海陆相泥页岩气体生成的半封闭模拟实验

宋董军; 吴陈君; 陈科; 张明峰; 何薇; 苏龙; 张东伟; 付爽; 妥进才

doi:10.3799/dqkx.2019.197

海陆相泥页岩气体生成的半封闭模拟实验

doi: 10.3799/dqkx.2019.197

宋董军^1,2, ,,
吴陈君¹,
陈科³,
张明峰¹,
何薇^1,2,
苏龙¹,
张东伟^1,2,
付爽^1,2,
妥进才^1, ,

1.
甘肃省油气资源研究重点实验室, 中国科学院西北生态环境资源研究院, 甘肃兰州 730000
2.
中国科学院大学, 北京 100049
3.
中国地质调查局油气资源调查中心, 北京 100083

基金项目:

国家自然科学基金项目 41672127

国家自然科学基金项目 41602151

国家科技重大专项 2017ZX05036003-007

详细信息

作者简介:
宋董军(1993-), 男, 博士研究生, 从事油气地质及地球化学研究

通讯作者:
妥进才

中图分类号: P618
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- 被引次数: 0
出版历程
- 收稿日期: 2019-08-05
- 刊出日期: 2019-11-15

Gas Generation from Marine and Terrestrial Shales by Semi-Closed Pyrolysis Experiments

Song Dongjun^{1,2
,
,},
Wu Chenjun¹,
Chen Ke³,
Zhang Mingfeng¹,
He Wei^1,2,
Su Long¹,
Zhang Dongwei^1,2,
Fu Shuang^1,2,
Tuo Jincai^{1
, ,}

1.
Key Laboratory of Petroleum Resources, Gansu Province; Northwest Institute of Eco-Environment and Resources, Chinese Academy of Sciences, Lanzhou 730000, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
Oil & Gas Survey, China Geological Survey, Beijing 100083, China

摘要

摘要: 明确不同沉积环境下页岩气生成机理的差异性对于页岩气成因机理及页岩气地球化学特征研究具有重要意义.选择低演化阶段的海相（中元古界洪水庄组）和陆相（三叠统延长组长7段）泥页岩进行了半封闭热模拟实验，对其气体产物进行了组分和碳同位素分析.结果表明，洪水庄组页岩产气量要远远低于同温度条件下长7段泥岩的产气量.同时，长7段泥岩气体产物二次裂解程度比较高.洪水庄组页岩有机质母源以生油性为主，长7段泥岩沉积过程受到陆源混入，有机质母源以相对偏生气性为主.热模拟实验条件下黄铁矿转化成磁黄铁矿的过程也可能促进长7段泥岩烃类气的生成.热模拟实验中所用样品的状态，即柱状样或颗粒样，也可能会对气体的裂解行为产生影响.在这种情况下，南方地区页岩气高的甲烷产率以及碳同位素倒转可能与厚层页岩高的油气滞留率有关.
- 海相页岩 /
- 陆相泥岩 /
- 半封闭模拟实验 /
- 烃类气 /
- 排烃效率 /
- 差异性 /
- 油气地质
Abstract: Understanding differences of shale gas generation in different sedimentary environments has great significance to fully elucidate genesis mechanisms and geochemical characteristics of shale gas. In this study,semi-closed pyrolysis experiments were conducted on two lower-mature shales,including a marine shale from Hongshuizhuang Formation of Mesoproterozoic and a terrestrial mudstone from the Chang 7 Member of Yanchang Formation of Upper Triassic. The pyrolyzed gas productions were performed for gas constituent and carbon isotope analysis,aiming to investigate influences on gas generation from the nature of organic matter,mineralogical characteristics and rock fabric. The results show the discrepancy of sources of organic matter exists in the two shales,causing the amount of gas generated from Hongshuizhuang shale was lower than that of the Chang 7 Member under the same pyrolysis temperature. Meanwhile,the secondary cracking content of gas productions in the Chang 7 Member mudstone was relatively high. Organic matter in Hongshuizhuang Formation is oil-prone,but organic matter in the Chang 7 Member mudstone is relatively gas-prone due to mixture of continental materials. Moreover,the transformation process from pyrite to pyrrhotine also can be conducive to advancing the generation of hydrocarbon gas in the Chang 7 Member mudstone. The rock fabrics used in the pyrolysis experiments would lead to different cracking behaviors of gas. In this scenario,the characteristics of high methane composition and rollover of carbon isotope of shale gas in the South China may be associated with higher retention of oil and gas in those thick shales.
- marine shale /
- continental mudstone /
- semi-closed pyrolysis experiment /
- hydrocarbon gas /
- expulsion efficiency /
- difference /
- petroleum geology

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图 1 海相页岩(KC)热模拟气体产率

Fig. 1. Gas yields of the marine shale (KC) in the pyrolysis experiments

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图 2 陆相泥岩(F14)热模拟气体产率

Fig. 2. Gas yields of the terrestrial mudstone (F14) in the pyrolysis experiments

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图 3 海陆相泥页岩热模拟气体干燥系数变化

a.海相页岩(KC)；b.陆相泥岩(F14)

Fig. 3. Changes of gas dryness coefficients of the marine and terrestrial shales in the pyrolysis experiments

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图 4 热模拟气体碳同位素变化

Fig. 4. Variations of carbon isotope of gas productions in the pyrolysis experiments

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图 5 热模拟烃类气的ln(C₁/C₂) vs. ln(C₂/C₃)图(a)、δ¹³C₂-δ¹³C₃ vs. ln(C₂/C₃)图(b)、δ¹³C₂-δ¹³C₃ vs.(C₂/C₃)图(c)、δ¹³C₂-δ¹³C₃ vs. δ¹³C₁图(d)

Fig. 5. Plots of ln(C₁/C₂) vs. ln(C₂/C₃) (a), δ¹³C₂-δ¹³C₃ vs. ln(C₂/C₃) (b), δ¹³C₂-δ¹³C₃ vs. (C₂/C₃) (c) and δ¹³C₂-δ¹³C₃ vs. δ¹³C₁ (d) for the pyrolytic gases

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图 6 场发射扫描电镜下F14泥岩样品部分热模拟固体残渣的矿物溶蚀现象

Fig. 6. Mineral dissolution of parts of F14 solid residues after pyrolysis experiments under FE-SEM

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表 1 原始样品的有机地球化学信息

Table 1. Organic geochemical characteristics of original samples

样品名	岩性	TOC (%)	R_o* (%)	S₁ (mg HC/g)	S₂ (mg HC/g)	S₃ (mg CO₂/g)	T_max (℃)	HI (mg HC/g TOC)	OI (mg CO₂/g TOC)
F14	泥岩	4.49	0.77	1.41	11.58	0.12	442	216.04	2.24
KC	页岩	5.18	0.76*	0.5	15.62	0.93	440	268.00	16.00
注：R_o依据公式“R_o=0.018×T_max-7.16”计算得到(Jarvie et al., 2007).“*” R_o估计依据见补充材料.

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表 2 原始样品的矿物组成信息

Table 2. Mineralogical characteristics of original samples

样品名	石英(%)	钠长石(%)	钾长石(%)	黄铁矿(%)	粘土矿物(%)
样品名	石英(%)	钠长石(%)	钾长石(%)	黄铁矿(%)	伊蒙混层	高岭石
F14	40	15	11	4	21	9
KC	70	nd	14	nd	16	nd
注：“nd”代表未检测到.

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表 3 模拟气的气体组分特征

Table 3. Gas compositions of pyrolysis experiments

温度(℃)	估计R_o^* (%)	样品	非烃类气			烃类气					干燥系数(%)	总气	烃类气	非烃气
			N₂	CO₂	H₂S	C₁	C₂	C₃	C₄₊	C₂₊		mL/g TOC
			mL/g TOC									mL/g TOC
250		KC	29.41	13.99	0.00	0.24	0.03	0.02	0.04	0.11	71.86	44.00	0.35	43.75
300			49.04	27.41	0.00	0.71	0.19	0.12	0.10	0.44	62.83	78.16	1.15	77.01
350	0.9~1.2		200.10	15.41	0.00	2.84	1.08	0.66	0.54	2.29	55.49	222.89	5.13	217.77
400			245.29	5.46	0.00	8.08	2.58	1.50	1.25	5.36	60.28	266.98	13.44	253.34
450	1.5~2.0		336.33	9.67	0.00	27.32	5.94	2.53	0.98	17.32	74.31	386.77	44.64	361.52
500			197.86	37.71	0.00	157.87	17.18	3.02	1.97	22.90	87.68	418.59	180.77	237.82
550	2.5~3.0		113.81	109.20	0.00	330.70	23.94	4.03	2.96	34.09	91.45	589.19	364.79	224.40
250		F14	90.17	20.82	0.00	0.46	1.38	6.68	6.67	14.73	3.06	127.22	15.20	112.02
300			127.95	52.42	0.00	0.85	0.63	3.54	5.77	9.94	7.86	192.57	10.79	181.78
350	0.9~1.2		155.33	71.16	0.00	8.42	3.53	4.11	5.25	12.90	39.50	249.44	21.33	228.11
400			78.25	103.57	0.02	76.77	29.04	21.41	20.47	70.91	51.98	330.21	148.14	182.07
450	1.5~2.0		74.84	109.92	0.46	164.16	54.05	31.43	16.50	101.98	61.68	453.46	267.60	185.86
500			123.69	118.15	0.02	246.64	39.53	10.66	6.50	56.69	81.31	548.09	304.83	243.26
550	2.5~3.0		66.37	250.27	0.06	509.66	37.85	6.70	3.51	48.06	91.38	880.38	562.66	317.72
注：“*” R_o估计依据见补充材料.

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表 4 模拟气的碳同位素

Table 4. Carbon isotope of pyrolysis gas productions

温度(℃)	KC (‰ PDB)				F14 (‰ PDB)
温度(℃)	δ¹³C₁	δ¹³C₂	δ¹³C₃	δ¹³C_CO2	δ¹³C₁	δ¹³C₂	δ¹³C₃	δ¹³C_CO2
250	-41.9	-34.5	-32.6	-27.4	nd	-36.3	-36.1	-4.0
300	-44.7	-40.2	-40.0	-32.2	nd	-39.0	-37.7	-4.3
350	-51.0	-42.2	-40.7	-31.0	-48.5	-39.2	-38.2	-5.1
400	-47.8	-38.4	-37.3	-28.3	-47.4	-38.0	-36.6	-8.4
450	-50.6	-37.3	-34.9	-35.0	-44.7	-37.4	-33.4	-13.8
500	-37.4	-34.5	-34.4	-33.3	-39.8	-32.5	-32.0	-16.2
550	-36.9	-28.5	-31.9	-33.3	-36.0	-28.7	-31.0	-22.3
注：“nd”代表未检测到.

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表 5 模拟实验条件下2类泥页岩残留油产率

Table 5. Residual oil yields of the studied shales under pyrolysis experiments

温度(℃)	KC残留油产率(mg/g TOC)	F14残留油产率(mg/g TOC)
250	18.03	66.62
300	15.60	156.31
350	34.44	189.23
400	3.88	15.89
450	1.33	2.77
500	0.62	2.28
550	0.64	2.73

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