Study on the Differences in Distribution and Composition Characteristics of Tricyclic Terpanes Under Intensive Biodegradation: A case study from oilsands in the northwestern margin of Junggar Basin

WANG Shan; ZHANG Min

doi:10.14027/j.issn.1000-0550.2022.012

Volume 41 Issue 4

Aug. 2023

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WANG Shan, ZHANG Min. Study on the Differences in Distribution and Composition Characteristics of Tricyclic Terpanes Under Intensive Biodegradation: A case study from oilsands in the northwestern margin of Junggar Basin[J]. Acta Sedimentologica Sinica, 2023, 41(4): 1192-1201. doi: 10.14027/j.issn.1000-0550.2022.012

Citation:

WANG Shan, ZHANG Min. Study on the Differences in Distribution and Composition Characteristics of Tricyclic Terpanes Under Intensive Biodegradation: A case study from oilsands in the northwestern margin of Junggar Basin[J]. Acta Sedimentologica Sinica, 2023, 41(4): 1192-1201. doi: 10.14027/j.issn.1000-0550.2022.012

Study on the Differences in Distribution and Composition Characteristics of Tricyclic Terpanes Under Intensive Biodegradation: A case study from oilsands in the northwestern margin of Junggar Basin

doi: 10.14027/j.issn.1000-0550.2022.012

WANG Shan^{1, 2
,},
ZHANG Min^{1, 2
,
,}

1.
Hubei Key Laboratory of Petroleum Geochemistry and Environment, Wuhan 430100, China
2.
College of Resources and Environment, Yangtze University, Wuhan 430100, China

Funds:

National Natural Science Foundation of China 42072165

CNPC Special Research 2019E2601

Received Date: 2021-05-24
Accepted Date: 2022-02-28
Rev Recd Date: 2022-01-20

Available Online: 2022-02-28

Publish Date: 2023-08-10

Abstract

The Junggar Basin is rich in oil sand resources. The northwestern margin of the Fengcheng oil sand mining area is the most important oil sand distribution area in the Junggar Basin. In this paper, the gas chromatography- mass spectrometry GC-MS of saturated and aromatic hydrocarbons in the oil sand sample extracts, such as normal alkanes, regular steranes, mono-aromatic steranes, short-chain triaromatic steranes, and rearranged steranes, were undetectable； in addition, the abundance of hopanes, pregnane, and long-chain triaromatic steranes were rare. Severe biodegradation has occurred, and the degradation level can reach level 8 or higher. As far as the overall carbon number distribution of tricyclic terpanes is concerned, with the increase of biodegradation, the anti-degradation ability of tricyclic terpanes will decrease with the increase of carbon number, i.e., tricyclic terpanes （TT） are resistant to biodegradation. The distribution appeared to be the following： high carbon number（C₂₈-C₃₁TT） > medium carbon number（C₂₃-C₂₆TT） > low carbon number （C₁₉-C₂₂ TT）. However, for a single tricyclic terpane compound, C19 and C20, C₂₂ and C₂₃, and C₂₆ and C₂₈ tricyclic terpanes tend to increase their resistance to degradation as the carbon number increases. Therefore, the use of the relative ratio of tricyclic terpane compounds, namely C₁₉-C₂₂ TT /C₂₈-C₃₁ TT、C₂₃-C₂₆ TT /C₂₈-C₃₁ TT、C₁₉-C₂₂ TT /C₂₃-C₂₆ TT、C₂₃ TT /C₃₁ TT, is proposed to describe the degree of severe biodegradation of crude oil and provide a geochemical basis for crude oil to undergo secondary alteration, especially biodegradation.
- Junggar Basin,
- biodegradation,
- tricyclic terpanes,
- oil sand

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0. 引言

全世界范围内,超过1/5的原油被细菌破坏或改造^[1]。1969年Winter et al.^[2]首次将自然条件下正构烷烃的消耗解释为原油生物降解作用后,生物降解的概念被定义并在全球广泛应用。国内外学者对生物降解作用进行了大量的研究发现,生物的降解作用是一个准阶梯式的过程,饱和烃中的类异戊二烯、姥鲛烷和植烷会在正构烷烃被消耗后发生降解,随后生物降解会破坏原油中的规则甾烷和烷基化芳香族化合物,然后依次是藿烷、芳香甾族烃类、重排甾烷、三环萜烷,且在高级阶段,似乎生成某些生物标志化合物,如25-降藿烷和断藿烷^[3⁃4]。而在生物降解过程中,各生物标志化合物系列又有一定的降解顺序,比如在严重生物降解原油中,甾烷系列被降解或被蚀耗的先后顺序为:ααα20R>αββ20R>αββ20S≥ααα20S,C₂₇>C₂₉>C₂₈规则甾烷>重排甾烷,C₂₇,C₂₈,C₂₉甾烷>C₂₀,C₂₁甾烷（式中>表示优先降解）；C₃₁和C₃₂升藿烷对生物降解的易感性比C₃₀藿烷强,而升藿烷系列中高碳数的藿烷同系物具有优先抵御生物降解的能力,尤其是C₃₅五升藿烷^[5⁃8]。一般认为的芳烃序列为烷基苯、萘、苯并噻吩、菲、二苯并噻吩,其抗生物降解的能力随着芳环数和烷基取代基数的增加而增加^[9⁃10]。

Anders et al.^[11]和Callegos^[12]1971年在Uinta绿河页岩中首次发现C₂₀-C₂₅三环萜烷以来,有关三环萜烷的研究也引起人们的关注。随后在1983年Moldowan et al.^[13]通过离子跃迁分析从石油样品中识别了C₁₉-C₄₅三环萜烷系列的化合物,后来学者又将此系列化合物的识别扩展到C₅₄^[14]。与此同时,国内学者开始将三环萜烷化合物应用到原油的生源输入及油源对比的研究^[15⁃16]。1979年,Seifert et al.^[17]通过在实验室模拟自然发生的生物降解过程,证实了三环萜烷可以在大多数严重降解的情况下存活,随后不断有学者证明三环萜烷是抗生物降解能力较强的化合物之一^[18⁃21],其中Lin et al.^[21]在1989年发现三环萜烷可能发生蚀变的等级与重排甾烷持平,生物降解等级大于8级。

近年来,国内外学者关于生物降解作用对原油的影响以及生物降解原油中生物标志化合物的特征研究越来越多。Bost et al.^[22]在喜氧细菌富集培养物实验中发现C₂₈三环萜烷会先于C₂₉三环萜烷降解；马遵敬^[23]研究哈山地区二叠系原油时发现低碳数三环萜烷分子抗生物降解能力可能更强；程熊等^[24]研究得出三环萜烷系列化合物（除C₂₀三环萜烷以外）抗生物降解能力随碳数的增加而增强；Huang et al.^[25]则得出一些严重生物降解样品中C₂₆三环萜烷是唯一存在的三环萜烷系列化合物。然而,针对三环萜烷系列化合物内组成与原油生物降解程度之关系的文献鲜有报道。基于前人研究,笔者以准噶尔盆地西北缘生物降解的油砂为例,重点探讨了遭受强烈生物降解作用原油中三环萜烷化合物分布与组成特征,提出了一些评价原油遭受生物降解程度比值,为遭受强烈生物降解作用原油的地区油气勘探提供地球化学依据。

1. 地质概况

准噶尔盆地油砂主要分布在盆地边缘,沿盆地或凹陷外缘富集和展布。迄今为止,西北缘是准噶尔盆地油气最多、油气藏规模最大的地区,盆地深层至浅层分布着常规原油—稠油—油砂。自东北向西南方向延伸约200 km,包括夏子街、风城、乌尔禾、百口泉、克拉玛依、红山嘴、小拐、车排子等油田,各油田之间的物性变化较大,有正常原油,也有大量的稠油以及少量的轻质油^[26⁃27]。风城油砂矿区是西北缘最大的油砂矿区,地层较为简单, 自下而上为石炭系（C）、上侏罗统齐古组（J₃q）或缺失,下白垩统吐谷鲁组（K₁t）、第四系（Q）四套地层。油砂主要赋存于下白垩统吐谷鲁组、上侏罗统齐古组。

准噶尔盆地属于山间型中间地块盆地,在地质历史演化过程中,它又是一个大型的复合叠加盆地。在盆地的地史演化过程中,西北缘构造活动主要表现为逆掩断裂,形成延伸250 km的推覆体构造带。推覆体构造带位于中央生油坳陷区的西北侧,与玛湖生油坳陷相邻,丰富的油源为油气藏提供了物质基础；长期的断裂活动、频繁的地层超覆、不整合为油气运移提供了良好的通道,断裂带的隐伏性,为油气聚集提供了较好的圈闭条件。因此,风城区齐古组、吐谷鲁组油藏形成于不整合面之上的超覆尖灭带属于稠油油藏。

研究表明,准噶尔盆地西北缘具有多期次成藏的特征,第一次成藏时间较早,主要是三叠纪末期的印支运动使西北缘逆掩断裂带剧烈活动,丰富的油气运移形成了二叠系—三叠系的早期油藏；第二次是侏罗纪—白垩纪时期的燕山运动,使西北缘造成齐古组的不整合,从而使印支期形成的油藏遭受破坏,沿不整合面发生第二次运移,形成齐古组油藏；燕山运动晚期活动强度减弱,西北缘在盆地中心沉降过程中,相对速度较慢,出现了吐古鲁组的超覆不整合及局部地段的微弱断裂活动,促使油气第三次运移,形成了吐古鲁组油藏和地面大面积油砂。据地化指标分析对比,不论浅层深层,稠油稀油,均具有较为一致的特性,油源来自玛湖凹陷,其推覆构造各部位油藏皆为同源原油^[28]。

2. 样品与实验

风城地区的油砂与稠油具有伴生的关系,本文主要分析了风城地区风砂51井、风砂52井、风砂53井、风砂54井、风砂55井、风砂56井和风砂58井等7口井共22个油砂样品,样品主要涉及下白垩统吐谷鲁组、上侏罗统齐古组,其埋深分别介于95.5~178.1 m、141.8~270.8 m。对所有样品分别进行了饱和烃和芳烃的色谱—质谱分析,首先用正己烷（100 mL）沉淀油砂抽提原油中的沥青质,然后用柱色层把脱沥青质原油分离成饱和烃（正己烷作冲洗剂）、芳香烃（甲苯作冲洗剂）。饱和烃和芳烃的色谱—质谱分析实验条件如下。

饱和烃GC-MS分析：仪器型号为HP-GC 6980/5873MSD。色谱柱为HP-5MS弹性石英毛细柱（30 m×0.125 mm×0.125 μm）,以脉冲不分流方式进样,脉冲压力为15 psi,进样温度300 ℃,He为载气,流速为1 mL/min。升温程序如下：初始温度50 ℃,恒温2 min后,以3 ℃/min的速率升温至310 ℃,并维持恒温18 min,EI电离方式,电离能量70 eV,采用内标法对饱和烃进行定量,正构烷烃的标样为C₂₄D₅₀,甾萜类标样为5α-雄甾烷。

芳烃GC-MS分析：仪器型号为HP-GC6890/5973 MSD,色谱柱为HP-5MS（60 m×0.25 mm×0.25 μm）,汽化室温度为290 ℃,进样方式是脉冲不分流进样且采用恒流模式,载气流速为1 mL/min。柱炉温的升温程序为：以20 ℃/min升至100 ℃,然后再以3 ℃/min升至310 ℃,恒温18 min。质谱采用EI电离方式,电离能量为70 eV,接口温度为280 ℃,采集方式为全扫描模式,扫描质量范围50~450 amu,采用内标法对芳烃进行定量,标样为D₁₀蒽。

4. 结论

（1）准噶尔盆地西北缘油砂样品中,正构烷烃、类异戊二烯烷烃、常规甾烷已经蚀变检测不到,藿烷类化合物、孕甾烷、升孕甾烷及长链三芳甾烷少量分布；三环萜烷绝对浓度异常丰富,有较完整的25-降藿烷系列化合物分布且绝对浓度含量较高,判断研究区原油曾遭受过强烈的生物降解作用,降解等级为8级以上。

（2） ETR参数揭示了研究区侏罗系样品的降解程度稍高于白垩系。通过各碳数比值与深度的关系研究,将三环萜烷化合物碳数划分为低碳数（C₁₉-C₂₂）、中碳数（C₂₃-C₂₆）和高碳数（C₂₈-C₃₁）。研究表明随着生物降解作用的增强,三环萜烷化合物的抗降解能力会随着碳数的增加而减弱,即三环萜烷抗生物降解能力为高碳数（C₂₈-C₃₁TT）<中碳数（C₂₃-C₂₆TT）<低碳数（C₁₉-C₂₂TT）。

（3）降藿烷系列化合物和伽马蜡烷指数与C₁₉-C₂₂TT/C₂₈-C₃₁TT、C₂₃-C₂₆TT/C₂₈-C₃₁TT、C₂₃TT/C₃₁TT做了相关的对比研究,发现随着生物降解程度的增加,C₁₉-C₂₂TT/C₂₈-C₃₁TT、C₂₃-C₂₆TT/C₂₈-C₃₁TT、C₂₃TT/C₃₁TT、C₁₉-C₂₂TT/C₂₃-C₂₆TT的比值均随之增大；且伽马蜡烷指数与这些指标均具有较好的相关性,而降藿烷系列化合物的绝对浓度与相对比值已不能用来判断受到强烈生物降解的样品,因此在选用降藿烷化合物相关参数来判断受到强烈生物降解作用地区的样品时,需要慎重选择。

Reference (41)

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井号	层位	孕甾烷	伽马蜡烷	C₂₉NH	三芳甾烷	Tm/Ts	C₂₀/C₁₉TT	TT/H	（C₂₀+C₂₁）/C₂₆TT	G/C₃₀H	C₂₉NH/C₃₀H
风砂53	K₁t	348.55	170.45	1 106.51	97.53	4.11	3.68	4.19	0.92	0.99	6.48
风砂52	K₁t	0	305.25	917.04	58.83	7.13	4.49	3.02	1.14	1.13	3.39
风砂52	K₁t	263.62	61.78	775.90	39.43	4.14	6.13	4.89	0.23	0.68	8.50
风砂54	K₁t	372.19	269.47	1 038.53	60.80	6.53	4.39	3.33	0.63	1.57	6.05
风砂51	K₁t	290.56	185.47	696.20	43.63	6.32	4.93	3.66	1.59	1.05	3.96
风砂55	K₁t	400.68	667.29	687.10	44.11	14.30	5.25	1.40	1.77	0.73	0.75
风砂54	K₁t	500.02	365.41	1 146.36	33.82	7.11	6.13	4.39	2.07	1.11	3.47
风砂55	K₁t	340.19	185.76	840.52	89.21	6.53	4.25	5.93	0.80	1.17	5.30
风砂51	K₁t	417.59	277.94	920.74	76.38	6.68	4.28	3.50	1.43	1.17	3.86
风砂53	K₁t	353.38	57.74	1 178.18	78.88	4.01	7.25	4.24	0.26	0.49	10.08
风砂55	J₃q	351.21	159.08	901.95	71.62	5.18	5.01	3.67	0.71	1.06	6.00
风砂56	J₃q	553.05	299.68	880.01	72.82	11.30	6.22	5.35	3.09	1.37	4.04
风砂53	J₃q	506.58	164.59	1 055.60	62.36	0	5.85	8.81	3.66	1.31	8.40
风砂52	J₃q	452.72	293.39	790.48	60.74	9.91	5.63	4.66	2.91	1.36	3.66
风砂55	J₃q	563.19	187.14	1 240.22	69.26	0	5.89	7.12	3.50	1.16	7.68
风砂56	J₃q	584.64	238.83	1 041.31	65.89	0	5.63	6.37	3.58	1.33	5.78
风砂54	J₃q	594.80	433.47	994.86	66.83	11.69	5.97	3.17	3.51	0.74	1.69
风砂58	J₃q	666.58	479.40	859.59	58.50	14.18	5.89	4.16	1.18	2.49	4.47
风砂51	J₃q	594.01	660.44	4 307.56	86.66	0	6.94	2.75	3.40	1.33	8.68
风砂54	J₃q	575.33	385.31	749.55	45.05	11.39	6.23	3.79	2.24	1.23	2.39
风砂51	J₃q	632.56	326.83	1 077.57	44.03	10.08	6.10	5.37	2.93	1.20	3.95
风砂53	J₃q	525.38	151.40	1 176.87	117.93	4.33	6.24	8.48	3.95	1.08	8.38

Study on the Differences in Distribution and Composition Characteristics of Tricyclic Terpanes Under Intensive Biodegradation: A case study from oilsands in the northwestern margin of Junggar Basin

doi: 10.14027/j.issn.1000-0550.2022.012

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