石油与天然气地质 ›› 2023, Vol. 44 ›› Issue (1): 186-194.doi: 10.11743/ogg20230115

• 油气地质 • 上一篇    

MoS2在低熟有机质热演化生烃中的催化作用

李亢1,2,3,4(), 卢鸿1,2(), 马宏良5, 赵忠峰1,2,3, 黄华梅4, 彭平安1,2   

  1. 1.中国科学院 广州地球化学研究所 有机地球化学国家重点实验室,广东 广州 510640
    2.中国科学院 深地科学卓越创新中心,广东 广州 510640
    3.中国科学院大学,北京 100049
    4.南海规划与环境研究院,广东 广州 510300
    5.广东泽域实验设备 有限公司,广东 广州 510440
  • 收稿日期:2022-05-27 修回日期:2022-11-10 出版日期:2023-02-01 发布日期:2023-01-13
  • 通讯作者: 卢鸿 E-mail:likang1116@163.com;luhong@gig.ac.cn
  • 第一作者简介:李亢(1994—),男,博士研究生,油气地球化学。E?mail: likang1116@163.com
  • 基金项目:
    中国科学院A类战略性先导科技专项(XDA14010102);国家重点研发计划重点专项(2017YFC0603102);国家重点研发项目(2019YFC0605502);国家自然科学基金项目(41973069)

Catalytic role of MoS2 in hydrocarbon generation during thermal evolution of low-maturity kerogen

Kang LI1,2,3,4(), Hong LU1,2(), Hongliang MA5, Zhongfeng ZHAO1,2,3, Huamei HUANG4, Ping’an PENG1,2   

  1. 1.State Key Laboratory of Organic geochemistry, Guangzhou Institute of Geochemistry, CAS, Guangzhou, Guangdong 510640, China
    2.CAS Center for Excellence in Deep Earth Science, Guangzhou, Guangdong 510640, China
    3.University of Chinese Academy of Sciences, Beijing 100049, China
    4.South China Sea Institute of Planning and Environment Research, Guangzhou, Guangdong 510300, China
    5.Guangdong Zeyu Experimental Equipment Co. , Guangzhou, Guangdong 510440, China
  • Received:2022-05-27 Revised:2022-11-10 Online:2023-02-01 Published:2023-01-13
  • Contact: Hong LU E-mail:likang1116@163.com;luhong@gig.ac.cn

摘要:

MoS2常用作有机质催化加氢热解的高效催化剂,通过活化流动相的高压H2来提高热解产物的产率。但是MoS2催化剂是否对有机质自身热演化生烃有影响却少有研究。为此,通过对低成熟Alum页岩干酪根及添加MoS2催化剂的干酪根进行热模拟生烃对比实验,探究了MoS2对干酪根热演化生烃的影响。实验结果表明MoS2的加入使低熟干酪根具有更高的成烃潜力:①使轻烃(C6-14)峰值产率增加且峰值温度前移24 ℃,但重烃(C14+)峰值产率显著降低,表明MoS2加速了重烃向轻烃的热裂解转化;②使湿气产率在峰值温度(456 ℃)前轻微增加,但峰值温度后明显降低,表明MoS2促进了湿气的生成及后期的裂解;③使甲烷(C1)产率明显增加,特别是在528 ℃后C1增加了近50 %,这可能是因为MoS2促进了高-过成熟阶段干酪根的加氢作用;④通过FeS2(黄铁矿)与MoS2催化效应的系统对比,认为两种催化效应的差异主要受催化剂的结构、稳定性及硫的活性控制。

关键词: MoS2催化剂, 加氢, 催化效应, 硫, 热模拟, 干酪根, 生烃潜力

Abstract:

MoS2 has been commonly used as an efficient catalyst for the kerogen hydropyrolysis to improve the yield with activated high-pressure and mobile phase of H2. However, there is little document on whether MoS2 has a certain effect on the thermal maturation of organic matter and hydrocarbon generation. In this study, the effects of MoS2 on the thermal evolution of organic matter and hydrocarbon generation are investigated by comparative thermal simulation experiments on kerogen of low maturity from the Alum Shale with and without MoS2 added. The results show that low-mature kerogen has greater potential for hydrocarbon generation in presence of MoS2. MoS2 acts to increase the peak yield of light hydrocarbons (C6-14), while decrease the peak yield of heavy hydrocarbons (C14+), and lowering the temperature of peak hydrocarbon generation by about 24 ℃ at the same time, indicating that MoS2 serves to accelerate the thermal cracking of heavy hydrocarbons to light hydrocarbons. The adding of MoS2 also can slightly increase the yield of wet gases (C2-5) before the peak hydrocarbon generation temperature (456 ℃) is reached, but significantly decrease it after the temperature surpasses its peak hydrocarbon generation value, indicating that MoS2 can promote the generation and later cracking of wet gases. In addition, the existence of MoS2 also remarkably raise the yield of methane (C1), especially at a temperature higher than 528 ℃ when the methane yield increases by nearly 50 %, a possible result of MoS2 promoting the hydrogenation of kerogen at the high-to-over-mature stage. The difference of catalytic effect between pyrite (FeS2) and MoS2 is systematically compared, which is mainly controlled by the structure, stability and sulfur activity of catalysts.

Key words: MoS2 catalyst, hydrogenation, catalytic effect, sulfur, thermal simulation, kerogen, hydrocarbon generation potentia

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