低熟页岩干酪根分子结构及生烃特征——以渤海湾盆地辽河坳陷曙光地区古近系沙河街组为例

doi:10.11743/ogg20250207

Abstract

Abstract:

Exploring the structure and hydrocarbon generation characteristics of kerogen at a molecular scale and revealing its reaction pathway for hydrocarbon generation and generation model holds great significance for the study on the hydrocarbon generation of kerogen in low-maturity shales and shale oil exploration. A combination of analytical techniques including ultimate analysis， solid-state ¹³C nuclear magnetic resonance （¹³C NMR） spectroscopy， X-ray photoelectron spectroscopy （XPS）， and Fourier transform infrared spectroscopy （FTIR）， is applied to investigate the heteroatom morphology， carbon skeleton structure， and aliphatic and aromatic functional groups of kerogen in low-maturity shales from the 4th member of the Paleocene Shahejie Formation in the Shuguang area， Western Sag， Liaohe Depression. Accordingly， a two-dimensional average molecular structure model of kerogen is established with C₁₈₈H₃₁₀O₁₄N₄S， which boasts a high proportion （73.40 %） of aliphatics， a low proportion of aromatics， and long aliphatic chains （methylene chain carbon number： 5.04）. The results of the reactive force field molecular dynamics （ReaxFF MD） simulation reveal that the mass fractions of gaseous hydrocarbons （C₁—C₄）， light oil components （C₅—C₁₃）， and heavy oil components （C₁₄—C₃₉） reach up to 41.32 % at 3 500 K， 20.75 % at 3 300 K， and 30.22 % at 2 800 K， respectively， with a conversion rate of kerogen pyrolysis up to 61.67 %. The hydrocarbon generation process of kerogen in the shales progresses through multiple stages， including structural transformation， weak bond breaking， strong bond breaking， secondary cracking， and polycondensation reaction sequentially. During these stages， kerogen molecules undergo the bond breaking of heteroatoms and carbon-hydrogen atoms in both aliphatics and aromatics， as well as dehydrogenation-induced polycondensation reactions of aromatic rings.

Key words: structural characteristics, average molecular structure model, hydrocarbon generation reaction pathway, hydrocarbon generation model, kerogen, low-maturity shale, Western Sag, Liaohe Depression, Bohai Bay Basin

CLC Number:

TE122.1

Guili MA, Junqing CHEN, Changtao YUE, Yue MA, Yuying WANG, Hong PANG, Fujie JIANG, Xungang HUO. Molecular structure and hydrocarbon generation characteristics of kerogen in low-maturity shales： A case of the Paleocene Shahejie Formation in Shuguang area， Liaohe Depression， Bohai Bay Basin[J]. Oil & Gas Geology, 2025, 46(2): 427-442.

Figures/Tables 17

Fig. 1

Fig. 2

Table 1

Fig. 3

Table 2

Fig.4

Table 3

Structural assignment and relative contents of carbon atoms with NMR chemical shifts in organic matter of shales from the Shuguang area， Western Sag， Liaohe Depression"

碳原子类型	化学位移/10^-6	归属	表达式	符号	相对含量/%
脂肪族碳	3 ~ 4	脂肪族终端甲基碳1	CH₃—CH₃	$f a l M$	6.40
	14 ~ 16	脂肪族终端甲基碳2	R—CH₃	$f a l M$	18.44
	16 ~ 22	芳香族甲基碳	Ar—CH₃	$f a r A$	27.79
	22 ~ 36	脂肪族亚甲基碳	CH₂—CH₃	$f a l H$	18.58
	36 ~ 50	次甲基碳和季碳	CH，C	$f a l D$	3.99
芳香族碳	100 ~ 110	质子化芳香族碳1	Ar—H	$f a r H$	3.65
	111 ~ 118	质子化芳香族碳2	Ar—H	$f a r H$	14.03
	123 ~ 129	质子化芳香族碳3	Ar—H	$f a r H$	4.74
	137 ~ 148	脂肪族取代基碳	Ar—C	$f a l C$	2.38

Table 3

Fig.5

Table 4

Table 5

Fig. 6

Table 6

Comparison of structural parameters between the average molecular structure model of kerogen and the tested shale samples from the Shuguang area， Western Sag， Liaohe Depression"

结构参数	符号	实验值	模型值
脂碳率/%	$f a r$	75.20	73.40
芳碳率/%	$f a l$	24.80	26.60
烷链支化度	$B I$	0	0
亚甲基链碳数	$C n$	4.94	5.04
桥碳与周碳比	$X B P$	0	0

Table 6

Fig. 7

Fig.8

Fig. 9

Fig. 10

Fig. 11

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分析项目	元素含量/%					原子量比值				干酪根类型
分析项目	N	C	H	S	O	H/C	O/C	N/C	S/C	干酪根类型
分析结果	1.939	78.223	10.915	1.023	7.900	1.660	0.080	0.020	0.005	Ⅰ型

元素XPS图谱峰	官能团	归属结构	结合能/eV	相对面积/%
C1s	脂肪族和芳香族碳	C=C，C—C，C—H	284.80	87.20
	与醚键、羟基相连的碳	C—O，C—OH	286.36	9.29
	羰基碳	O=C	287.96	2.35
	羧基碳	O=C—O	289.26	1.16
O1s	羰基氧	C=O	530.20	0.86
	碳-氧单键氧	C—O	532.36	95.98
	羧基氧	COOH	534.10	3.16
N1s	吡啶氮		399.89	94.56
N1s	吡咯氮		401.90	5.44
S2p	脂肪族硫	C=S	161.65	24.28
	噻吩硫		163.59	14.68
	亚砜硫	S=O	168.74	61.04

所属区域	波数范围/cm^-1	峰位波数/cm^-1	归属结构	峰面积	相对含量/%
芳香烃区域	900 ~ 700	700.61	3H	5.87	10.35
		724.87	3H	27.43	48.35
		760.65	3H	2.01	3.54
		826.85	2H	15.94	28.08
		877.44	1H	5.50	9.68
含氧官能团区域	1 800 ~ 1 000	1 047.50	烷基醚C—O	29.01	1.67
		1 130.39	醇羟基C—OH	55.37	3.18
		1 253.28	酚羟基Ar—OH	412.78	23.74
		1 311.77	芳香醚C—O	52.43	3.01
		1 374.85	芳香结构上的CH₃	182.96	10.52
		1 451.76	烷基上的CH，CH₂	263.83	15.17
		1 589.21	芳香结构C=C	610.73	35.15
		1 708.28	羧基COOH	131.46	7.56
脂肪烃区域	3 000 ~ 2 800	2 849.38	对称的—CH₂—	267.91	24.77
		2 871.39	对称的—CH₃—	79.33	7.33
		2 922.15	反对称的—CH₂—	631.79	58.41
		2 963.82	反对称的—CH₃—	102.66	9.49
羟基区域	3 600 ~ 3 100	3 338.26	醚—OH	312.46	70.07
羟基区域	3 600 ~ 3 100	3 464.70	氢键缔合的—OH（或—NH），酚类	133.48	29.93

名称	原子量比值
名称	H/C	O/C	N/C	S/C
实际样品（—）	1.662 8	0.075 8	0.021 3	0.004 9
构建模型（分子式C₁₈₈H₃₁₀O₁₄N₄S）	1.648 9	0.074 5	0.021 2	0.005 3
相对误差/%	-0.833 8	-1.757 1	-0.109 9	8.554 1

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Molecular structure and hydrocarbon generation characteristics of kerogen in low-maturity shales： A case of the Paleocene Shahejie Formation in Shuguang area， Liaohe Depression， Bohai Bay Basin

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