Carbon isotopic compositions and origin of Paleozoic crude oil in the platform region of Tarim Basin, NW China

PETROLEUM EXPLORATION AND DEVELOPMENT Volume 44, Issue 6, December 2017 Online English edition of the Chinese language journal Cite this article as: PETROL. EXPLOR. DEVELOP., 2017, 44(6): 1053–1060.

RESEARCH PAPER

Carbon isotopic compositions and origin of Paleozoic crude oil in the platform region of Tarim Basin, NW China ZHU Xinjian1, CHEN Jianfa1,*, WU Jianjun1, 2, WANG Yifan1, ZHANG Baoshou2, ZHANG Ke2, HE Liwen1 1. State Key Laboratory of Petroleum Resources and Prospecting, China University of Petroleum, Beijing 102249, China; 2. PetroChina Tarim Oilfield Company, Xinjiang Korla 841000, China

Abstract: Based on the carbon isotopic compositions of Cambrian-Ordovician source rocks Kerogen Samples and Paleozoic crude oil in the platform region of Tarim Basin, the origin and source of Paleozoic crude oil were investigated. There are at least two sets of source rocks with different carbon isotope compositions in the Cambrian, the Lower Cambrian source rock with lighter carbon isotope composition and Middle-Upper Cambrian source rock with heavier carbon isotope composition, while the Ordovician source rock is somewhere in between. The δ13C values of Paleozoic crude oil samples are wide in distribution range, from -35.2‰ to -28.1‰. The crude oil with lighter carbon isotopic compositions (δ13C<-34.0‰) was mainly derived from Lower Cambrian source rock, and the crude oil with heavier carbon isotopic composition (δ13C>-29.0‰) was mainly derived from the Middle-Upper Cambrian source rocks, and the crude oil with δ13C value in between may be derived from Cambrian source rocks. It is concluded through analysis that the Cambrian source rock could become the major source rock in the Tarim Basin and the platform region has huge potential oil and gas resources in the deep formations. Key words: Tarim Basin; Cambrian; Ordovician; marine hydrocarbon; oil source; carbon isotope composition

Introduction The origin of oil and gas in the platform region of the Tarim Basin, NW China has long been controversial, restricting the exploration of deep formations in the basin[14]. Previous biomarkers correlation between crude oil and source rocks shows that the biomarkers in the oil from Cambrian are characterized by six highs and one low (high contents of C28 sterane, gammacerane, triaromatic dinoslerane, 4-methyl-sterane, 24-norcholestane, tricyclic terpane and low content of diasterane), while biomarkers in the oil from the Ordovician have opposite characteristics, which have been the basis for identification of Cambrian or Ordovician oil sources[58]. Study on carbon isotope features of oil shows the oil produced by Cambrian source rock has heavier carbon isotopic composition than that produced by Ordovician source rock, so it is believed that the oil produced by Cambrian source rock in Tarim Basin should have more heavier carbon isotopes, while the oil from Ordovician should have more lighter carbon isotope[912]. In 2013, commercial oil and gas flow was obtained from the Cambrian dolomite below the thick gypsum in Well ZS1, Tazhong Uplift, which brought about new questions on the understanding of marine hydrocarbon source rocks in the

platform region[1320]. According to the geological background, the oil and gas in the Cambrian dolomite in Well ZS1 may originate from the Cambrian source rock[17]; but the geochemical characteristics of Cambrian oil and gas in this well differ widely from the previous knowledge on Cambrian oil, and are similar to those of Ordovician crude oil[9]. Analysis of geological conditions show the Cambrian oil in Well ZS1 cannot come from the Ordovician, which implies that the current understanding on the geochemical characteristics of the Cambrian oil isn’t comprehensive. The Paleozoic hydrocarbon reservoirs in the platform region are buried deep and higher in thermal evolution degree, so some biomarkers indicating the origin and sedimentary environment of parental material have changed due to the effect of thermal evolution. With the increase of maturity, the components with poor thermal stability in biomarkers in source rock and oil gradually reduce, hence the conventional biomarkers in different oil or source rocks may become similar. Besides, the concentration of biomarkers in crude oil with high thermal evolution degree would also significantly reduce, thus the characteristics of biomarkers will change considerably when oils of different thermal evolution degrees mix[21].

Received date: 23 Mar. 2017; Revised date: 21 Aug. 2017. * Corresponding author. E-mail: [email protected] Foundation item: Supported by the China National Science and Technology Major Project (2016ZX05007-003); the National Natural Science Foundation of China (41572108). Copyright © 2017, Research Institute of Petroleum Exploration and Development, PetroChina. Published by Elsevier BV. All rights reserved.

ZHU Xinjian et al. / Petroleum Exploration and Development, 2017, 44(6): 1053–1060

Due to the relatively high thermal evolution degree of Paleozoic reservoirs and multiple sets of hydrocarbon source rocks in the platform region, identifying oil source by biomarkers can be ambiguous. A large number of studies reveal that the carbon isotopic composition of crude oil is mainly controlled by the carbon isotopic composition of source rock[1112,2225]. The effect of thermal evolution on the carbon isotopic composition of crude oil is relatively small, and in the process of thermal evolution, the change of the carbon isotopic composition of crude oil does not exceed 2‰ generally[2223]. Therefore, the carbon isotopic composition of crude oil can be used as an effective means of identifying the origin of oil in deep strata in the platform region. The carbon isotopic compositions of the oil in Well ZS1 and Well ZS5 are relatively light, which is consistent with the carbon isotopic composition characteristic of the global Cambrian crude oil, with δ13C values of generally less than 34‰[2630]. The carbon isotopic composition shows that there is not just one type oil from Cambrian with heavier carbon isotopic composition in the platform region and it can't be concluded that the oil with lighter carbon isotopic composition is from Ordovician. In order to clarify the origin and source of the marine oil in the platform region, carbon isotopic composition features of Paleozoic oil in the platform region are examined, and the major source rock in the region is sorted out according to the carbon isotopic composition of kerogen of different Cambrian and Ordovician formations in this study, which can provide a scientific basis for the next step oil and gas exploration.

1.

Geological setting The Tarim Basin, located at the northwest edge of China is

Fig. 1.

a large superimposed sedimentary basin developed on preSinian continental crust base. The platform region of Tarim Basin mainly include Tabei Uplift, Tazhong Uplift, Bagchu Uplift, Tadong Uplift and Northern Depression, which are characteristic by the Paleozoic marine sedimentation (Fig. 1). The main exploration target in the platform region is the Paleozoic hydrocarbon system. The main potential source rocks include the Ordovician, the Tuershaketage Formation and Moheershan Formation in the Middle - Upper Cambrian and the Yuertusi Formation and Xidashan Formation in the Lower Cambrian[48,31]. The current knowledge indicates that the Ordovician source rock is mainly distributed in the slope of the Tazhong and Tabei area, the Middle - Upper Cambrian source rocks are mainly in the Tadong area, and Lower Cambrian source rocks mainly in the Keping-Bachu area in north section of the Bachu Uplift and Tadong area[8]. Carboniferous, Silurian and especially Ordovician and Cambrian are the main reservoirs of the hydrocarbon system in the Paleozoic in the platform region of the Tarim Basin, and reservoirs in different regions are different to some extent in era (Fig. 2).

2.

Samples and methods

One hundred and thirty-three crude oil samples were collected in the Cambrian, Ordovician, Silurian and Carboniferous strata from 10 oil and gas fields in the platform region of the Tarim Basin (Fig. 1). The source rock samples were mainly collected from Cambrian - Ordovician source rocks. The samples of Cambrian source rocks were taken from Well H4 in Bauchu Uplift, Well XH1 in Tabei Uplift, Well TD2 in Tadong Uplift and the outcrop section (Sugetbulak, Xiaoerbulake, Shiairike) in Keping – Aksu area, western Tarim Basin and Kuruktag outcrop section in eastern Tarim Basin. The samples of Ordovician source rocks were taken from Well

Distribution of structure units, outcrop profiles and sampling oil fields in Tarim Basin.

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Isotope Component - Isotopic Mass Spectrometry GB/T 18340.2-2010” in the State Key Laboratory of Petroleum Resources and Prospecting, China University of Petroleum, Beijing. The δ13C values were calibrated relative to the PeeDee Belemnite (PDB) with an error of less than 0.1‰.

3.

Results and discussion

3.1. Carbon isotopic compositions of crude oil and source rocks

Fig. 2. Composite stratigraphic columnar section of the Paleozoic in the platform region of Tarim Basin.

LN46 in Tabei Uplift and Dawangou outcrop section in Keping area (Fig. 1). The kerogens were extracted from the source rock samples according to the standard “Isolation Method For Kerogen From Sedimentary Rock GBT 19144-2010”, and analyzed the carbon isotopic composition of the kerogen. The stable carbon isotopic composition was analyzed according to the standard “Determination of Organic Carbon Table 1.

Analysis results of 133 oil samples show they have δ13C values from 35.2‰ to 28.1‰ (Table 1), and oil samples of different regions follow some regularities. The oil in Bashitopu field in Maigaiti Slope of Bachu Uplift in the west of the platform has lighter carbon isotopic composition (with δ13C values from 35.2‰ to 33.1‰)than that in Hetianhe field (with δ13C values from 29.7‰ to 28.1‰). The oil samples from Yingmai2 Oilfield have δ13C values from 33.8‰ to 32.5‰, and oil samples from Lunnan Oilfield, Hadexun Oilfield and Jiefangqu Oilfield located in Tabei Uplift 32.5‰ – 30.8‰. And the oil samples from Tazhong Uplift in the central region of the basin have δ13C values from 33.2‰ to 29.8‰, with wide variations. Furthermore, the carbon isotopic composition of oil in Tabei Uplift turns heavier gradually from west to east (Fig. 3), for example, the average δ13C value of the oil samples from Yingmai2 field in the western Tabei Uplift is 33.1‰, to the Jiefangqu field in the eastern Tabei Uplift, it is 31.6‰. In addition, in Tazhong Uplift, oil samples from the Silurian and Carboniferous have lighter carbon isotopic composition (33.2‰ to 32.1‰), oil samples from the Ordovician have heavier carbon isotopic composition (from 31.5‰ to 30.5‰) (Fig. 4). The carbon isotopic composition of crude oil is mainly controlled by its hydrocarbon parent, and is affected little by thermal maturity and migration. The statistical results of the carbon isotopic compositions of the kerogen in source rocks in different parts of the platform region reveal that the carbon isotopic composition of kerogen of Cambrian source rock has two peaks (Fig. 5), the carbon isotopic composition of the

Carbon isotopic composition of Paleozoic oil samples taken from the platform region of Tarim Basin.

Location or oil field Sampling formation Number of samples Range of carbon isotopic composition/‰ Average of carbon isotopic composition/‰ Bashituopu Hetianhe

C

5

35.2  33.1

34.2

C, O

5

29.7  28.1

29.0

Yingmai2

O

14

33.8  32.5

33.1

Halahatang

O

24

32.8  31.6

32.3

C, O

5

33.2  31.9

32.6

Tahe

C

4

32.3  32.1

32.2

Hadexun

C, O

8

32.5  31.1

32.1

Lunan

Donghetang

C, O

17

32.2  30.8

31.7

Jiefangqu

C

6

31.9  31.2

31.6

Tazhong

C, O, S

45

33.2  29.8

31.7

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Fig. 3. Plane distribution histogram of carbon isotopic composition of crude oil in Tabei area.

Fig. 4. Vertical distribution histogram of carbon isotopic composition of crude oil in Tazhong area (N—number of samples).

Fig. 5. Distribution characteristics of carbon isotopic composition of different hydrocarbon source rocks in the platform region of Tarim Basin.

kerogen in Lower Cambrian hydrocarbon source rocks is lighter (with δ13C values mainly from 36.0‰ to 34.0‰), while that of the kerogen in Middle-Upper Cambrian hydrocarbon source rocks is heavier (with δ13C values mainly from 30.0‰ to 27.0‰), and the carbon isotopic composition of kerogen of Ordovician source rocks is slightly lighter than that of Middle-Upper Cambrian source rocks (with δ13C values mainly from 31.0‰ to 28.0‰). The carbon isotopic composition of hydrocarbon source rocks is mainly controlled by the parent material and deposi-

tional environment. In Early Cambrian, the “Oceanic Anoxic Event” (OAE) happened at numerous locations all over the world, resulting in a reduction environment with high content of CO2 and low content of O2. The δ13C value of organic matter is more negative in a reduction environment. Besides, organic matter is depleted less in a reduction environment, and the 12C in organic matter is easy to preserve. Therefore, the organic matter produced in Early Cambrian is more negative in δ13C value. In the Early Cambrian, the platform region in Tarim Basin was in a strong reducing sedimentary environment, the Lower Cambrian Yuertusi Formation source rock is rich in aryl-isoprenoid compounds, indicating this set of source rock was formed in anaerobic and strongly reducing sedimentary environment[3233]. Studies show that under anaerobic condition, the organism antecedents like anaerobic bacteria have lighter carbon isotopic composition, and the Cambrian formation is rich in anaerobic bacteria with lighter carbon isotopes[3436], moreover, the enrichment of aryl-isoprenoid compounds in the formation also indicates flourish of sulfur bacteria in the Early Cambrian in the platform region[37]. Liu et al found through study that different organisms in the Cambrian hydrocarbon source rocks in the platform region had different carbon isotopic compositions[38], the hydrocarbon source rock originated from planktonic algae had higher carbon isotopic composition, and the source rock from benthic organisms had lighter carbon isotopic composition, so it is inferred that benthic organisms were flourishing in the early Cambrian. Thus the special anaerobic bacteria and strong reduction environment in Early Cambrian in the platform region of Tarim Basin are the main reasons causing the more negative carbon isotopic composition of the source rocks in the Lower Cambrian. In the Middle - Late Cambrian, the sedimentary environment turned more oxidized due to the rise of O2 content, causing plankton to multiply massively and heavier carbon isotopic composition of the Middle - Upper Cambrian and Ordovician source rocks than that of the Lower Cambrian[3940]. Clearly, the differences in δ13C value in different layers of hydrocarbon source rocks are closely related to the changes in organisms and sedimentary environment in early Paleozoic in the platform region of Tarim Basin. 3.2.

Oil classification and oil source analysis

Based on previous studies, the Paleozoic crude oil in the platform region can be divided into three types according to the characteristics of carbon isotopic composition of crude oil and source rock kerogen and geological background (Table 2). The typeⅠoil has δ13C value from 35.2‰ to 33.1‰ with an average of 34.3‰, and oils from Well Qun 5, Qungu1 in the Bashituopu field, and Well ZS5 (Wusonger Formation in Upper Cambrian) in the Tazhong area belong to this type. The carbon isotopic composition of this kind of oil is in good agreement with that of the Lower Cambrian source rock. In the Bashituopu field located north of the Bashituopu fault in

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Table 2.

Carbon isotopic composition and classification of Paleozoic crude oil in the platform region of Tarim Basin.

Oil type

Location or oil field

Formation Range of carbon isotopic composition/‰ Average of carbon isotopic composition/‰

Bashituopu, Well ZS1, Well ZS1

C, — C

35.2  33.1

34.3

II

Hetianhe, Well TD2

C, O, — C

29.7  28.5

28.9

III

Yingmai2, Halahatang, Tahe, Donghetang, Hadexun, Lunan, Jiefangqu, Tazhong

C, O, S

33.8  29.8

32.1

I

Fig. 6.

The section of oil reservoir of the Bashituopu field.

the northern section of Maigaiti Slope, the Bashituopu Fault inclining south cutting down to the Cambrian system links the Cambrian oil source and provides vertical migration channel for oil and gas[4142] (Fig. 6). Moreover, this area has Lower Cambrian Yuertusi Formation good source rock, but no Ordovician source rock, so it is concluded that the crude oil in the area should be derived from the Lower Cambrian source rock. In the Well ZS5, there is a thick gypsum layer below the Ordovician, so it is difficult for the oil and gas to migrate from the Ordovician source rock on top through the overlying thick gypsum layer down to the Cambrian reservoir, and the carbon isotopic composition of crude oil in Well ZS5 is consistent with that of the Lower Cambrian source rock, so it is speculated that the oil and gas in ZS5 are also originated from the Lower Cambrian source rock. The statistic results of the carbon isotopic composition of typical crude oils from Cambrian source rocks in the world show that the crude oil in Cambrian bottom is characterized by lighter carbon isotopic composition, with δ13C value of generally less than 34‰. For example, the crude oil from the Lower Cambrian in Oman Basin has an average δ13C of 34.5‰[29], and the oil from lower Cambrian in Eastern Siberian Basin has an average δ13C of 35.1‰[30]. As mentioned above, in Early Cambrian, the special sedimentary environment and organisms are the main factors leading to the abnormally negative carbon isotopic composition of related organic matters. This type of oil with lighter carbon isotopic composition in the platform region is similar to typical Cambrian bottom oils in other basins across the world. Therefore,

it is deemed that the oil in the platform region with abnormally negative carbon isotopic composition is originated from Lower Cambrian source rock depositing in strong reduction sedimentary environment. The type II oil has δ13C of 29.7‰ to 28.5‰ and 28.9‰ on average, represented by oils in Well TD2 and the Hetianhe area. The crude oil in Well TD2 is formed in the basin facies, but that in the Hetianhe area in the platform facies. This type of oil has carbon isotopic composition highly consistent with that of Middle - Upper Cambrian source rock. Previous researches reveal that this kind of oil has six highs and one low characteristics of biomarkers, and apparently heavier δ13C. Most researchers believed that this kind of oil is from Cambrian source rock in the platform region[912,4344]. As mentioned above, the Lower Cambrian source rock in the platform region has lighter δ13C, so the oil with heavier carbon isotope can’t be from the Lower Cambrian source rock, rather it has good consistency with the Middle - Upper Cambrian source rock with heavier carbon isotopes. Therefore, it can be concluded that this kind of oil is originated from Middle - Upper Cambrian source rock based on previous researches, geological background and characteristics of carbon isotopic composition. Then type III oil has δ13C from 33.8‰ to 29.8‰, with an average of 32.1‰. This kind of crude oil is widely distributed in the platform region in the Ordovician, and also in the Carboniferous and Silurian. Study on oil and gas accumulation and geochemical features show that this kind of oil is of mixed origin[1112]. As mentioned above, the kerogen of Ordovician source rock in the platform region mainly ranges from 31‰ to 29 ‰ in δ13C, and the oil generated by Ordovician source rock is likely to range from 32‰ to 30‰ in δ13C. The crude oil formed by mixing the crude oils from these two sets of Cambrian source rocks has δ13C from 33‰ to 30‰. In this case, it is difficult to tell the source rock of this type crude oil based on the carbon isotopic composition alone. In the platform region of Tarim Basin, it was marine sedimentary environment which is similar in the period from the Cambrian to Ordovician, and the thermal evolution of crude oil in Paleozoic is relatively high. Therefore, the oil originating from the Lower Cambrian has some similar biomarker characteristics with that from Ordovician source rock, making it difficult to distinguish the crude oil from Cambrian source rock[17]. It is necessary to combine the distribution of hydrocarbon source rock, geological background, other geochemical parameters and hydrocarbon accumulation characteristics

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to sort out the origin of this kind of oil. 3.3.

Geological significance

The carbon isotopic composition of crude oil has apparent inheritance features, and is mainly controlled by the carbon isotopic composition of hydrocarbon source rock, while the influences of thermal evolution and migration are minor. There are three types of crude oils with different characteristics of carbon isotopic compositions in the platform region, indicating the complexity of organism and depositional environment in the early Paleozoic there. Comparison of the carbon isotopic compositions between Paleozoic crude oil and Lower Paleozoic source rocks in the platform region shows that oils in Bashituopu area and Well ZS5 have carbon isotopic compositions consistent with that of the Lower Cambrian source rock, while oil in Well TD2 has carbon isotopic composition comparable with that of the Middle - Upper Cambrian source rock. In the platform region of Tarim Basin, there is another kind of crude oil from Cambrian with low δ13C besides the kind of crude oil from Cambrian with high δ13C. Therefore, regarding the crude oil with high δ13C value as the typical representative of crude oil from the Cambrian source rock is one-sided, which is not a comprehensive understanding due to limited data available in the past. Therefore, it shouldn’t be considered unilaterally that the Cambrian source rock can only generate oil with high δ13C in Tarim Basin. The study results available show that the Cambrian source rocks are widely distributed, thick and higher in total organic matter abundance, meeting the requirements of major source rock. In contrast, the Ordovician source rock is limited in distribution, thin and lower in organic matter abundance[8,4547],. As mentioned above, the Lower Cambrian hydrocarbon source rock has lower carbon isotopic composition of kerogen (with δ13C values mainly from 36.0‰ to 34.0‰), while the Middle-Upper Cambrian hydrocarbon source rock has higher carbon isotopic composition of kerogen (with δ13C values mainly from 30.0‰ to 27.0‰). And the mixture of the two kinds of oil generated by the two types of Cambrian source rocks may have the δ13C values from 33‰ to 30‰. Therefore, the possibility that the type Ⅲ oil is derived from Cambrian source rock can't be ruled out, also the contribution of the Ordovician source rock cannot be denied. Hence, Cambrian source rock has the geological and geochemical conditions to become the major hydrocarbon source rock in the platform region of Tarim Basin. With sufficient oil source, the deep Cambrian has great potential of oil exploration, which broadens the oil and gas exploration range in Cambrian and even Paleozoic strata in Tarim Basin.

4.

Conclusions

Analysis of carbon isotopic composition shows there are at least two sets of source rocks with different carbon isotopic compositions in the Cambrian in the platform region, the

Lower Cambrian source rock with lighter carbon isotopic composition and Middle - Upper Cambrian source rock with heavier carbon isotopic composition. The difference is mainly caused by the parent material and sedimentary environment. The features of carbon isotopic compositions of oil samples show the oil generated by Cambrian source rock in the platform region includes two types, the type with lighter carbon isotopic composition (δ13C of less than 34‰) derived from Lower Cambrian source rock, and the type with heavier carbon isotopic composition (δ13C values of more than 29‰) derived from the Middle - Upper Cambrian source rock. The crude oil with high δ13C is not the only type of crude oil produced by Cambrian source rock in the platform region. According to the geological and geochemical characteristics of the source rocks, Cambrian source rock can be the major hydrocarbon source rock and has great potential of petroleum exploration in deep formations in the platform region of Tarim Basin.

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