Kinetic and equilibrium reactions on natural and laboratory generation of thermogenic gases from Type II marine shale

Li, Xiaoqiang; Horita, Juske

doi:10.1016/j.gca.2022.07.020

Kinetic and equilibrium reactions on natural and laboratory generation of thermogenic gases from Type II marine shale

Journal Article · Mon Jul 25 00:00:00 EDT 2022 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2022.07.020· OSTI ID:1977159

Li, Xiaoqiang ^[1]; Horita, Juske ^[2]

Texas Tech Univ., Lubbock, TX (United States); OSTI
Texas Tech Univ., Lubbock, TX (United States)

The phenomenon that laboratory pyrolysis experiments produce much wetter gases than those in natural reservoirs is a long-recognized and debated problem in the investigation of natural gases in sedimentary basins. In this study, we explore the discrepancy by pyrolyzing a type II kerogen from the Woodford Shale in Oklahoma, compared with the previous results on the produced natural gases from the Arkoma Basin generated from the same source rock (Liu et al., 2019) with the discussion of gas and isotopic compositions at bulk and position-specific (PS) levels. An improved GC-pyrolysis-GC IRMS method is applied for the determination of PS δ¹³C of propane produced in the pyrolysis of the Woodford Shale at Easy %R_o from 0.76 to 3.27. Kinetic and thermodynamic considerations of the chemical and isotopic compositions of the natural and laboratory pyrolysis gases suggest that the generation of light hydrocarbons involves uni-directional cracking reactions, exchange reactions with water, and likely reversible reactions among light hydrocarbons and other H-containing volatiles. After the gas generation in the unconventional Woodford Shale reservoirs, the C₁-C₄ gases might have approached close to chemical equilibrium of C₁-C₃ and isotope equilibrium of C₂-C₁ and C₃-C₁ pairs at their peak temperatures. The capping H for the generation of C₁-C₄ in the Woodford Shale gases appears to have experienced at least partial exchange with the water, while that in the pyrolysis gases is only originated from organic-bound compounds with large kinetic isotope effects (KIE). Our findings indicate that elevated compound-specific and PS δ¹³C values of propane in the wet-gas cracking stage are significantly influenced by the breakdown of the thermally stable compounds (e.g., remaining kerogen, residues). A first synthesis of PS δ¹³C and δ²H isotopic compositions of propane from this study and the literature data suggests relatively similar isotopic structures of propane precursors in kerogens. Finally, this study demonstrates that PS isotope analysis of propane can contribute to identifying various geological (e.g., maturation, wet-gas cracking, H exchange, diffusion) and biodegradation processes.

View Accepted Manuscript (DOE)

Research Organization:: Texas Tech Univ., Lubbock, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0016271

OSTI ID:: 1977159

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Journal Issue: C Vol. 333; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Kinetic and equilibrium reactions on natural and laboratory generation of thermogenic gases from Type II marine shale

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