of methylphenanthrene with depth/temperature in naturally evolved and thermally simulated shale samples from Western Canada Basin

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图 9 西加拿大盆地热模拟系列样品菲系列化合物参数变化趋势

Figure 9. Trend of variations in parameters of phenanthrene series compounds in thermally simulated series samples from Western Canada Basin

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表 1 西加拿大盆地上白垩统科罗拉多群二白斑组页岩自然系列及热模拟系列原始样品烃源岩特征

Table 1. Hydrocarbon source rock characteristics of original samples from naturally evolved and thermally simulated series from Second White Specks Formation of Cretaceous Colorado Group, Western Canada Basin

井号	深度/m	样品数量	有机碳含量/%	生烃潜量/(mg/g)	R_o/%	T_max/℃
1^*	510.00	1	5.85	25.27	0.49	406
1	502.65~545.32	13	1.83~10.04(5.69)	7.82~53.45(24.92)	0.50	400~432(412)
2	736.50~745.50	5	3.66~7.44(5.50)	10.62~45.70(26.68)	0.56	412~433(417)
3	989.55~996.47	5	1.07~4.49(3.73)	2.26~23.53(17.87)	0.60	411~416(414)
4	1 211.75~1 217.55	3	4.82~7.66(6.05)	28.22~44.23(34.11)	0.66	421~429(424)
5	1 899.80~1 911.50	5	0.85~1.6(1.18)	1.70~3.05(2.23)	0.81~0.86(0.84)	445~447(445)
6	2 602.55~2 638.00	12	1.51~2.8(2.11)	2.54~7.29(4.12)	1.18~1.25(1.20)	448~457(453)
7	2 768.25~3 047.55	49	1.08~3.19(1.94)	0.81~4.87(2.51)	1.36~1.90(1.63)	442~466(456)
注：表中数据意义为最小值~最大值(平均值)；*代表热模拟系列的原始样品。

下载: 导出CSV

表 2 西加拿大盆地热模拟样品萘、菲参数

Table 2. Parameters of methylphenanthrene in thermally simulated samples from Western Canada Basin

温度/℃	R_o/%	TMNR	TeMNR	(9+1)-/ (3+2)-MP	2, 3-/ 1, 9-DMP	(2, 3+1, 9)-/ (1, 8+1, 2)-DMP	MPI₁	MPI₂
200	0.51	0.32	0.51	1.97	0.52	1.21	0.41	0.43
225	0.54	0.33	0.49	1.58	0.59	1.19	0.49	0.52
250	0.59	0.34	0.51	1.64	0.84	1.06	0.47	0.51
275	0.65	0.24	0.45	1.59	1.04	0.79	0.56	0.63
300	0.76	0.23	0.41	1.38	1.03	0.66	0.67	0.79
310	0.81	0.22	0.44	1.33	1.47	0.64	0.71	0.89
325	0.93	0.22	0.41	1.18	1.51	0.75	0.82	1.04
350	1.10	0.20	0.41	1.02	1.77	0.95	0.92	1.16
375	1.49	0.29	0.59	0.72	2.60	0.98	1.24	1.53
400	1.86	0.53	0.67	0.53	5.42	1.15	1.45	1.72
425	2.15	-	1.00	0.22	17.57	3.09	1.78	2.12
450	2.28	-	-	0.11	13.02	2.93	0.96	1.12
注：TMNR=(1, 3, 7-)/(1, 3, 7-+1, 2, 5-)TMN；TeMNR=1, 3, 6, 7-TeMN/[1, 3, 6, 7+(1, 2, 5, 6+1, 2, 3, 5)-TeMN]；MPI₁=1.5×(2-MP+3-MP)/(P+1-MP+9-MP)；MPI₂=3×(2-MP)/(P+1-MP+9-MP)。

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