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Variations of yields and molecular and isotopic compositions in gases generated from Miocene strata of the Carpathian Foredeep (Poland) as determined by hydrous pyrolysis

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Abstract

Hydrous pyrolysis (HP) experiments at 330 and 355 °C for 72 h have been performed to simulate gas generation and expulsion, and to evaluate the yields of hydrocarbon and non-hydrocarbon components of thermogenic gases generated and expelled from shales of the Miocene strata of the Polish Outer Carpathian Foredeep (POCF). Mechanisms of thermogenic gas generation and expulsion were established based on the results of Rock–Eval, vitrinite reflectance Ro and δ13C of organic matter and mineralogical analyses of the matrix of original shales and shales after HP experiments, as well as the yields, molecular and stable carbon, hydrogen, nitrogen and sulphur isotope compositions of gases generated during HP. The analysed Miocene immature dispersed organic matter in clayey–muddy deposits is mainly type III kerogen. The yield of methane generated from shales of the Lower and Upper Badenian Skawina Formation in the western sector of POCF is higher than that the Upper Badenian and Lower Sarmatian strata of the eastern sector. A partial isotopic reversal of δ13C1 < δ13C3 < δ13C2 was observed in all gases produced at both HP 330 and 355 °C. CO2 can be mainly generated during HP by the dissolution of carbonates and to a lesser extent by decarboxylation. H2S generation during HP can be related to the decomposition of both organic and inorganic compounds. N2 was produced by the decomposition of nitrogen bonds of organic matter.

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source rock maturity after Gerling et al. (1997) and range of fixed-NH4 after Mingram et al. (2005). For sample keys and stratigraphy of samples see Table 5 and Fig. 11

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Acknowledgements

This research was undertaken as part of the Polish National Science Centre under grant no. UMO-2016/22/M/ST10/00589 (AGH University of Science and Technology, no. 28.28.140.70320). We would like to express our gratitude to two anonymous reviewers for their constructive comments and suggestions and to Paul Lillis, emeritus geochemist of the U.S. Geological Survey in Denver for improvement of both earlier and final versions of this manuscript. Sample collecting and experimental, analytical and editorial works by Joanna Gawęda-Skrok, Natalia Kmiecik, Adam Kowalski, Tomasz Kowalski, Jolanta Lepiarczyk, Tomasz Romanowski and Hieronim Zych from the AGH University of Science and Technology in Kraków are gratefully acknowledged.

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  1. Faculty of Geology, Geophysics and Environmental Protection, AGH University of Science and Technology, Al. Mickiewicza 30, 30-059, Kraków, Poland

    Maciej J. Kotarba, Elżbieta Bilkiewicz, Tomasz Bajda, Marta Waliczek & Krzysztof Jurek

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Kotarba, M.J., Bilkiewicz, E., Bajda, T. et al. Variations of yields and molecular and isotopic compositions in gases generated from Miocene strata of the Carpathian Foredeep (Poland) as determined by hydrous pyrolysis. Int J Earth Sci (Geol Rundsch) 111, 1823–1858 (2022). https://doi.org/10.1007/s00531-022-02206-0

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