中国陆相烃源岩氮同位素组成与有机质聚集

曹剑; 夏刘文; 胡文瑄; STÜEKENEva E; 支东明; 唐勇; 向宝力; 何文军

doi:10.11781/sysydz202305912

中国陆相烃源岩氮同位素组成与有机质聚集

doi: 10.11781/sysydz202305912

1.
南京大学地球科学与工程学院, 南京 210023
2.
School of Earth and Environmental Sciences, University of St Andrews, St Andrews, Scotland, KY16 9AL, UK
3.
中国石油吐哈油田分公司, 新疆哈密 839009
4.
中国石油新疆油田分公司, 新疆克拉玛依 834000

基金项目:

国家自然科学基金 42230808

国家自然科学基金 42203055

中国石油科技重大专项 2021DJ0108

详细信息

作者简介:
曹剑(1978—), 男, 博士, 教授, 本刊编委, 从事石油地质学和有机地球化学研究。E-mail: jcao@nju.edu.cn

中图分类号: TE122.1
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出版历程
- 收稿日期: 2023-07-26
- 修回日期: 2023-08-06
- 刊出日期: 2023-09-28

Nitrogen isotope compositions and organic matter accumulation in terrestrial hydrocarbon source rocks in China

1.
School of Earth Science and Engineering, Nanjing University, Nanjing, Jiangsu 210023, China
2.
School of Earth and Environmental Sciences, University of St Andrews, St Andrews, Scotland, KY16 9A, UK
3.
PetroChina Tuha Oilfield Company, Hami, Xingjiang 839009, China
4.
PetroChina Xinjiang Oilfield Company, Karamay, Xinjiang 834000, China

摘要

摘要: 氮作为重要的生命元素与有机质聚集之间具有成因联系，但尚未形成系统性、规律性认识。以中国广泛发育的二叠系—古近系陆(湖)相烃源岩为例，对此进行了探讨。结果表明，根据氮同位素(δ¹⁵N)组成，结合盐度和蒸发性碱类矿物特征，可将中国陆相烃源岩分为3组：近中性组1(δ¹⁵N平均值为4.0‰±1.5‰)、近中性组2(δ¹⁵N平均值为7.1‰±1.6‰)和碱性组(δ¹⁵N平均值为18.4‰±3.3‰)。在δ¹⁵N < 10‰的近中性组中，烃源岩的δ¹⁵N与有机质丰度、类型、生烃能力和页岩油潜力呈正相关，原因在于较高的δ¹⁵N值指征了生烃母质组成的变化。在δ¹⁵N>10‰的碱性组中，有机质类型都较好，页岩油潜力都较高，但烃源岩的δ¹⁵N与有机质聚集的响应关系不如中性组，反映有机质聚集受非δ¹⁵N其他综合因素的影响与控制。据此建立了基于δ¹⁵N划分出的3类湖相烃源岩的有机质聚集模式(< 5‰、5‰~10‰、>10‰)。δ¹⁵N具有示踪有机质聚集和烃源岩质量的潜力，以湖相烃源岩为例，低δ¹⁵N型(δ¹⁵N < 5‰)质量差，中—高δ¹⁵N型(δ¹⁵N>5‰)质量好。从氮同位素组成和氮循环这一新角度探讨了烃源岩有机质聚集，丰富了氮的生物地球化学与烃源岩地球化学研究。
- 有机质聚集 /
- 氮同位素 /
- 初级生产力 /
- 有机质保存条件 /
- 陆相烃源岩
Abstract: As an important biological element, nitrogen is causally linked with organic matter accumulation, but a systematic and regular understanding has not been developed. This paper discusses this issue by taking the widely developed Permian-Paleogene terrestrial (lacustrine) hydrocarbon source rocks in China as an example. The results show that the terrestrial source rocks in China can be classified into three groups according to the nitrogen isotope (δ¹⁵N) compositions and combined with the salinity and evaporative alkali mineral characteristics: the circum-neutral group 1 (average δ¹⁵N=4.0‰±1.5‰), the circum-neutral group 2 (average δ¹⁵N=7.1‰±1.6‰), and the alkaline group (average δ¹⁵N=18.4‰±3.3‰). In the circum-neutral group with δ¹⁵N < 10‰, the δ¹⁵N of the source rocks is positively correlated with organic matter abundance, type, hydrocarbon generating capacity and shale oil potential due to the fact that higher δ¹⁵N characterizes changes in the composition of the hydrocarbon generating bio-precursors. In the alkaline group with δ¹⁵N>10‰, the organic matter types are good and shale oil potentials are higher, but the response relationship between δ¹⁵N of source rocks and organic matter accumulation is not as good as that of the circum-neutral group, reflecting that the organic matter accumulation in alkaline group is influenced by other comprehensive factors other than δ¹⁵N. Accordingly, the organic matter accumulation models of three types of lacustrine source rocks (< 5‰, 5‰-10‰, and >10‰) classified on the basis of δ¹⁵N were established. The δ¹⁵N has the potential to trace organic matter accumulation and quality of source rocks. For example, low δ¹⁵N type (δ¹⁵N < 5‰) is of poor quality and medium-high δ¹⁵N type (δ¹⁵N>5‰) is of good qualityin lacustrine source rocks. This paper enriches the biogeochemical and hydrocarbon source rock geochemical studies of nitrogen by exploring organic matter accumulation in source rocks from the new perspective of nitrogen isotope composition and nitrogen cycling.
- organic matter accumulation /
- nitrogen isotopes /
- primary productivity /
- preservation conditions of organic matter /
- continental hydrocarbon source rocks
注释:

1) 所有作者声明不存在利益冲突。

1) 利益冲突声明/Conflict of Interests

2) 作者贡献/Authors’Contributions

2) 曹剑、夏刘文、Eva E Stüeken参与实验设计并完成实验操作；曹剑、夏刘文、胡文瑄、支东明、唐勇、向宝力、何文军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。

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图 1 中国陆相湖盆烃源岩δ¹⁵N和有机质聚集特征的相关性

δ¹⁵N数据来自文献[26]，鄂尔多斯盆地T₃y₇数据来自文献[17, 25]。

Figure 1. Correlation analysis of δ¹⁵N and organic matter accumulation of source rocks in terrestrial lacustrine basins in China

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图 2 δ¹⁵N对中国陆相湖盆烃源岩质量的影响

ω(TOC)、δ¹³C_org和δ¹⁵N数据来自文献[26]，鄂尔多斯盆地T₃y₇数据来自文献[17, 25]。

Figure 2. Response of δ¹⁵N to the quality of hydrocarbon source rocks in terrestrial lacustrine basins in China

下载: 全尺寸图片幻灯片

图 3 δ¹⁵N、ω(P)/ω(Al)、Mo_EF、ω(TOC)、S₁+S₂、δ¹³C_org、I_H、PG/ω(TOC)和OSI随深度变化特征

a.南襄盆地泌阳凹陷核桃园组程2井；b.准噶尔盆地玛湖凹陷湖盆中心区风城组(F20、FN7和AK1井的样品深度根据地层数据转换为FN5井的等效深度)。图a和图b中的岩性柱状图分别来自文献[23, 26]，ω(TOC)、δ¹³C_org和δ¹⁵N数据来自文献[26]。PG/ω(TOC)、OSI的单位为mg/g。

Figure 3. Characterization of δ¹⁵N, ω(P)/ω(Al), Mo_EF, ω(TOC), S₁+S₂, δ¹³C_org, I_H, PG/ω(TOC) and OSI with depth

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图 4 中国典型湖相烃源岩的有机质聚集模式

a.近中性组1的准噶尔盆地其他组烃源岩(P₁j、P₂w和P₂p)，修改自文献[28]；b.近中性组2的南襄盆地始新统核桃园组烃源岩，修改自文献[20, 56]；c.碱性组的准噶尔盆地二叠系风城组烃源岩，修改自文献[26]。(S₁+S₂)、I_H、PG/ω(TOC)、OSI的单位为mg/g。

Figure 4. Models of organic matter accumulation in typical lacustrine hydrocarbon source rocks in China

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图 5 海相和湖相环境中的氮循环基本方式

a.海相和近中性组1和组2湖相环境中的氮循环；b.碱性组湖相环境中的氮循环，修改自文献[15]。ε=δ¹⁵N_产物－δ¹⁵N_反应物(图中单位为‰)。

Figure 5. Pathways of nitrogen cycling in marine and lacustrine environments

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表 1 研究样品清单

Table 1. Sample list for this study

项目	准噶尔盆地	四川盆地中部	鄂尔多斯盆地	松辽盆地	渤海湾盆地东濮凹陷	江汉盆地潜江凹陷	南襄盆地泌阳凹陷	柴达木盆地西部	准噶尔盆地玛湖凹陷	准噶尔盆地吉木萨尔凹陷
层位	P₁j、P₂w、P₂p	J₁z_d	T₃y₇	K₂qn	E_2-3s	E₂q	E₂h₃	E₂xg	P₁f	P₂l
样品数/个	27	9		9	9	10	9	10	66	5
δ¹⁵N/‰	1.2~8.8	3.0~5.7	2.5~5.0	3.9~10.8	5.4~8.4	4.7~8.9	6.0~9.8	3.9~8.0	10.1~24.4	10.6~16.8
氮循环	δ¹⁵N平均值为4.0‰±1.5‰，反硝化作用控制			δ¹⁵N平均值为7.1‰±1.6‰，反硝化作用控制					δ¹⁵N平均值为18.4‰±3.3‰，氨挥发作用控制
分组	近中性组1			近中性组2					碱性组
盐度	淡水—微咸水	淡水—微咸水	淡水—微咸水	微咸水—咸水	咸水—盐水	咸水—盐水	微咸水—盐水	微咸水—盐水	咸水—盐水	微咸水—盐水
氧化还原	氧化—贫氧			贫氧—缺氧					主体缺氧	贫氧—缺氧
ω(TOC)/%	0.4~2.5	1.2~3.6	3.6~10.1	0.7~3.1	0.3~2.4	1.1~4.4	1.8~4.4	0.4~1.6	0.2~3.1	1.4~7.8
δ¹³C_org/‰	-27.6~-20.3	-28.9~-26.5	-30.4~-28.3	-30.2~-25.9	-27.4~-23.4	-27.1~-23.7	-29.1~-25.9	-28.4~-23.1	-30.6~-24.0	-29.5~-25.2
ω(P)/ω(Al)/10^-3	0.7~26.7	3.8~18.2	9.1~57.8		8.3~8.3	12.2~26.8	8.0~29.4	5.8~17.1	0.7~15.0	7.4~14.9
ω(Ba)/ω(Al)/10^-3	1.9~12.2	6.6~9.4	5.4~11.4	10.5~35.1	3.3~22.1	4.0~18.2	6.7~14.3	4.7~60.0	0.8~73.7	5.3~9.4
Mo_EF	0.1~60.1	0.8~12.9	3.6~18.1	7.5~59.1	2.8~49.0	5.1~31.2	14.3~47.7	4.1~28.7	0.5~190.9	2.1~12.0
ω(SiO₂)/ω(Al₂O₃)	1.8~4.9	2.6~3.9	2.6~3.3		2.8~3.5	2.7~3.8	2.7~4.2	3.3~4.9	3.5~23.3	3.9~4.7
S₁+S₂	0.06~10.7	4.1~10.3		1.3~11.2	0.3~27.6	4.7~24.2	2.3~20.8	0.5~10.1	0.2~25.3	4.3~23.8
I_H	0.1~501.9	199.8~311.8		120.0~523.7	91.0~595.5	191.4~376.7	79.6~617.1	29.7~540.8	45.7~876.6	40.5~523.3
PG/ω(TOC)	3.3~543.3	248.9~410.8		182.7~970.5	94.6~648.5	418.9~790.3	126.6~655.4	49.8~635.7	49.8~983.5	54.3~796.1
OSI	0.5~473.2	25.1~121.5		62.8~446.8	3.2~116.7	121.1~561.8	29.0~211.7	20.1~188.2	13.8~272.8	4.1~723.6
注：δ¹⁵N、ω(TOC)、δ¹³C_org、盐度和氧化还原状态来自文献[26]；鄂尔多斯盆地T₃y₇数据来自文献[17, 25]；PG=(S₁+S₂)、I_H、PG/ω(TOC)和OSI=S₁/ω(TOC)的单位为mg/g。

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表 2 中国3类陆相湖盆烃源岩有机质聚集特征

Table 2. Characteristics of organic matter accumulation in three types of hydrocarbon source rocks in terrestrial lacustrine basins in China

烃源岩类型	δ¹⁵N/‰	层位	氧化还原状态	盐度	有机质聚集特征
低δ¹⁵N型，近中性组1	主体 < 5，均值4.0±1.5	准噶尔盆地其他组、T₃y₇、J₁z_d	氧化—贫氧	淡水—微咸水	初级生产力较低、有机质保存条件较差；生烃潜量低、有机质类型差、生烃能力较低、页岩油潜力低
中δ¹⁵N型，近中性组2	5~10，均值7.1±1.6	K₂qn、E_2-3s、E₂q、E₂h、E₂xg	氧化—缺氧	微咸水—盐水	初级生产力较高、有机质保存条件较好；生烃潜量高、有机质类型较好、生烃能力较高、页岩油潜力较高
高δ¹⁵N型，碱性组	>10，均值18.4±3.3	P₁f、P₂l	贫氧—缺氧	微咸水—盐水	初级生产力变化大、有机保存条件较好；有机质丰度变化大、有机质类型好、生烃能力变化大、页岩油潜力大

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