Origin of natural gases in the autochthonous Miocene strata of the Polish Carpathian Foredeep

• Autorzy: Kotarba M. J.
• Języki publikacji: PL

Abstrakty

EN

Methane concentrations in natural gases accumulated in the autochthonous Miocene strata of the Polish Carpathian Foredeep (between Kraków and Przemyśl) usually exceeded 90 vol%. Methane and part of the ethane were generated during microbial reduction of carbon dioxide in the marine environment, mainly during the sedimentation of Miocene clays and muds. It is possible that this microbial process has continued even recently. Higher light hydrocarbons (mainly propane, butanes and pentanes) were generated during the diagenesis and the initial stage of the low-temperature thermogenic process. Very small changes in the values of geochemical hydrocarbon indices and stable isotope ratios of methane, ethane and propane with depth are evidence for similar gas generation conditions within the whole Badenian and Lower Sarmatian successions. Only in a few natural gas accumulations within the Upper Badenian and Lower Sarmatian reservoirs are thermogenic gases or thermogenic components present, both generated from mixed, type III/II kerogen. These thermogenic gases, now accumulated mainly in the bottom part of Miocene strata, probably resulted from thermogenic processes in the Palaeozoic– Mesozoic basement and then migrated to the Miocene strata along the fault zones. The presence of low hydrogen concentrations (from 0.00 to 0.26 vol%) within the Miocene strata is related to recent microbial processes. Carbon dioxide and nitrogen, which are common minor constituents, were generated in both microbial and low-temperature thermogenic processes. However, CO2 has also undergone secondary processes, mainly dissolution in water during migration. Hydrogen sulphide, which occurs in natural gases of Lower Badenian strata, was most probably generated during microbial sulphate reduction of the Lower Badenian gypsum and anhydrites.

Słowa kluczowe

EN

microbial methane; stable carbon isotopes; thermogenic hydrocarbon gases; carbon dioxide; nitrogen; sulphide hydrogen; autochthonous Miocene strata; Polish Carpathian Foredeep

• Wydawca: Polskie Towarzystwo Geologiczne
• Czasopismo: Annales Societatis Geologorum Poloniae
• Rocznik: 2011
• Tom: Vol. 81, No 3
• Strony: 409--424
• Opis fizyczny: Bibliogr. 60 poz., rys., tab., wykr.

Twórcy

autor

Kotarba M. J.

• AGH University of Science and Technology, Faculty of Geology, Geophys ics and Environmental Protection, Al. Mickiewicza 30, 30-059 Kraków, Poland,

Bibliografia

• 1.Andreyeva-Grigorovich, A. S., Kulchytsky, Y. O., Gruzman, A. D., Lozynyak, P. Y., Petrashkevich, M. I., Portnyagina, L. O., Ivanina, A. V., Smirnov, S. E., Trofimovich, N. A., Savits-kaya, N. A. & Shvareva, N. J., 1997. Regional stratigraphic scheme for Neogene formations of the Central Paratethys in the Ukraine. Geologica Carpathica, 48: 123-136.
• 2.Andreyeva-Grigorovich, A. S., Oszczypko, N., Slączka, A., Oszczypko-Clowes, M., Savitskaya, N. A. & Trofimovicz, N., 2008. New data on the stratigraphy of the folded Miocene Zone at the front of the Ukrainian Outer Carpathians. Acta Geologica Polonica, 58: 325-353.
• 3.Anissimov, L., 1995. Origin of H2S in natural gases: Identification of geochemical processes. In: Grimalt, J. O. & Dorronsoro, C. (eds) Organic geochemistry: developments and applications to energy, climate, environment and human history. Selected Papers from the 17th International Meeting on Organic Geochemistry Donostia-San Sebastian, p. 1113-1114.
• 4.Ballentine, C. J. & Sherwood Lollar, B., 2002. Regional ground-water focusing of nitrogen and noble gases into the Hugoton-Panhandle giant gas field, USA. Geochimica et Cosmochimica Acta, 66: 2483-2497.
• 5.Berner, U. & Faber, E., 1996. Empirical carbon isotope/maturity relationships for gases from algal kerogens and terrigenous organic matter, based on dry, open-system pyrolysis. Organic Geochemistry, 24: 947-955.
• 6.Calikowski, A., 1983. Badania geochemiczne gazów ziemnych miocenu ana obszarze Husów-Kraków. W: Lenk, T. (ed.), Budowa geologiczna, warunki strukturalno-facjalne oraz perspektywy poszukiwań złóż gazu ziemnego w rejonie brzegu i pod nasunięciem Karpat. (In Polish). Prace Instytutu Górnictwa Naftowego i Gazownictwa, 45: 74-81.
• 7.Chung, H. M., Gormly, J. R. & Squires, R. M., 1988. Origin of gaseous hydrocarbons in subsurface environments: theoretical considerations of carbon isotope distribution. Chemical Geology, 71:91-103.
• 8.Coplen, T. B., 1995. Reporting of stable carbon, hydrogen, and oxygen isotopic abundances. In: Reference and intercomparison materials for stable isotopes of light elements. Proceedings of a consultants meeting held in Vienna, 1-3 December 1993. International Atomic Energy Agency, Vienna, p. 31-34.
• 9.Czepiec, I. & Kotarba, M. J., 1998. Paleoecology and organic matter in the Late Badenian and Early Sarmatian marine basin of the Polish part of the Carpathian Foredeep. Przegląd Geologiczny, 46: 732-736.
• 10.Dubessy, J., Pagel, M., Beny, J. M., Christensen, H., Hickel, B., Kosztolanyi, C. & Poty, B., 1988. Radiolysis evidenced by H2-O2 and H2-bearing fluid inclusions in three uranium deposits. Geochimica et Cosmochimica Acta, 52: 1155-1167.
• 11.Florkowski, T., 1985. Sample preparation for hydrogen isotope analysis by mass spectrometry. International Journal of Applied Radiation and Isotopes, 36: 991-992.
• 12.Gerling, P., Idiz, E., Everlien, G. & Sohns, E., 1997. New aspects on the origin of nitrogen in natural gas in Northern Germany. Geologische Jahrbuch, D103: 65-84.
• 13.Glogoczowski, J. J., 1976. Versuch der Aufstellung eines neuen "Hydrat" modells der Erdgasgenerierung im Miözan der Karpatenvorsenke. Zeitschrift für Angewandte Geologie, 26: 156-158.
• 14.Gutsalo, L. K. & Plotnikov, A. M., 1981. Carbon isotopic composition in the CH4-CO2 system as a criterion for the origin of methane and carbon dioxide in Earth natural gases. (In Russian, English summary). Doklady Akademyi Nauk SSSR, 259: 470-473.
• 15.Hałas, S., Lis, J., Szaran, J. & Żuk, W., 1973. Variability of isotopic composition of H2S in presence of deposits of natural gas. (In Polish, English summary). Przegląd Geologiczny, 21: 280-281.
• 16.Hawkes, H. E., 1972. Free hydrogen in genesis of petroleum. American Association of Petroleum Geologists Bulletin, 56: 2268-2277.
• 17.Hinrichs, K-U., Hayes, J. M., Bach, W., Spivack, A. J., Hmelo, L. R., Holm, N. G., Johnson, C. G. & Sylva, S. P., 2006. Biological formation of ethane and propane in the deep marine sediments. Proceedings National Academy of Sciences, 103: 14684-14689.
• 18.Jawor, E. & Kotarba, M., 1993. Origin of natural gas accumulated in Cenomanian and Miocene reservoirs in Brzezowiec field. (In Polish, English summary). Nafta, 49: 47-53.
• 19.Karnkowski, P., 1999. Oil and gas deposits in Poland. Geological Society "Geos", Kraków, 380 pp.
• 20.Kotarba, M., 1988. Geochemical criteria of origin of gases accumulated in the Upper Carboniferous coal-bearing strata of the Wałbrzych basin. (In Polish, English summary). Zeszyty Naukowe Akademii Górniczo-Hutniczej, 1199, Geologia, 42: 1 - 119.
• 21.Kotarba, M., 1992. Bacterial gases in Polish part of the Carpathian Foredeep and the Flysch Carpathians: isotopic and geological approach. In: Vially, R. (ed.), Bacterial Gas. Editions Technip, Paris, pp. 133-146.
• 22.Kotarba, M. J., 1995. Proces generowania siarkowodoru w utworach miocenu zapadliska przedkarpackiego. In: Geneza gazów akumulowanych w utworach miocenu zapadliska przedkarpackiego. (In Polish). AGH University of Science and Technology, Unpublished report, Kraków: 87-92.
• 23.Kotarba, M. J., 1998. Composition and origin gaseous hydrocarbons in the Miocene strata of the Polish part of the Carpathian Foredeep. Przegląd Geologiczny, 46: 751-758.
• 24.Kotarba, M. & Jawor, E., 1993. Petroleum generation, migration and accumulation in the Miocene sediments and Paleozoic-Mesozoic basement complex of the Carpathian Foredeep between Cracow and Pilzno (Poland). In: Spencer, A. M. (ed.), Generation, accumulation and production of Europe's hydrocarbons. Special Publication of the European Association of Petroleum Geologists, 3, Springer, Heidelberg: 295-301.
• 25.Kotarba, M. J. & Koltun, Y. V., 2006. The origin and habitat of hydrocarbons of the Polish and Ukrainian Parts of the Carpathian Province. In: Golonka, J. & Picha, F. J. (eds), The Carpathians and their foreland: geology and hydrocarbon resources. American Association of Petroleum Geologists, Memoir, 84: 395^42.
• 26.Kotarba, M. J. & Lewan, M. D., 2004. Characterizing thermogenic coalbed gas from Polish coals of different ranks by hydrous pyrolysis. Organic Geochemistry, 35: 615-646.
• 27.Kotarba, M. J. & Nagao, K., 2008. Composition and origin of natural gases accumulated in the Polish and Ukrainian parts of the Carpathian region: Gaseous hydrocarbons, noble gases, carbon dioxide and nitrogen. Chemical Geology, 255: 426- 438.
• 28.Kotarba, M., Szafran, S. & Espitalié, J., 1987. A study of organic matter and natural gases of Miocene sediments in the Polish part of the Carpathian Foredeep. Chemical Geology, 64: 197-207.
• 29.Kotarba, M. J., Kisielowska, E., Więcław, D., Akimienko, V., Bondar, V. A., Laurenavichus, K. S. & Zyakun, A. M., 1995. Badania mikrobiologiczne metanogenezy w utworach miocenu zapadliska przedkarpackiego. In: Geneza gazów akumulowanych w utworach miocenu zapadliska przedkarpackiego. (In Polish). AGH University of Science and Technology, Unpublished report, Kraków: 81-86.
• 30.Kotarba, M. J., Wilczek, T., Kosakowski, P., Kowalski, A. & Więcław D., 1998a. A study of organic matter and habitat of gaseous hydrocarbons in the Miocene strata of the Polish part of the Carpathian Foredeep. Przegląd Geologiczny, 46: 742-750.
• 31.Kotarba, M. J., Burzewski, W., Wilczek, T., Słupczyński, K., Kosakowski, P. & Botor, D., 1998b. Model of gaseous hydrocarbon generation in the Miocene strata of the Polish part of the Carpathian Foredeep. Przegląd Geologiczny, 46: 737-742.
• 32.Kotarba, M. J., Więcław, D., Kosakowski, P. & Kowalski, A., 2005. Hydrocarbon potential of source rocks and origin of natural gases accumulated in Miocene strata of the Carpathian Foredeep in Rzeszów area. (In Polish, English summary). Przegląd Geologiczny, 53: 67-76.
• 33.Kotarba, M. J., Curtis, J. B. & Lewan, M. D., 2009. Comparison of natural gases accumulated in Oligocene strata with hydrous pyrolysis gases from Menilite Shales of the Polish Outer Carpathians. Organic Geochemistry, 40: 769-783.
• 34.Kotarba, M. J., Peryt, T. & Koltun, Y. V., 2011. Model of micro-bial gas generation and prospectives of hydrocarbon exploration in the Miocene strata in the Polish and Ukrainian Carpathian Foredeep. Annales Societatis Geologorum Poloniae, 81: 523-548.
• 35.Krooss, B. M., Littke, R., Müller, B., Frielingsdorf, J., Schwochau, K. & Idiz, E. F., 1995. Generation of nitrogen and methane from sedimentary organic matter: implications on the dynamics of natural gas accumulations. Chemical Geology, 126: 291-318.
• 36.Krooss, B. M., Friberg, L., Gensterblum, Y., Hollenstein, J., Prinz, D. & Littke, R., 2005. Investigation of the pyrolytic liberation of molecular nitrogen from Paleozoic sedimentary rocks. International Journal of Earth Sciences, 94: 1023-1038.
• 37.Krouse, H. R., 1980. Stable isotope geochemistry of non-hydrocarbon constituents of natural gas. Proceedings of the World Petroleum Congress, Bucharest, 10: 85-92.
• 38.Krouse, H. R., Viau, C. A., Eliuk, L. S., Ueda, A. & Halas, S., 1988. Chemical and isotopic evidence of thermochemical sulfate reduction by light hydrocarbon gases in deep carbonate reservoirs. Nature, 333: 415-419.
• 39.Lillis, P. G., 2007. Upper Cretaceous microbial petroleum systems in north-central Montana. The Mountain Geologist, 44: 11-35.
• 40.Maksimov, S. P., Ancupov, P. V., Botnieva, T. A., Niecajev, O. L., Karnkowski, P., Korab, Z., Stępniewska, E. & Calikowski, A., 1982. Gases of the Zechstein Main Dolomite. (In Polish, English summary). Nafta, 38, 6: 41-44.
• 41.Myśliwiec, M., Plezia, B. & Świętnicka, G., 2004. The Miocene gas fields discovered in the NE part of the Carpathian Foredeep on the base of the Direct Hydrocarbon Indicators on the seismic data. (In Polish, English summary). Przegląd Geologiczny, 52: 395-402.
• 42.Ney, R., Burzewski, W., Bachleda, T., Górecki, W., Jakóbczak, K. & Słupczyński, K., 1974. Outline of paleogeography and evolution of lithology and facies of Miocene layers of the Carpathian Foredeep. (In Polish, English summary). Prace Geologiczne Komisji Nauk Geologicznych PAN, Oddział w Krakowie, 82: 1-65.
• 43.Oremland, R. S., Whiticar, M. J., Strohmaier, F. S. & Kiene, R. P., 1986. Bacterial ethane formation from reduced, ethylated sulfur compounds in anoxic sediments. Geochimica et Cosmochimica Acta, 52: 1895-1904.
• 44.Oszczypko, N., 1997. The Early-Middle Miocene Carpathian peripheral foreland basin (Western Carpathians, Poland). Przegląd Geologiczny, 45: 1054-1063.
• 45.Oszczypko, N. & Ślączka, A., 1989. Evolution of Miocene basin in the Polish Outer Carpathians and their Foredeep. Geologica Carpathica, 40: 9-28.
• 46.Oszczypko, N., Krzywiec, P., Popadyuk, I. & Peryt, T., 2006. Carpathian Foredeep Basin (Poland and Ukraine): Its sedimentary, structural, and geodynamic evolution. In: Golonka, J. & Picha, F. J. (eds), The Carpathians and their foreland: geology and hydrocarbon resources, American Association of Petroleum Geologists, Memoir, 84: 293-350.
• 47.Rice, D. D., 1992. Controls, habitat, and resource potential of ancient bacterial gas. In: Vially, R. (ed.), Bacterial Gas. Editions Technip, Paris: 91-117.
• 48.Rice, D. D. & Claypool, J., 1981. Generation, accumulation and resource potential of biogenic gas. American Association of Petroleum Geologists Bulletin, 65: 5-25.
• 49.Rooney, M. A., Claypool, G. E. & Chung, H. M., 1995. Modeling thermogenic gas generation using carbon isotope ratios of natural gas hydrocarbons. Chemical Geology, 126: 219-232.
• 50.Savary, V. & Pagel, M., 1997. The effects of water radiolysis on local redox conditions in the Oklo, Gabon, natural fission reactors 10 to 16. Geochimica et Cosmochimica Acta, 61: 4479-4494.
• 51.Schoell, M., 1988. Multiple origins of methane in the Earth. Chemical Geology, 71: 1-10.
• 52.Stahl, W., 1977. Carbon and nitrogen isotopes in hydrocarbon re-search and exploration. Chemical Geology, 20: 121-149.
• 53.Worden, R. H., Smalley, P. C. & Oxtoby, N. H., 1995. Gas souring by thermochemical sulphate reduction at 140°C. American Association of Petroleum Geologists Bulletin, 79: 854-863.
• 54.Whiticar, M. J., 1994. Correlation of natural gases with their sources. In: Magoon, L. B. & Dow, W. G. (eds), The petroleum system -from source to trap. American Association of Petroleum Geologists Memoir, 60: 261-283.
• 55.Whiticar, M. J., Faber, E. & Schoell, M., 1986. Biogenic methane formation in marine and freshwater environments: CO2 reduction vs. acetate fermentation - Isotope evidence. Geochimica et Cosmochimica Acta, 50: 693-709.
• 56.Zinger, A. S., 1962. Molecular hydrogen in gas dissolved in waters of oil-gas fields, Lower Volga Region. Geochemistry, 10: 1015-1023.
• 57.Zobell, C. R., 1947. Microbial transformation of molecular hydrogen in marine sediments, with particular reference to petroleum. American Association of Petroleum Geologists Bulletin, 31: 1709-1751.
• 58.Zhang, T., Amrani, A., Ellis, G. S., Ma, Q. & Tang, Y., 2008. Experimental investigation on thermochemical sulfate reduction by H2S initiation. Geochimica et Cosmochimica Acta, 72: 3518-3530.
• 59.Zhu, Y., Shi, B. & Fang, C., 2000. The isotopic compositions of molecular nitrogen: implications on their origins in natural gas accumulations. Chemical Geology, 164: 321-330.
• 60.Zou, Y.-R., Cai, Y., Zhang, Ch., Zhang, X. & Peng, P., 2007. Variations of natural gas carbon isotope-type curves and their interpretation - A case study. Organic Geochemistry, 38: 1398-1415.