期刊
CHEMICAL ENGINEERING JOURNAL
卷 377, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2018.10.212
关键词
Bitumen- and carbonates-free kerogen; Non-isothermal pyrolysis; Kinetics; Non-linear least squares analysis; Two-stage reaction model
资金
- VISTA - Statoil
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
- Shanghai Rising-Star Program [17QA1401200]
- 111 Project of the Ministry of Education of China [B08021]
Fundamentally understanding the pyrolysis kinetics of kerogen is of prime scientific and industrial importance. Herein, bitumen- and carbonates-free kerogen sample is prepared through Soxhlet extraction followed by decarbonation of Green River oil shale, and its pyrolysis is studied by non-isothermal thermogravimetric analysis. The systematic analyses show that both the Popescu and master plots methods are not applicable to describe the kerogen pyrolysis process due to the changed reaction model and the varied activation energy over certain conversion range, respectively, while the piecewise non-linear least squares analysis is identified as an effective method to discriminate the most probable kinetic model from commonly used 15 reaction models based on four solid-state pyrolysis mechanisms. Two-stage reaction model, i.e., F1 at the early stage and F2 at the later one, is proposed to well describe the kerogen pyrolysis process, which demonstrates a wide applicability owing to their insensitivities on the heating rate and estimation methods of the activation energies. The methodology revealed here could be applicable to determine other solid-state pyrolysis kinetics and reaction mechanism.
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