南堡凹陷原油高分辨质谱特征及其地球化学意义

万中华; 李素梅; 王政军; 任苗颂; 张红臣; 孟祥兵; 孙爱艳

doi:10.3799/dqkx.2015.164

南堡凹陷原油高分辨质谱特征及其地球化学意义

doi: 10.3799/dqkx.2015.164

万中华^1,,
李素梅^{1, 2, ,},
王政军³,
任苗颂³,
张红臣³,
孟祥兵^{1, 2, 4},
孙爱艳³

1.
中国石油大学油气资源与探测国家重点实验室, 北京 102249
2.
中国石油大学盆地与油藏研究中心, 北京 102249
3.
中国石油冀东油田公司勘探开发研究院, 河北唐山 063004
4.
中国石油新疆油田分公司重油开发公司, 新疆克拉玛依 834000

基金项目:

国家重大专项基金项目 2011ZX05006-006-02-006

国家自然科学基金项目 41473047

教育部高等学校博士学科点专项科研基金项目 20120007110002

中国石油大学油气资源与探测国家重点实验室基金项目 PRP/indep-1-1101

详细信息

作者简介:
万中华(1986-), 男, 博士研究生, 主要从事化石能源形成与富集机制研究.E-mail: wan007.hi@163.com

通讯作者:
李素梅, E-mail: smli@cup.edu.cn

中图分类号: P618.13
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出版历程
- 收稿日期: 2015-06-06
- 刊出日期: 2015-11-15

Characterization of Crude Oils from Nanpu Depression by High Resolution Mass Spectrometry and Its Geochemical Significance

1.
State Key Laboratory of Petroleum Resources and Prospecting, China University of Petroleum, Beijing 102249, China
2.
Research Center of Basin and Reservoir, China University of Petroleum, Beijing 102249, China
3.
Research Institute of Exploration and Development, Jidong Oilfield Company, PetroChina, Tangshan 063004, China
4.
Heavy Oil Development Company, Xinjiang Oilfield, PetroChina, Karamay 834000, China

摘要

摘要: 南堡凹陷深部油气资源丰富, 油气成因研究薄弱.首次采用高分辨质谱(负离子电喷雾离子源(electrospray ionization, 简称ESI)傅里叶变换离子回旋共振质谱(Fourier transform ion cyclotron resonance mass spectrometry, 简称FT-ICR MS)技术对南堡凹陷原油中杂原子化合物的组成与分布特征及其地球化学意义进行了研究.应用负离子ESI FT-ICR MS检测出9种主要杂原子组合类型, 分别为N₁、N₁O₁、N₁O₂、N₁O₃、N₂、O₁、O₂、O₃和O₄类, 其中N₁、O₁和O₂类在所有样品中普遍存在且相对丰度较高.经研究发现成熟度对原油中N₁、O₁类化合物碳数分布、缩合度有明显的控制作用.实验观察到N₁类DBE(等效双键数)=12, 15的高低分子量同系物相对丰度参数C_16-20/C_21-50-DBE₁₂-N₁和C_20-24/C_25-50-DBE₁₅-N₁、N₁类缩合度参数DBE₁₂/DBE₉-N₁及O₁类缩合度参数DBE_8-9/DBE₄-O₁与成熟度指标Ts/Tm、TMNr具有良好的相关性, 认为它们可作为该区原油成熟度评价指标, 反映烃类演化的热动力学原理.南堡凹陷不同层系原油高分辨质谱特征有明显差异, 指示其可应用于母源岩性质识别.综合研究认为, FT-ICR MS在成熟度评价、油气成因与油源识别等方面地球化学意义显著, 其在油气地球化学理论研究和油气勘探中具有潜在的应用价值.
- 南堡凹陷 /
- 原油 /
- 高分辨质谱 /
- 成熟度 /
- 地球化学.
Abstract: Nanpu depression is abundant in deep oil and gas resources, but the origin of the hydrocarbon is still unclear. High resolution mass spectrometry (negative-ion electrospray ionization (ESI) Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS)) is utilized to carry out the composition and distribution of heteroatom compounds of crude oils from the Nanpu depression and its geochemical significance for the first time. The heteroatoms, N₁, N₁O₁, N₁O₂, N₁O₃, N₂, O₁, O₂, O₃ and O₄ class species, were identified by negative-ion ESI FT-ICR MS. And N₁, O₁, O₂ class species are universal in all samples with higher relative abundance. It is found that thermal maturity obviously controls the distribution of carbon numbers and the degree of condensation of N₁ and O₁ class species. It is observed that parameters like C_16—20/C_21—50-DBE₁₂-N₁, C_20—24/C_25—50-DBE₁₅-N₁, DBE₁₂/DBE₉-N₁ and DBE_8—9/DBE₄-O₁ have a good correlation with Ts/Tm and TMNr. They could be used as indicators of thermal maturity of crude oils in the depression, reflecting the kinetics of thermal evolution of hydrocarbons. Significant difference was found among different layers of oils detected by negative-ion ESI FT-ICR MS, indicating that it can be applied to characterize source rocks. After a comprehensive investigation, we believe that FT-ICR MS technique is applicable in multiple geochemical aspects, such as maturity level estimation and source rock and relevant hydrocarbons determination. FT-ICR MS is significant in both the compositional characterization of the NSO compounds and the application in petroleum exploration.
- Nanpu depression /
- crude oil /
- high resolution mass spectrometry /
- maturity /
- geochemisitry.

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图 1 南堡凹陷区域构造单元与采样点分布

Fig. 1. Tectonic units of the Nanpu depression and location of the oils collected

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图 2 南堡凹陷原油杂原子化合物类型及其相对丰度

Fig. 2. Relative abundance of heteroatom class species in the crude oils from the Nanpu depression

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图 3 南堡凹陷原油中N₁系列化合物碳数、DBE及其强度关系

Fig. 3. Relation of DBE versus the carbon number of the N₁ class in crude oils by negative-ion ESI FT-ICR MS from the Nanpu depression

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图 4 南堡凹陷第三系原油、潜山原油中N₁类化合物DBE系列的分布特征

Fig. 4. Distribution characteristics of the N₁ compounds with different DBE values for Tertiary oils (a) and buried hill oils (b) from the Nanpu depression

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图 5 南堡凹陷原油中不同DBE系列的N₁类化合物碳数分布特征

Fig. 5. Carbon curve of the N₁ class with DBE=9, 12 and 15 in the selected oils from the Nanpu depression

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图 6 南堡凹陷原油中O₁系列化合物碳数、DBE及其强度关系

Fig. 6. Relation of DBE versus the carbon number of the O₁ class in crude oils by negative-ion ESI FT-ICR MS from the Nanpu depression

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图 7 南堡凹陷原油中不同DBE系列的O₁类化合物分布特征

Fig. 7. Distribution characteristics of the O₁ compounds with different DBE values for the oils studied from the Nanpu depression

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图 8 南堡凹陷原油中不同DBE系列的O₁类化合物碳数分布特征

Fig. 8. Carbon curve of the O₁ class with DBE=4, 8 and 9 in selected oils from the Nanpu depression

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图 9 南堡凹陷原油中脂肪酸类化合物碳数分布特征

Fig. 9. Distribution pattern of carbon numbers of fatty acids in the selected oils

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图 10 南堡凹陷原油N₁、O₁类化合物高分辨质谱参数与色质参数关系

Fig. 10. Cross plots of FT-ICR MS parameters with GC-MS parameters of the N₁ and O₁ classes in the oils studied from the Nanpu depression

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表 1 南堡凹陷原油色谱、色谱-质谱参数

Table 1. GC and GC-MS parameters of the selected oils from the Nanpu depression

编号	井号	井段(m)	层位	CPI	OEP	Pr/Ph	20S	αββ	Ts/Tm	Tri-/Pent	G/C₃₀H	4-m/C₂₉St	C_21—22/C_27—29St	Dia/Reg	TMNr
1	G89-4	3385.9~3700.2	Es₃	1.09	1.07	1.48	0.57	0.38	0.72	0.119	0.046	0.699	0.046	0.171	0.390
2	GC30-28	3203.0~3666.8	Es₃	1.09	1.08	1.36	0.54	0.44	1.33	0.074	0.046	1.117	0.037	0.185	0.419
3	G19	3608.2~4040.8	Es₃	1.08	1.05	1.38	0.52	0.47	1.52	0.079	0.048	1.081	0.036	0.206	0.431
4	NP23-P2201	2824.4~3020.0	Ng	1.17	1.03	1.46	0.41	0.36	0.93	0.055	0.145	0.357	0.032	0.186	0.605
5	NP203X1	2595.0~3148.6	Ng	1.14	1.09	1.37	0.46	0.39	0.92	0.088	0.098	0.382	0.033	0.189	0.666
6	NP32-X3212	2700.8~2703.0	Ng	1.14	1.15	1.42	0.54	0.45	1.73	0.052	0.060	0.088	0.032	0.319	0.579
7	NP4-19	1877.0~1879.0	Ng	1.13	1.09	1.48	0.54	0.42	1.38	0.077	0.093	0.335	0.037	0.315	0.667
8	G66-28	2625.0~2634.0	Ed₁	1.14	1.05	1.65	0.47	0.39	1.02	0.060	0.066	0.314	0.029	0.285	0.392
9	NP32-X3015	3734.2~3789.8	Ed₁	1.17	1.05	1.61	0.57	0.46	1.81	0.057	0.059	0.105	0.036	0.329	0.493
10	B26-2	2294.0~2298.0	Ed₁	1.13	1.07	1.61	0.53	0.44	1.75	0.064	0.078	0.307	0.036	0.307	0.533
11	B26-6	2734.0~2909.0	Ed₁	1.14	1.08	1.56	0.51	0.44	1.92	0.066	0.081	0.353	0.036	0.345	0.559
12	NP1	2379.8~2410.0	Ed₁	1.10	1.01	1.39	0.55	0.42	1.09	0.169	0.275	0.326	0.055	0.237	0.680
13	NP4-31	3932.2~3960.6	Ed₂	1.13	1.03	1.48	0.48	0.41	1.08	0.076	0.108	0.356	0.032	0.285	0.567
14	NP280	4575.0~4600.0	O	1.08	1.03	1.34	0.62	0.55	4.94	0.447	0.136	0.460	0.077	0.381	0.766
15	NP23-P2009	5182.7~5452.0	O	1.08	1.08	1.25	0.60	0.53	6.20	0.409	0.158	0.426	0.087	0.388	0.920
16	NP23-P2002	4875.0~5150.0	O	1.07	1.06	1.19	0.60	0.53	7.48	0.40	0.149	0.436	0.085	0.403	0.925
17	PG2	5165.2~5192.0		1.12	1.04	1.69	0.62	0.53	6.31	0.698	0.182	0.094	0.189	0.601	0.953
注：CPI.碳优势指数；OEP.奇偶优势比；Pr/Ph.姥鲛烷/植烷；20S.C₂₉甾烷ααα20S/(S+R)；αββ.C₂₉甾烷αββ/(ααα+αββ)；Ts/Tm.18α(H)-/17α(H)-三降藿烷；Tri-/Pent.三环萜烷/五环萜烷；G/C₃₀H.伽马蜡烷/C₃₀藿烷；4-m/C₂₉St.4-甲基甾烷/C₂₉规则甾烷；C_21—22/C_27—29St.C_21—22/C_27—29甾烷；Dia/Reg.重排甾烷/规则甾烷；TMNr.三甲基萘指数=1, 3, 7-/(1, 3, 7-+1, 2, 5-)三甲基萘.

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表 2 南堡凹陷原油负离子ESI FT-ICR MS参数

Table 2. Basic parameters of the oils analyzed by negative-ion ESI FT-ICR MS from the Nanpu depression

编号	井号	层位	含量(%)									A	B	C	D
编号	井号	层位	N₁	N₁O₁	N₁O₂	N₁O₃	N₂	O₁	O₂	O₃	O₄	A	B	C	D
1	G89-4	Es₃	56.17	4.35	0.0	0.0	0.0	19.26	20.22	0.0	0.0	0.046	0.113	0.720	0.669
2	GC30-28	Es₃	63.96	4.81	0.0	0.55	0.0	19.81	10.86	0.0	0.0	0.061	0.142	0.738	0.545
3	G19	Es₃	63.59	3.35	0.0	0.0	0.0	17.32	13.38	0.0	2.36	0.085	0.187	0.774	0.651
4	NP23-P2201	Ng	49.60	3.77	2.76	0.0	0.0	28.06	15.81	0.0	0.0	0.054	0.076	0.603	0.422
5	NP203X1	Ng	49.47	2.65	0.0	0.0	0.0	29.32	18.55	0.0	0.0	0.049	0.080	0.784	0.525
6	NP32-X3212	Ng	60.63	3.24	0.50	0.0	0.0	21.42	14.21	0.0	0.0	0.040	0.090	1.021	0.922
7	NP4-19	Ng	56.0	4.21	1.64	0.0	0.0	29.23	8.92	0.0	0.0	0.050	0.098	0.793	0.528
8	G66-28	Ed₁	35.52	3.66	2.05	0.33	0.0	35.62	20.38	2.43	0.0	0.020	0.041	0.677	0.284
9	NP32-X3015	Ed₁	67.80	4.89	1.84	0.0	0.0	20.14	5.33	0.0	0.0	0.102	0.185	0.927	0.397
10	B26-2	Ed₁	49.40	3.51	0.0	0.0	0.0	34.26	12.82	0.0	0.0	0.040	0.059	0.688	0.394
11	B26-6	Ed₁	48.66	4.34	0.0	0.0	0.0	36.89	10.11	0.0	0.0	0.054	0.082	0.631	0.413
12	NP1	Ed₁	30.95	6.43	4.69	0.0	0.0	12.41	45.52	0.0	0.0	0.064	0.124	0.898	1.084
13	NP4-31	Ed₂	44.69	3.26	0.71	0.0	0.0	43.49	7.86	0.0	0.0	0.061	0.079	0.734	0.347
14	NP280	O	77.20	4.92	0.0	0.0	0.55	12.13	5.20	0.0	0.0	0.263	0.469	1.280	1.613
15	NP23-P2009	O	75.14	1.77	0.0	0.0	0.0	18.28	3.89	0.68	0.25	0.129	0.293	1.297	1.649
16	NP23-P2002	O	73.59	3.63	0.0	0.0	0.0	17.82	4.97	0.0	0.0	0.131	0.302	1.265	1.597
17	PG2		31.24	1.31	0.0	0.36	0.0	16.43	39.91	4.99	5.75	0.281	0.462	1.989	2.403
注：A.C_16—20/C_21—50-DBE₁₂-N₁，N₁类DBE=12的高低分子量同系物相对丰度参数；B.C_20—24/C_25—50-DBE₁₅-N₁，N₁类DBE=15的高低分子量同系物相对丰度参数；C.DBE₁₂/DBE₉-N₁，N₁类缩合度参数；D.DBE_8—9/DBE₄-O₁，O₁类缩合度参数.

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