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Natural Gas Geoscience ›› 2020, Vol. 31 ›› Issue (7): 931-938.doi: 10.11764/j.issn.1672-1926.2020.05.006

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The influence of pressure on hydrocarbon gas generation and carbon isotope of methane from type III kerogen

Chun-min HE1,2(),Jun GAN3,Gang LIANG3,Xing LI3,Xing WANG1,2,Hui TIAN1()   

  1. 1.State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
    2.University of Chinese Academy of Sciences, Beijing 100049, China
    3.Zhanjiang Branch, CNOOC China Ltd. , Zhanjiang 524057, China
  • Received:2020-01-30 Revised:2020-04-30 Online:2020-07-10 Published:2020-07-02
  • Contact: Hui TIAN E-mail:hechmin@mail2.sysu.edu.cn;tianhui@gig.ac.cn
  • Supported by:
    China National Science and Technology Major Project(2016ZX05026-002-005);Guangdong Natural Science Foundation(2016A030310119)

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Abstract:

Samples from transitional source rocks of Qiongdongnan Basin were pyrolyzed under 50 MPa, 100 MPa and 150 MPa, in order to tentatively discuss the effects of pressure on hydrocarbon gas generation and carbon isotope fractionation of methane. The results presented that increasing pressure would retard the hydrocarbon gas yield when pyrolytic temperature was low (EqVRO% less than 2.69%), and when it came to wet gases, the retardation was more significant than methane. However, there would be little influence of pressure at high pyrolytic temperature (EqVRO% more than 2.77%), or even slightly promoting methane generation. Calculated kinetic parameters showed that activation energy and frequency factor increased with growing pressure, as a result of that growing pressure makes the gas in the closed gold tube expand to do more work as well as the reactant concentration enrichment. At the rate of 5 ℃/Ma, pressure increases from 50 MPa to 150 MPa, which will result in the temperature increase of about 10 ℃ for every 50 MPa in the gas window. When temperature is higher than 260 ℃, the effect of pressure is no longer obvious. The experiment results also presented that growing pressure makes methane rich in 12C1. And it could result in 3.2‰ negative shift of carbon isotope values from 50 MPa up to 150 MPa. Meanwhile, the relationships between carbon isotope values and methane conversion were not the same under different pressures, indicating that negative shift of methane carbon isotope value was not only related to the retardation of methane generation, but also related to the slight changes happened to methane generation mechanism, which resulted in the changes in the distribution of the difference of activation energy between 13C1 and 12C1.

Key words: Qiongdongnan Basin, Hydrocarbon gases, Carbon isotope value of methane, Kinetics, Overpressure

CLC Number: 

  • TE122.1+13

Table 1

Geochemical parameters of mudstone and corresponding kerogen samples from Yacheng Formation of Well YC13-1-2"

样品类型深度/m层位沉积相

TOC

/%

S2/（mg/g）

IH

/(mg/gTOC)

Tmax

/oC

RO/%δ13Corg/‰

干酪根

类型

泥岩3 989~4 014崖城组海陆过渡相11.213.3118.74611.05-27.3III
干酪根3 989~4 014崖城组海陆过渡相64.481.8127.0462--27.5III

Fig.1

Hydrocarbon gas yields of transitional kerogen from Yacheng Formation of Well YC13-1-2 under different pressure"

Fig.2

The evolution of carbon isotope values of methane generated from transitional kerogen from Yacheng Formation of Well YC13-1-2 under different pressures"

Fig.3

The frequency factors and distribution of activation energy for C1-5 generation from the transitional kerogen of Yacheng Formation of Well YC13-1-2 under different pressures"

Table 2

Various kinetic paramters of methane carbon isotope fraction for kerogen from Yacheng Formation of Well YC13-1-2 under different pressures"

压力/MPa13A/12AβL/(cal/mol)βH/(cal/mol)μ/(kcal/mol)Σ/%δ13Cinit/‰
501.02256448.6864.0-27.5
1001.02157050.6867.0-27.5
1501.02246553.5016.46-27.5

Fig.4

Influence of pressure on hydrocarbon gases yield from transitional kerogen of Yacheng Formation of Well YC13-1-2 under geological condition (5 oC/Ma)"

Fig.5

Influence of pressure on the evolution of methane yield and carbon isotope value of methane generated from transitional kerogen of Yacheng Formation of Well YC13-1-2 under geological condition (5 oC/Ma)"

Fig.6

The relationships between methane carbon isotope values and conversion under different pressures"

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