Skip to main content
Log in

Origin and secondary processes in petroleum in the eastern part of the Polish Outer Carpathians

  • Original Paper
  • Published:
International Journal of Earth Sciences Aims and scope Submit manuscript

Abstract

A geochemical study of crude oil and natural gas from producing wells and seeps within the Lower Cretaceous–Oligocene sandstone reservoirs of the most eastern part of the Polish Outer Carpathians was conducted for the evaluation of their origin, migration pathways and the effects of secondary processes (biodegradation, water washing and evaporative fractionation). The petroleum was generated from mixed marine/terrigenous organic matter (type-II/III kerogen) occurring mostly in Oligocene Menilite beds in the Silesian and Skole nappes. Shales within Upper Cretaceous–Palaeocene Istebna and Lower Cretaceous Veřovice, Lgota and Spas beds are considered as an additional source of hydrocarbons (mainly gaseous). Biodegradation processes were recorded in numerous oils, especially occurring in seeps, but the extent of these processes is not severe, because steranes and terpanes were not affected. All oils are more-or-less water washed, while the evaporative fractionation processes are developed only on a minimal scale. The natural gases are primarily of thermogenic origin, usually co-genetic with oil and often contain components of secondary microbial degradation of both oil and natural gas (13C-enriched CO2 and 13C-depleted CH4). Gases with the highest microbial methane contribution have been recorded in petroleum accumulated in Dwernik and Łodyna fields.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11
Fig. 12
Fig. 13
Fig. 14
Fig. 15
Fig. 16
Fig. 17
Fig. 18
Fig. 19
Fig. 20
Fig. 21

Similar content being viewed by others

References

  • Aitken CM, Jones DM, Larter SR (2004) Anaerobic hydrocarbon biodegradation in deep subsurface oil reservoirs. Nature 431:291–294

    Google Scholar 

  • Akinlua A, Ajayi TR, Adeleke BB (2006) Niger Delta oil geochemistry: Insight from light hydrocarbons. J Petrol Sci Eng 50:308–314

    Google Scholar 

  • Asif M, Grice K, Fazeelat T (2009) Assessment of petroleum biodegradation using stable hydrogen isotopes of individual saturated hydrocarbon and polycyclic aromatic hydrocarbon distributions in oils from the Upper Indus Basin, Pakistan. Org Geochem 40:301–311

    Google Scholar 

  • Baciu C, Ionescu A, Etiope G (2018) Hydrocarbon seeps in Romania: Gas origin and release to the atmosphere. Mar Petrol Geol 89:130–143

    Google Scholar 

  • Baskin DK, Peters KE (1992) Early generation characteristics of a sulfur-rich Monterey kerogen. AAPG Bull 16:1–13

    Google Scholar 

  • Beach F, Peakman TM, Abbot GD, Sleeman R, Maxwell JR (1989) Laboratory thermal alteration of triaromatic steroid hydrocarbons. Org Geochem 14:109–111

    Google Scholar 

  • 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. Org Geochem 24:947–955

    Google Scholar 

  • Berner U, Faber E (1997) Carbon isotope/maturity relationships for gases from algal kerogens and terrigenous organic matter. Geol Jahrb D103:129–145

    Google Scholar 

  • Bessereau G, Roure F, Kotarba MJ, Kuśmierek J, Strzetelski W (1996) Structure and hydrocarbon habitat of the Polish Carpathians. In: Ziegler PA, Horvath F (eds) Peri-Tethys Memoir 2: Structure and Prospects Alpine Basins and Forelands, Mém Muséum Nat d’Hist Natur 170:343–373

  • Blanc P, Connan J (1994) Preservation, degradation, and destruction of trapped oil. In: Magoon LB, Dow WG (eds) The petroleum system—from source to trap. AAPG Memoir, vol 60. The American Association of Petroleum Geologists, Tulsa, OK, pp 237–247

    Google Scholar 

  • Boote DRD, Sachsenchofer RF, Tari G, Arbouille D (2018) Petroleum provinces of the Paratethyan Region. J Petrol Geol 41:247–298

    Google Scholar 

  • Chen J, Zhang H, Huang H, Li X, Shi S, Liu F, Chen L (2013) Impact of anaerobic biodegradation on alkylphenanthrenes in crude oil. Org Geochem 61:6–14

    Google Scholar 

  • Cheng X, Hou D, Xu C, Wang F (2016) Biodegradation of tricyclic terpanes in crude oils from the Bohai Bay Basin. Org Geochem 101:11–21

    Google Scholar 

  • Cheng X, Hou D, Mao R, Xu C (2018) Severe biodegradation of polycyclic aromatic hydrocarbons in reservoired crude oils from the Miaoxi Depression, Bohai Bay Basin. Fuel 211:859–867

    Google Scholar 

  • Chung HM, Gormly JR, Squires RM (1988) Origin of gaseous hydrocarbons in subsurface environments: theoretical considerations of carbon isotope distribution. Chem Geol 71:91–103

    Google Scholar 

  • Cieszkowski M, Ślączka A (2001) The Polish Carpathians—General geology. In: Paulo A, Krobicki M (eds) Field trip C. 12th Meeting of Association of European Geological Societies & 72nd Convention of Polish Geological Association, pp 99–108

  • Connan J (1984) Biodegradation of crude oils in reservoirs. In: Brooks J, Welte DH (eds) Advances in petroleum geochemistry, vol 1. Academic Press, London, pp 299–335

    Google Scholar 

  • Coplen TB (2011) Guidelines and recommended terms for expression of stable-isotope-ratio and gas-ratio measurement results. Rapid Commun Mass Spectrom 25:2538–2560

    Google Scholar 

  • Curtis JB, Kotarba MJ, Lewan MD, Więcław D (2004) Oil/source rock correlations in the Polish Flysch Carpathians and Mesozoic basement and organic facies of the Oligocene Menilite Shales: insights from hydrous pyrolysis experiments. Org Geochem 35:1573–1596

    Google Scholar 

  • Dahl JE, Moldovan JM, Peters KE, Claypool GE, Rooney MA, Michael GE, Mello MR, Kohnen ML (1999) Diamondoid hydrocarbons as indicators of natural oil cracking. Nature 399:54–57

    Google Scholar 

  • Dai J, Song Y, Dai C, Wang D (1996) Geochemistry and accumulation of carbon dioxide gases in China. AAPG Bull 10:1615–1626

    Google Scholar 

  • Dai J, Chen H, Shen X (2005) Geochemistry and occurrence of inorganic gas accumulations in Chinese sedimentary basins. Org Geochem 36:1664–1688

    Google Scholar 

  • Davis JB (1967) Petroleum microbiology. Elsevier, Amsterdam

    Google Scholar 

  • Didyk BM, Simoneit BRT, Brassel SC, Eglinton G (1978) Organic geochemical indicators of paleoenvironmental conditions of sedimentation. Nature 272:216–222

    Google Scholar 

  • Dolfing J, Larter SR, Head IM (2008) Thermodynamic constraints on methanogenic crude oil biodegradation. ISME J 2:442–452

    Google Scholar 

  • Dziadzio PS, Borys Z, Kuk S, Masłowski E, Probulski J, Pietrusiak M, Górka A, Moryc J, Baszkiewicz A, Karnkowski P, Karnkowski PH, Pietrusiak M (2006) Hydrocarbon resources of the Polish Outer Carpathians—reservoir parameters, trap types, and selected hydrocarbon fields: A stratigraphic review. In: Golonka J, Picha FJ (eds) The Carpathians and their foreland: geology and hydrocarbon resources. AAPG Memoir, vol 84. The American Association of Petroleum Geologists, Tulsa, OK, pp 259–291

    Google Scholar 

  • Dziadzio PS, Matyasik I, Garecka M, Szydło A (2016) Lower Oligocene Menilite Beds, Polish Outer Carpathians: supposed deep-sea flysch locally reinterpreted as shelfal, based on new sedimentological, micropalaeontological and organic-geochemical data. Prace Naukowe Instytutu Nafty i Gazu - Państwowego Instytutu Badawczego 213:119

    Google Scholar 

  • Etiope G, Feyzullayev A, Milkov AV, Waseda A, Mizobe K, Sun CH (2009) Evidence of subsurface anaerobic biodegradation of hydrocarbons and potential secondary methanogenesis in terrestrial mud volcanoes. Mar Petrol Geol 26:1692–1703

    Google Scholar 

  • Forsythe JC, Martin R, De Santo I, Tyndall R, Arman K, Pye J, De Nicolais N, Nelson RK, Pomerantz AE, Kenyon-Roberts S, Zuo JY, Betancourt SS, Reddy C, Peters KE, Mullins OC (2017) Integrating comprehensive two-dimensional gas chromatography and downhole fluid analysis to validate a spill-fill sequence of reservoirs with variations of biodegradation, water washing and thermal maturity. Fuel 191:538–554

    Google Scholar 

  • Galimov EM (1986) Isotopic method for the revealing of oil source deposits on the example of some regions of the USSR. Izv Academ Nauk SSSR, Ser Geol 4:3–21 (in Russian)

    Google Scholar 

  • Golonka J, Gahagan L, Krobicki M, Marko F, Oszczypko N, Ślączka A (2006) Plate-tectonic evolution and paleogeography of the circum-Carpathian region. In: Golonka J, Picha FJ (eds) The Carpathians and their foreland: geology and hydrocarbon resources. AAPG Memoir, vol 84. The American Association of Petroleum Geologists, Tulsa, OK, pp 11–46

    Google Scholar 

  • Gondek B, Pomykała Z (1982) Carpathian crude oils in the light investigation of of n-alkane and isoprenoid hydrocarbons. Przegląd Geologiczny 30:64–69 (in Polish with English abstract)

    Google Scholar 

  • Gong D, Ma R, Chen G, Ma W, Liao F (2017) Geochemical characteristics of biodegraded natural gas and its associated low molecular weight hydrocarbons. J Nat Gas Sci Eng 46:338–349

    Google Scholar 

  • Grice K, Robert A, Kagi RI (2000) Diamandoid hydrocarbon ratios as indicators od biodegradation in Australian crude oils. Org Geochem 31:67–73

    Google Scholar 

  • Grieg LM, Duncan KE, Suflita JM (2008) Bioenergy production via microbial conversion of residual oil to natural gas. Appl Environ Microbiol 74:3022–3029

    Google Scholar 

  • Hajto M, Szewczyk J (2013) Thermal analysis of the Eastern Carpathians. In: Górecki W (ed) Geothermal atlas of the Eastern Carpathians. Kraków, AGH-UST, pp 454–483 (in Polish with English summary)

    Google Scholar 

  • Holba AG, Dzou LIP, Hickey JJ, Franks SG, May SJ, Lenney T (1996) Reservoir geochemistry of South Pass 61 Field, Gulf of Mexico: Compositional heterogeneities relfecting filling history and biodegradation. Org Geochem 24:1179–1198

    Google Scholar 

  • Huang W-Y, Meinschein WG (1979) Sterols as ecological indicators. Geochim Cosmochim Acta 43:739–745

    Google Scholar 

  • Hughes WB, Holba AG, Dzou LIP (1995) The ratios of dibenzothiophene to phenantrene and pristine to phytane as indicators of depositional environment and lithology of petroleum source rocks. Geochim Cosmochim Acta 59:3581–3598

    Google Scholar 

  • Jaekel U, Musat N, Adam B, Kuypers M, Grundmann O, Musat F (2013) Anaerobic degradation of propane and butane by sulfate-reducing bacteria enriched from marine hydrocarbon cold seeps. ISME J 7:885–895

    Google Scholar 

  • James AT, Burns BJ (1984) Microbial alteration of subsurface natural-gas accumulations. AAPG Bull 68:957–960

    Google Scholar 

  • Jankowski L, Kopciowski R, Ryłko W (2004) Geological map of the Outer Carpathians: borderlands of Poland, Ukraine and Slovakia. Pol Geol Institute, Warsaw

    Google Scholar 

  • Jones DM, Head IM, Gray ND, Adams JJ, Rowan AK, Aitken CM, Bennett B, Huang H, Brown A, Bowler BF, Oldenburg T, Erdmann M, Larter SR (2008) Crude-oil biodegradation via methanogenesis in subsurface petroleum reservoirs. Nature 451:176–180

    Google Scholar 

  • Karnkowski P (1999) Oil and gas deposits in Poland. Geological Society “Geos”, Krakow

    Google Scholar 

  • Karnkowski P, Ozimkowski W (1998) The distribution of oil and gas fields in relation to satellite image interpretation: an example from the Polish East Carpathians and the adjacent foredeep. J Petrol Geol 21:213–231

    Google Scholar 

  • Köester J, Rospondek M, Schouten S, Kotarba M, Zubrzycki A, Sinninghe Damste JS (1998) Biomarker geochemistry of a foreland basin: Oligocene Menilite Formation in the Flysch Carpathians of Southeast Poland. Org Geochem 29:649–669

    Google Scholar 

  • Koltun YV (1992) Organic matter in Oligocene Menilite Formation rocks of the Ukrainian Carpathians: palaeoenvironment and geochemical evolution. Org Geochem 18:423–430

    Google Scholar 

  • Koltun Y, Espitalie J, Kotarba M, Roure F, Ellouz N, Kosakowski P (1998) Petroleum generation in the Ukrainian External Carpathians and their adjacent foreland. J Petrol Geol 3:265–268

    Google Scholar 

  • Kosakowski P, Więcław D, Kotarba MJ (2009) Source rock characteristic of the selected flysch deposits in the transfrontier area of the Polish Outer Carpathians. Geologia AGH 35:155–190 (in Polish with English abstract)

    Google Scholar 

  • Kosakowski P, Koltun Y, Machowski G, Poprawa P, Papiernik B (2018) The geochemical characteristics of the Oligocene–Lower Miocene Menilite Formation in the Polish and Ukrainian Outer Carpathians: a review. J Petrol Geol 41:319–335

    Google Scholar 

  • Köster J, Kotarba M, Lafargue E, Kosakowski P (1998) Source rock habitat and hydrocarbon potential of Oligocene Menilite Beds (Flysch Carpathians, Southeast Poland): an organic geochemical and isotope approach. Org Geochem 29:543–558

    Google Scholar 

  • Koszarski L, Geroch S, Wiser T, Naeser C (1985) Scheme of chronostratigraphy of Polish Carpathians flysch deposits based on tephrochronological data. Fundamental researches in the western part of the Polish Carpathians: GUIDE to excursion 1. Carpatho-Balkan Geol Assoc XIII Congress, Krakow, p 30

    Google Scholar 

  • Kotarba MJ (1998) Isotopic and pyrolysis studies of organic matter and natural gases from the Flysch Carpathian strata of the Kuźmina-1 deep well (Poland). Abstracts of AAPG Annual Meeting, Salt Lake City, May 17–20, A375, p 6

  • Kotarba MJ, Koltun YV (2006) Origin and habitat of hydrocarbons of the Polish and Ukrainian parts of the Carpathian Province. In: Golonka J, Picha FJ (eds) The Carpathians and their foreland: geology and hydrocarbon resources. AAPG Memoir, vol 84. The American Association of Petroleum Geologists, Tulsa, OK, pp 395–443

    Google Scholar 

  • Kotarba MJ, 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. Chem Geol 255:426–438

    Google Scholar 

  • Kotarba MJ, Nagao K (2015) Molecular and isotopic compositions and origin of natural gases from Cambrian and Carboniferous-Lower Permian reservoirs of the onshore Polish Baltic region. Int J Earth Sci 104:241–261

    Google Scholar 

  • Kotarba MJ, Więcław D, Koltun YV, Lewan MD, Marynowski L, Dudok IV (2005) Organic geochemical study and genetic correlations between the Oligocene Menilite source rocks and oil and natural gas from surface seepages and from deep accumulations in the Starunia area (Ukrainian Carpathians). In: Kotarba MJ (ed) Polish and Ukrainian geological survey in 2004–2005 years in Starunia at the area of finds of woolly rhinoceroses and other extinct vertebrates. Polish Geological Institute and “Geosphere”, Warszawa–Kraków, pp 125–146

    Google Scholar 

  • Kotarba MJ, Wieclaw D, Koltun YV, Marynowski L, Kuśmierek J, Dudok IV (2007) Organic geochemical study and genetic correlation of natural gas, oil and Menilite source rocks in the area between San and Stryi rivers (Polish and Ukrainian Carpathians). Org Geochem 38:1431–1456

    Google Scholar 

  • Kotarba MJ, Curtis JB, Lewan MD (2009a) Comparison of natural gases accumulated in Oligocene strata with hydrous pyrolysis from Menilite Shales of the Polish Outer Carpathians. Org Geochem 40:769–783

    Google Scholar 

  • Kotarba MJ, Fabiańska M, Więcław D, Kowalski A, Zych H (2009b) Biological markers and stable carbon isotope studies of bitumen impregnating quaternary sediments at Starunia palaeontological site and vicinity (Carpathian region, Ukraine). Ann Soc Geol Pol 79:463–480

    Google Scholar 

  • Kotarba MJ, Więcław D, Dziadzio P, Kowalski A, Bilkiewicz E, Kosakowski P (2013) Organic geochemical study of source rocks and natural gas and their genetic correlation in the central part of the Polish Outer Carpathians. Mar Petrol Geol 45:106–120

    Google Scholar 

  • Kotarba MJ, Więcław D, Dziadzio P, Kowalski A, Kosakowski P, Bilkiewicz E (2014) Organic geochemical study of source rocks and natural gas and their genetic correlation in the eastern part of the Polish Outer Carpathians and Palaeozoic–Mesozoic basement. Mar Petrol Geol 56:97–122

    Google Scholar 

  • Kotarba MJ, Więcław D, Bilkiewicz E, Dziadzio P, Kowalski A (2017) Genetic correlation of source rocks and natural gas in the Polish Outer Carpathians and Paleozoic–Mesozoic basement east of Kraków (southern Poland). Geol Q 61:569–589

    Google Scholar 

  • Kotarba MJ, Więcław D, Bilkiewicz E, Radkovets NY, Koltun YV, Kmiecik N, Romanowski T, Kowalski A (2019) Origin of oil and natural gas in the western part of the Ukrainian Outer Carpathians: geochemical and geological approach. Mar Petrol Geol 103:596–619

    Google Scholar 

  • Kruge MA, Mastalerz M, Solecki A, Stankiewicz BA (1996) Organic geochemistry and petrology of oil source rocks, Carpathian Overthrust region, southeastern Poland—implications for petroleum generation. Org Geochem 24:897–912

    Google Scholar 

  • Książkiewicz M (1977) The tectonics of the Carpathians. In: Pożaryski W (ed) Geology of Poland, vol 4. Tectonics. Wydawnictwo Geologiczne, Warszawa, pp 476–620

    Google Scholar 

  • Kuśmierek J, Machowski G (2008) Oil seeps in the area of the eastern Polish Carpathians and their prognostic significance. Prace Instytutu Nafty i Gazu 150:247–250 (in Polish with English abstract)

    Google Scholar 

  • Larter S, di Primio R (2005) Effects of biodegradation on oil and gas field PVT properties and the origin of oil rimmed gas accumulations. Org Geochem 36:299–310

    Google Scholar 

  • Larter S, Wilhelms A, Head I, Koopmans M, Aplin A, di Primio R, Zwach C, Erdmann M, Telnaes N (2003) The controls on the composition of biodegraded oils in the deep subsurface—part 1: biodegradation rates in petroleum reservoirs. Org Geochem 34:601–613

    Google Scholar 

  • Lewan MD (1984) Factors controlling the proportionality of vanadium to nickel in crude oils. Geochim Cosmochim Acta 48:2231–2238

    Google Scholar 

  • Lewan MD, Kotarba MJ, Curtis JB, Więcław D, Kosakowski P (2006) Oil generation kinetics for organic facies with Type-II and -IIS kerogen in the Menilite Shales of the Polish Carpathians. Geochim Cosmochim Acta 70:3351–3368

    Google Scholar 

  • López L (2014) Study of the biodegradation levels of oils from the Orinoco Oil Belt (Junin area) using different biodegradation scales. Org Geochem 66:60–69

    Google Scholar 

  • Lubaś J (2007) Possibilities of enhanced oil recovery of the Carpathian oil deposits. Wiadomości Naftowe i Gazownicze 10:4–8 (in Polish)

    Google Scholar 

  • Maćkowski T, Kuśmierek J, Reicher B, Baran U, Kosakowski P, Łapinkiewicz AP, Machowski G, Papiernik B, Szczygieł M, Zając A, Zych I (2009) Two-dimensional models of the organic-matter thermal transformation and hydrocarbon expulsion in the transfrontier zone of the Polish and Ukrainian Carpathians. Geologia AGH 35:191–222 (in Polish with English abstract)

    Google Scholar 

  • Magnier C, Moretti I, Lopez JO, Gaumet F, Lopez JG, Letouzey J (2004) Geochemical characterization of source rocks, crude oils and gases of Northwest Cuba. Mar Petrol Geol 21:195–214

    Google Scholar 

  • Marcinkowski A, Szewczyk E (2008) Productivity of Carpathian reservoir rocks in the light of hydrocarbon production history. Geologia AGH 34:405–421 (in Polish with English abstract)

    Google Scholar 

  • Marzi R, Torkelson BE, Olson RK (1993) A revised carbon preference index. Org Geochem 20:1303–1306

    Google Scholar 

  • Masterson WD, Dzou LIP, Holba AG, Fincannon AL, Ellis L (2001) Evidence for biodegradation and evaporative fractionation in West Sak, Kuparuk and Prudhoe Bay field areas, North Slope, Alaska. Org Geochem 32:411–441

    Google Scholar 

  • Matyasik I (1994) Geochemical exploration of the Menilite, Inoceramian and Spas beds of the Skole unit in Carpathian flysch. Nafta-Gaz 6:234–244 (in Polish with English abstract)

    Google Scholar 

  • Matyasik I, Dziadzio PS (2006) Reconstruction of petroleum systems based on integrated geochemical and geological investigations: Selected examples from the Middle Outer Carpathians in Poland. In: Golonka J, Picha FJ (eds) The Carpathians and their foreland: geology and hydrocarbon resources. AAPG Memoir, vol 84. The American Association of Petroleum Geologists, Tulsa, OK, pp 497–518

    Google Scholar 

  • Matyasik I, Kupisz L (1996) Geological and geochemical conditions of the hydrocarbon generation in the Menilite Beds from the south part of the Strzyżów Depression. The 2nd Conf. on the geochemical and petrophysical investigations in oil and gas exploration, Janowice, 10–12.04, pp 179–197

  • Matyasik I, Steczko A, Philp RP (2000) Biodegradation and migrational fractionation of oils from the Eastern Carpathians, Poland. Org Geochem 31:1509–1523

    Google Scholar 

  • Milkov AV (2011) Worldwide distribution and significance of secondary microbial methane formed during petroleum biodegradation in conventional reservoirs. Org Geochem 42:184–207

    Google Scholar 

  • Milkov AV (2018) Secondary microbial gas. In: Wilkes H (ed) Oils and lipids: diversity, origin, chemistry and fate, handbook of hydrocarbon and lipid microbiology. Springer, Berlin, pp 1–10

    Google Scholar 

  • Milkov AV, Etiope G (2018) Revised genetic diagrams for natural gases based on a global dataset of > 20,000 samples. Org Geochem 125:109–120

    Google Scholar 

  • Moldowan JM, Seifert WK, Gallegos EJ (1985) Relationship between petroleum composition and depositional environment of petroleum source rocks. AAPG Bull 69:1255–1268

    Google Scholar 

  • Moldowan JM, Sundararaman P, Schoell M (1986) Sensitivity of biomarker properties to depositional environment and or source input in the Lower Toarcian of southwest Germany. Org Geochem 10:915–926

    Google Scholar 

  • Orr WL (2001) Evaluating kerogen sulfur content from crude oil properties: cooperative Monterey organic geochemistry study. In: Isaacs CM, Rullkötter J (eds) The monterey formation: from rocks to molecules. Columbia University Press, New York, pp 348–367

    Google Scholar 

  • Palacas JG, Monopolis D, Nicolaou CA, Anders DE (1986) Geochemical correlation of surface and subsurface oils, western Greece. Org Geochem 10:417–423

    Google Scholar 

  • Pallasser RJ (2000) Recognising biodegradation in gas/oil accumulations through the δ13C compositions of gas components. Org Geochem 31:1363–1373

    Google Scholar 

  • Palmer S (1984) Effect of water washing on C15 + hydrocarbon fraction of crude oils from northwest Palawan, Philippines. AAPG Bull 68:137–149

    Google Scholar 

  • Palmer SE (1993) Effect of biodegradation and water washing on crude oil composition. In: Engel MH, Macko SA (eds) Organic geochemistry. Plenum Press, New York, pp 511–533

    Google Scholar 

  • Pan C, Yu L, Liu J, Fu J (2006) Chemical and carbon isotopic fractionations of gaseous hydrocarbons during abiogenic oxidation. Earth Planet Sci Lett 246:70–89

    Google Scholar 

  • Peters KE, Moldowan JM, Sundararaman P (1990) Effects of hydrous pyrolysis on biomarker thermal maturity parameters: monterey phosphatic and siliceous members. Org Geochem 15:249–265

    Google Scholar 

  • Peters KE, Moldowan JM, Mc Caffrey MA, Fago FJ (1996) Selective biodegradation of extended hopanes to 25-norhopanes in petroleum reservoirs. Insights from molecular mechanics. Org Geochem 24:765–783

    Google Scholar 

  • Peters KE, Walters CC, Moldowan JM (2005) The biomarker guide. In: Biomarkers and isotopes in petroleum exploration and earth history, vol 2. Cambridge University Press, New York

  • Pomykała Z (1982) Degradation of Carpathian oils. Nafta 38:135–139 (in Polish with English abstract)

    Google Scholar 

  • Rögl F (1999) Mediterranean and Paratethys. Facts and hypotheses of an Oligocene to Miocene paleogeography (short overview). Geol Carpath 50:339–349

    Google Scholar 

  • Sachsenhofer RF, Popov SV, Bechtel A, Coric S, Francu J, Gratzer R, Grunert P, Kotarba MJ, Mayer J, Pupp M, Rupprecht BJ, Vincent SJ (2018) Oligocene and Lower Miocene source rocks in the Paratethys: palaeogeographical and stratigraphic controls. In: Simmons MD, Tari GC, Okay AI (eds) Petroleum Geology of the Black Sea: Spec Publ Geol Soc 464:267–306

  • Sandulescu M (1988) Cenozoic tectonic history of the Carpathians. In: Royden L, Horvath F (eds) The Pannonian Basin: a study in basin evolution. AAPG Memoir, vol 45. The American Association of Petroleum Geologists, Tulsa, OK, pp 17–25

    Google Scholar 

  • Sechman H, Dzieniewicz M (2009) Analysis of results of surface geochemical surveys in the transfrontier zone of the Polish and Ukrainian Carpathians. Geologia AGH 35:109–127 (in Polish with English abstract)

    Google Scholar 

  • Seifert WK, Moldowan JM (1978) Applications of steranes, terpanes and monoaromatics to the maturation, migration and source of crude oils. Geochim Cosmochim Acta 42:77–95

    Google Scholar 

  • Seifert WK, Moldowan JM (1986) Use of biological markers in petroleum exploration. Meth Geochem Geoph 24:261–290

    Google Scholar 

  • Shanmugam G (1985) Significance of coniferous rain forests and related organic matter in generating commercial quantities of oil, Gippsland Basin, Australia. AAPG Bull 69:1241–1254

    Google Scholar 

  • Sinninghe Damsté JS, Kenig F, Koopmans MP, Köster J, Schouten S, Hayes JM, De Leeuw JW (1995) Evidence for gammacerane as an indicator of water column stratification. Geochim Cosmochim Acta 59:1895–1900

    Google Scholar 

  • Ślączka A, Kaminski MA (1998) A Guidebook to Excursions in the Polish Flysch Carpathians. Field Trips for Geoscientists. Grzybowski Foundation Spec Public 6:173

  • Ślączka A, Kruglow S, Golonka J, Oszczypko N, Popadyuk I (2006) The general geology of the Outer Carpathians, Poland, Slovakia, and Ukraine. In: Golonka J, Picha FJ (eds) The Carpathians and their foreland: geology and hydrocarbon resources. AAPG Memoir, vol 84. The American Association of Petroleum Geologists, Tulsa, OK, pp 221–258

    Google Scholar 

  • Ślączka A, Golonka J, Oszczypko N, Cieszkowski M, Słomka T, Matyasik I (2014) Occurrence of Upper Jurassic–Lower Cretaceous black organic-rich pelitic sediments as targets for unconventional hydrocarbon exploration in the Outer Carpathians and adjacent part of the Alps. AAPG Bull 98:1967–1994

    Google Scholar 

  • Sofer Z (1984) Stable carbon isotope compositions of crude oils: application to source depositional environments and petroleum alteration. AAPG Bull 68:31–49

    Google Scholar 

  • Stahl WJ (1980) Compositional changes and 13C/12C fractionations during the degradation of hydrocarbons by bacteria. Geochim Cosmochim Acta 44:1903–1907

    Google Scholar 

  • Steczko A, Słoczyński T (2007) Reservoir geochemistry as a tool to estimation factors and processes which caused changes in hydrocarbons composition of oils. Nafta-Gaz 63:243–252 (in Polish with English abstract)

    Google Scholar 

  • Sun Y, Chen Z, Xu S, Cai P (2005) Stable carbon and hydrogen isotopic fractionation of individual n-alkanes accompanying biodegradation: evidence from a group of progressively biodegraded oils. Org Geochem 36:225–238

    Google Scholar 

  • Sweeney RE, Taylor P (1999) Biogenic methane derived from biodegradation of petroleum under environmental conditions and in oil and gas reservoirs. In: Schoell M, Claypool J (eds) Proceedings of the AAPG Hedberg Research Conference, 6–10 June, 1999

  • Tao S, Wang Ch, Du J, Liu L, Chen Z (2015) Geochemical application of tricyclic and tetracyclic terpanes biomarkers in crude oils of NW China. Mar Petrol Geol 67:460–467

    Google Scholar 

  • Tao K, Liu X, Chen X, Hu X, Cao L, Yuan X (2017) Biodegradation of crude oil by a defined co-culture of indigenous bacterial consortium and exogenous Bacillus subtilis. Bioresour Technol 224:327–332

    Google Scholar 

  • ten Haven HL, Lafargue E, Kotarba M (1993) Oil/oil and oil/source rock correlations in the Carpathian Foredeep and Overthrust, south-east Poland. Org Geochem 20:935–959

    Google Scholar 

  • Thompson KFM (1983) Classification and thermal history of petroleum based on light hydrocarbons. Geochim Cosmochim Acta 47:303–316

    Google Scholar 

  • Thompson KFM (1987) Fractionated aromatic petroleum and the generation of gas-condensates. Org Geochem 11:573–590

    Google Scholar 

  • Thompson KFM (2010) Aspects of petroleum basin evolution due to gas advection and evaporative fractionation. Org Geochem 41:370–385

    Google Scholar 

  • Townsend GT, Prince RC, Suflita JM (2003) Anaerobic oxidation of crude oil hydrocarbons by the resident microorganisms of a contaminated anoxic aquifer. Environ Sci Technol 37:5213–5218

    Google Scholar 

  • Vandré C, Cramer B, Gerling P, Winsemann J (2007) Natural gas formation in the western Nile delta (Eastern Mediterranean): Thermogenic versus microbial. Org Geochem 38:523–539

    Google Scholar 

  • Venosa AD, Zhu X (2003) Biodegradation of crude oil contaminating marine shorelines and freshwater wetlands. Spill Sci Technol Bull 8:163–178

    Google Scholar 

  • Wang WC, Zhang LY, Liu WH, Kang Y, Ren JH (2005) Effects of biodegradation on the carbon isotopic composition of natural gas—a case study in the Bamianhe oil field of the Jiyang Depression, Eastern China. Geochem J 39:301–309

    Google Scholar 

  • Welhan JA (1988) Origins of methane in hydrothermal systems. Chem Geol 71:183–198

    Google Scholar 

  • Wenger LM, Davis CL, Isaksen GH (2002) Multiple controls on petroleum biodegradation and impact on oil quality. SPE Reserv Eval Eng 5:375–383

    Google Scholar 

  • Whiticar MJ (1994) Correlation of natural gases with their sources. In: Magoon LB, Dow WG (eds) The petroleum system—from source to trap. AAPG Memoir, vol 60. The American Association of Petroleum Geologists, Tulsa, OK, pp 261–283

    Google Scholar 

  • Więcław D (2002) Origin of Oligocene oils from the Polish Flysch Carpathians: organic sulphur in the kerogen of the Menilite Shales and kinetics of hydrocarbon generation process: Ph.D. thesis, AGH University of Science and Technology, Kraków, p 131 (in Polish)

  • Więcław D (2011) Origin of liquid hydrocarbons accumulated in the Miocene strata of the Polish Carpathian Foredeep and its Paleozoic–Mesozoic basement. Ann Soc Geol Pol 81:443–458

    Google Scholar 

  • Więcław D, Kotarba MJ, Kuśmierek J, Kowalski A, Machowski G (2008) Perpendicular changeability of source-rock indices of the Menilite Beds in selected profiles of the eastern part of Polish Outer Carpathians. Prace Instytutu Nafty i Gazu 150:455–460 (in Polish with English abstract)

    Google Scholar 

  • Więcław D, Kotarba MJ, Kowalski A (2010) Origin of oils accumulated in the Middle Cambrian reservoirs of the Polish part of the Baltic region. Geol Q 54:205–216

    Google Scholar 

  • Więcław D, Kotarba MJ, Kowalski A, Koltun YV (2012) Origin and maturity of oils in the Ukrainian Carpathians and their Mesozoic basement. Geol Q 56:153–168

    Google Scholar 

  • Wilhelms A, Larter SR, Head I, Farrimond P, di-Primio R, Zwach C (2001) Biodegradation of oil in uplifted basins prevented by deep-burial sterilization. Nature 411(6841):1034–1037

    Google Scholar 

  • Wingert WS (1992) G.c.-m.s. analysis of diamondoid hydrocarbons in Smackover petroleums. Fuel 71:37–43

    Google Scholar 

  • Wróbel M, Kosakowski P, Więcław D (2016) Petroleum processes in the Palaeozoic–Mesozoic strata of the Grobla–Limanowa area (basement of the Polish Carpathians). Geol Geophys Environ 42:185–206

    Google Scholar 

  • Wu Y, Zhai L, Xu S, Han Z, Yuan X, Wu J, Wu Z (2017) Biodegradation characteristics of heavy oil and correlation with group composition and carbon isotopes. Petrol Sci Technol 35:190–195

    Google Scholar 

Download references

Acknowledgements

The research has been financially supported by the National Science Centre grant No. UMO-2014/15/B/ST10/00131 (18.18.140.666/N84). Two anonymous reviewers provided very constructive reviews, which greatly improved the discussion and hypotheses presented in the manuscript. Analytical and editorial works by Joanna Gawęda-Skrok, Hieronim Zych and Tomasz Kowalski from the AGH University of Science and Technology are kindly acknowledged. We are also very grateful to Marek Pietrusiak from the Polish Petroleum Company in Sanok for his help in collecting of geological and reservoir data.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Dariusz Więcław.

Additional information

Paul G. Lillis is now retired.

Appendix: Description of the oil and gas fields and seeps in the study area

Appendix: Description of the oil and gas fields and seeps in the study area

Silesian nappe—oil and gas field

In the Silesian nappe in the analysed area 13 petroleum accumulations were discovered: Wetlina, Rudawka Rymanowska, Mokre, Dwernik, Zatwarnica, Rajskie, Tarnawa–Wielopole, Czarna, Strachocina, Grabownica, Sanok–Zabłotce, Jurowce–Srogów and Turze Pole–Zmiennica (Karnkowski and Ozimkowski 1998; Karnkowski 1999).

The Wetlina gas field (discovered in 1965, abandoned in 2001) is a small (70 Mm3), field comprising accumulations in an imbricated fan complex of Krosno beds and sandstone intercalations within the Menilite beds on average depth ca. 2320 m. The trap is associated with a thrust fault, which is subdivided by transverse faults into several blocks. This field is located on the boundary of the Dukla and Silesian nappes on the most southern part of the study area (Figs. 1, 5).

The Rudawka Rymanowska oil field (discovered in 1889, abandoned in 2005) is located in the most SW part of the study area (Figs. 1, 4). The fold, where the deposit is located, is strongly sliced and overturned. The deposit occurs within horizons of Krosno beds at a depth of 200–800 m and Ciężkowice Sandstone at a depth of 45–500 m. In both reservoirs the trap is lithologically sealed by shales. Since the beginning of exploitation from the Krosno beds and Ciężkowice Sandstone ca. 6 thousand tons of oil and ca. 0.4 Mm3 of gas and ca. 4.4 Mm3of gas, respectively have been obtained.

The Mokre oil field (discovered in 1913, abandoned in 2005) is represented by Stefan-41 well (St-41) (Fig. 1). Oil is accumulated in Lower Krosno beds at two levels (60–1100 and 1200–2000 m). The field has produced over 86.5 Kt of oil and over 10 Mm3of associated gas. Hydrocarbons are accumulated in NW–SE oriented asymmetric duplex-type anticlinal structure cut by the SW–NE oriented transverse dislocations into several separated blocks which constitute the individual fracture type of reservoirs (Karnkowski 1999).

The Dwernik oil field (discovered in 1984, abandoned in 2001) and Zatwarnica oil field (discovered in 1962, in production) are connected to the same WNW-ESE oriented small anticline. Dwernik and Zatwarnica oil fields are located in central and in the western parts of this structure, respectively (Figs. 1, 5). The reservoirs occur at depths between 500 and 1000 m and 250 and 1135 m, respectively (Fig. 5). The reservoir for both of oil fields is Lower Krosno beds. Total production from Zatwarnica and Dwernik gas-driven deposits is ca 8 Kt of oil and ca. 2.6 Mm3and 3.8 Kt of oil and 0.3 Mm3 of associated gas, respectively.

Rajskie oil field (discovered in 1880, abandoned in 1999) was sampled in Rj-7 well (Fig. 1). The trap is associated with an asymmetric anticline with a gently dipping SE limb and a steep NE one. The reservoirs are Krosno beds. In total, three horizons were distinguished which can be correlated long distances along the strike of the anticline. Five other horizons are of local extent. The depths of the horizons vary from 150 to 475 m. The trap is of both structural and stratigraphic type (Karnkowski 1999). Total production from the field is 27.3 Kt of oil and 8.9 Mm3 of associated gas.

The Tarnawa–Wielopole oil field (discovered in 1900, abandoned in 2002) (sampled in TW-25 and TW-32 wells; Fig. 1) is accumulated in Lower and Middle Krosno beds, traced a long distance along WNW-ESE oriented asymmetrical fold. Additionally, the anticline is cut by transverse faults. Gas-driven oil production was obtained from three fractured horizons: 680 m, 765 m and 1225 m. Total production from the field is 286.8 Kt of oil and 43.6 Mm3 of associated gas.

The Czarna oil field (discovered in 1936) is still in production (Figs. 1, 5). The field is present in an asymmetrical anticlinal structure that is strongly disturbed tectonically. The deposit is accumulated in multiple horizons within Krosno Beds and is sealed lithologically and in part tectonically. The most productive reservoirs are zones adjacent to the faults, particularly the longitudinal ones. Eleven producing horizons are distinguished at depths from 130 to 1170 m. Total production from the field is: 263.2 Kt of oil and 21.3 Mm3 of associated gas.

Sanok–Zabłotce (discovered in 1951, in production), Jurowce–Srogów (discovered in 1921, in production) and Strachocina (discovered in 1928, gas storage from 2011) gas fields are located in a long anticlinal structure (Fig. 1). Sanok–Zabłotce is the smallest field with cumulative production ca. 860 Mm3 from an average depth ca. 950 m (Fig. 4) and is located in eastern part of the fold. To the west the Jurowce–Srogów gas field is located with total production to date of 6.6 Mm3 of gas. The Strachocina gas field is the biggest gas field in the Polish Outer Carpathians and has produced more than 4.5 Bcm of gas from average depth of 935 m (Fig. 3). The Sanok–Zabłotce, Jurowce–Srogów and Strachocina structures form a normal anticline in the Istebna beds (Figs. 3, 4). The main producing horizons are within the Istebna sandstone that is sealed by the Istebna shales (Table 1).

The Turze Pole–Zmiennica (discovered in 1883, in production) oil field is located in the western part of the above described structure (Figs. 1, 3). The total production of oil to date is ca. 267.8 Kt and over 63 Mm3 of gas and over 4.5 Kt of light oil. Oil is accumulated in sandstones of the Lgota, Istebna, Ciężkowice and Hieroglyphic beds. The traps are stratigraphic in Ciężkowice and Hieroglyphic sandstones or tectono-stratigraphic (in Lgota and Istebna sandstones) and hosted in a strongly folded and tilted to SW anticlinal structure. Hydrocarbons are accumulated at the depth of 100–860 m.

In the most northwestern part of the Silesian nappe, the Grabownica oil field (Figs. 1, 3) was discovered in 1898 (still in production). Reservoir rocks are Lower Cretaceous (Lgota beds and Grodziszcze Sandstone). The trap is located in a steep symmetrical anticline cut by NW–SE oriented faults into several blocks. In the axial part of the anticline a lower order steep fault is present, which additionally divides the anticline on two longitudinal blocks: southern and northern. Oil is accumulated in five horizons at an average depth of 730 m with total production to date of over 1 Mt and over 375.4 Mm3 of associated gas.

Skole nappe—oil and gas field

In the Skole nappe in the analysed area, five petroleum accumulations were discovered: Tyrawa Solna, Leszczowate–Wańkowa–Paszowa, Łodyna, Brzegi Dolne and Słonne.

The Tyrawa Solna oil field (discovered in 1900, abandoned in 2003) is a small deposit discovered in Kliwa Sandstone enclosed in Menilite beds (Figs. 1, 3). Since the beginning of exploitation ca. 54 Kt of oil and over 11 Mm3 of gas has been obtained from average depth 230 m. Hydrocarbons are accumulated in a sliced and overturned limb of an anticlinal structure in a lithological trap.

Leszczowate–Wańkowa–Paszowa, Łodyna and Brzegi Dolne oil fields were discovered in 1885, 1880 and 1881, respectively. These three oil fields are located in the southeastern part of the Skole nappe (Figs. 1, 6, 7). Total production from Leszczowate–Wańkowa–Paszowa oil field is ca. 1.446 Mt of oil and over 142 Mm3 of gas; in Łodyna oil field is ca. 307.5 Kt of oil and ca. 42 Mm3 of gas; in Brzegi Dolne oil field is ca. 13.5 Kt of oil and ca. 0.14 Mm3 of gas. All of these fields have a very complex, structural and stratigraphic trap type (Figs. 6, 7). Oil and associated gas accumulations occur in all of the deposits in the southern limb of the structure, in several pinch-out traps of the Kliwa Sandstone, which shows in many cases flexural narrowing [the result of backthrust faulting(?)] and tilting to the southwest. The average depth of hydrocarbons accumulation is 500 m (Dziadzio et al. 2006).

Słonne oil field is the smallest and most northeast-located oil field in the Skole nappe (Fig. 1); it was discovered in 1951 and abandoned in 1961. Oil is accumulated in the Upper Cretaceous Inoceramian beds (Fig. 3). The trap is connected to anticline cut in central part by small thrust fault. Total production was ca. 0.5 Kt of oil from the depth of 50–220 m.

Sampled oil and gas seeps

In the Polish (also in Ukrainian) Outer Carpathians oil and gas seeps are a common phenomenon (e.g. Kuśmierek and Machowski 2008; Kotarba et al. 2009a). They are the result of natural petroleum outflows from shallow deposits through fissures (mostly gas, Sechman and Dzieniewicz 2009), but mostly are a remnant of the improperly abandoned wells (Kotarba et al. 2009b).

Five oil seeps from the study area have been collected and analysed (Fig. 1), those are: Łopienka (reservoir: Krosno beds—old abandoned well); Zmiennica (reservoir: Ciężkowice Ss.—connected to the oil field); Płowce (reservoir: Krosno beds—old abandoned well); Żłobek (reservoir: Krosno beds—old abandoned dug well) belonging to the Silesian nappe and Wara (reservoir: Inoceramian Beds—an old abandoned well). Geochemical data of oil collected from a seep in Bandrów (reservoir: Kliwa Ss.—old abandoned dug well) belonging to the Skole nappe presented by Curtis et al. (2004) were used for discussion.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Więcław, D., Bilkiewicz, E., Kotarba, M.J. et al. Origin and secondary processes in petroleum in the eastern part of the Polish Outer Carpathians. Int J Earth Sci (Geol Rundsch) 109, 63–99 (2020). https://doi.org/10.1007/s00531-019-01790-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s00531-019-01790-y

Keywords

Navigation