Marine incursion events in the Late Cretaceous Songliao Basin: Constraints from sulfur geochemistry records

https://doi.org/10.1016/j.palaeo.2013.03.017Get rights and content

Highlights

  • The paper proved saline water conditions for the deposition of K2qn1.

  • Sulfur geochemical data shows contribution of marine incursion to such condition.

  • The marine incursion may have begun earlier than ever suggested.

Abstract

Songliao Basin in NE China developed the most productive oilfield in the world sourced from terrestrial rocks. The main source rock of the basin includes member 1 of the Qingshankou (K2qn1) and members 1 and 2 of the Nenjiang Formation (K2nj1–2). However the exact reasons for the formation of the source rock, especially the K2qn1 are still controversial. Former paleontological and organic geochemical research suggested that organic matter was deposited during marine incursion events of K2qn1 but further geochemical evidence is needed. This paper explores the distinct sulfate levels that distinguish marine from fresh waters of the Songliao paleo-lake. We undertook a systematic investigation the sulfur geochemistry of the sediments from top of member 4 of the Quantou Formation (K1q4) to top of member 1 of the Qingshankou (K2qn1). The ratio of organic carbon to the pyrite sulfur (TOC/PYS) proved the previously suggested saline conditions during the deposition of K2qn1; and the pyrite sulfur isotope indicated that marine incursion may not only have occurred for K2qn1, but also for top of K1q4. The exact time for the beginning of marine incursion is to be determined. The marine incursion within K2qn1 is not strong and partially controlled by the fluctuation of paleo-lake level. The present study will be helpful for understanding the contribution of marine incursion events to the burial of organic carbon in the Songliao paleo-lake, although further studies are still needed.

Introduction

As one of the largest late Mesozoic–Cenozoic continental sedimentary basins in East Asia, the Songliao Basin in NE China developed an almost complete Cretaceous succession (Chen, 1987, Chen, 2003). During the Cretaceous, the basin was a large rift basin that hosted a long-lived deep lake (Chen, 1987). This history enabled the basin to become the largest oil and gas producing basin in China, with China's largest oilfield, Daqing, being situated in the central part of the basin (Zhou and Littke, 1999).

Most of the source rocks in the Daqing oil field are terrestrial deposits; this may be the most productive oilfield in the world sourced from terrestrial rocks (Yang et al., 1985). However the exact reason for the formation of the mass hydrocarbon source rock, including the member 1 of Qingshankou and member 1 and 2 of Nenjiang Formation deposited in the Songliao Basin, is still unknown (Li and Pang, 2004). Prior studies of the formation of source rock in the Songliao Basin have found that the hydrocarbon source rock of Songliao was deposited under brackish-saline conditions (Hou et al., 2000 and references therein), despite the fact that the Songliao paleo-lake was mainly a freshwater lake during most of its life cycle. Paleontological and organic geochemical evidences suggested that salinity conditions may be due to an influx of seawater during a brief marine connection and lake transgression (Huang et al., 1999, Hou et al., 2000). For example the identification of marine dinophyceae, planktonic foraminifera, shark teeth, and biomarkers such as C30 4-desmethylsteranes in these strata would suggest conditions with a strong marine influence (Zhang and Zhou, 1976, Zhang et al., 1977, Gao et al., 1994a, Gao et al., 1994b, Huang et al., 1998, Gao and Zhao, 1999, Hou et al., 2000, Huang, 2007), however controversy questions the validity of these evidences (Ye and Zhong, 1990, Huang and Huang, 1998, Huang et al., 1999, Li et al., 2000, Ye et al., 2002). New evidences of the marine incursion events are still needed.

Different levels of sulfate distinguish fresh from marine water (~ 10 to hundreds of μM vs. 28 mM). The sulfate concentration of lake water would have increased and the geochemical behavior of sulfur changed if the lake was connected with the open ocean (Holmer and Storkholm, 2001). This effect is best illustrated by the modern Black Sea, which was formerly a fresh-water lake but was connected with the Mediterranean not long ago; sulfidic conditions prevail in the present water column (Yücel et al., 2010 and reference therein). A complete investigation of sulfur geochemistry of the sediments, i.e., the species and isotope ratio would be of help to understand the details of the sulfur cycle in an aquatic system (Holmer and Storkholm, 2001), and thus revealing the potential marine incursion events of this lake. Previous data have shown that the reduced sulfur was relatively enriched in member 1 of the Qingshankou and members 1 and 2 of the Nenjiang Formation deposited in the Songliao Basin, which makes such investigation possible (Huang, 2007). This work concentrates on the isotopic geochemistry of sulfur to elucidate if marine incursion events actually occurred during the deposition of member 1 of the Qingshankou Formation. The present study will also be of value in answering the long-debated question of whether the marine incursion really contributed to the organic carbon accumulation in the Songliao paleo-lake, because the sulfur cycle regulates the redox condition, nutrient status and affects the productivity of both the lake (Fleet et al., 1988, Caroca et al., 1993, Cohen, 2003) and marine systems (Adams et al., 2010).

Section snippets

Geological setting

The Songliao Basin is an intra-cratonic Cretaceous rift basin, as demonstrated by an abundance of data generated by the petroleum industry regarding its subsidence and geothermal histories, sedimentary facies, crustal underpinnings, and structural style (Song, 1997, Einsele, 2000). The evolution of the Songliao Basin consists of five stages: 1) a pre-late Jurassic pre-rift doming, 2) the latest Jurassic extensional fracturing, 3) the earliest Cretaceous full graben, 4) late Early to

Material and methods

The SK-1 drilling program, supported by the Ministry of Science and Technology of China (MOST) and the Daqing Oilfield, was initiated and conducted to recover complete cores from the upper Quantou to Taikang Formations in the Songliao Basin (Fig. 1a, b). A “one well-two holes” plan was implemented from August 18, 2006 to October 20, 2007 according to the site selection strategy (Huang, 2007). The northern hole, SK-1(N), recovered 1541.66 m of continuous core from Knj1 through the Yi'an Formation

Results

The analytical results of the TOC, pyrite sulfur and sulfur isotope are presented in Table 1. In member 4 of the Quantou Formation, the average content of pyrite sulfur is 0.55% with a range from 0.003 to 0.96%, and the sulfur isotope ratio (δ34S) varies from 17.29 to 21.51‰ and has an average of 19.47‰. In member 1 of the Qingshankou Formation, the pyrite sulfur is at the level from 0.03 to 1.74% with the average of 0.59%; and the sulfur isotope ratio (δ34S) ranges from 14.4 to 24.06% with an

Variation of the total organic carbon to pyrite sulfur ratios in member 4 of the Quantou Formation and member 1 of the Qingshankou Formation

Previous paleontological and organic geochemical evidences suggested that, although the paleo-Songliao lakes primarily hosted fresh waters during most of its lifetime, member 1 of the Qingshankou Formation was deposited under (semi-)saline conditions (Zhang and Zhou, 1976, Zhang et al., 1977, Gao et al., 1994a, Gao et al., 1994b, Huang et al., 1998, Gao and Zhao, 1999, Hou et al., 2000, Huang, 2007). This finding could also be further tested by the variation of total organic carbon to pyrite

Conclusion

Previous evidences from paleontological and organic geochemical research proposed that marine incursion events occurred during deposition of K2qn1 but this finding remains strongly contested and has led to extended debate without a definitive answer since the discovery of Daqing oilfield. One of the reasons for this uncertainty is the inadequacy of the former evidences in elucidating the detailed processes that occurred during the marine incursion events. Based on the distinct levels of sulfate

Acknowledgments

This study was jointly supported by National Key Basic Research Program of China Grant (No. 2012CB822005) and Natural Science Foundation of China (No. 40873022). We thank the staff of Stable Isotope Lab, the State Key Laboratory of Lithospheric Evolution situated in the Institute of Geology and Geophysics, Chinese Academy of Sciences, for their advice and assistance during stable isotope analysis. We also thank Prof. Xuelei Chu and Dr. Michael Formolo for their helpful discussions during the

References (79)

  • J.L. McKay et al.

    Sulphur isotope geochemistry of pyrite from the Upper Cretaceous Marshybank Formation, Western Interior Basin

    Sedimentary Geology

    (2003)
  • J.W. Morse et al.

    What determines sedimentary C/S ration

    Geochimica et Cosmochimica Acta

    (1995)
  • F.W. Nara et al.

    Climate control of sulfate influx to Lake Hovsgol, northwest Mongolia, during the last glacial—postglacial transition: constraints from sulfur geochemistry

    Palaeogeography, Palaeoclimatology, Palaeoecology

    (2010)
  • C.E. Rees

    A steady-state model for sulphur isotope fractio-nation in bacterial reduction processes

    Geochimica et Cosmochimica Acta

    (1973)
  • M. Rudnicki et al.

    Fractionation of sulfur isotopes during bacterial sulfate reduction in deep ocean sediments at elevated temperatures

    Geochimica et Cosmochimica Acta

    (2001)
  • J.H. Ryu et al.

    Sulfur biogeochemistry and isotopic fractionation in shallow groundwater and sediments of Owens Dry Lake, California

    Chemical Geology

    (2006)
  • S.J. Schenau et al.

    Sedimentary pyrite formation in the Arabian Sea

    Marine Geology

    (2002)
  • J.G. Sha et al.

    Late Mesozoic transgressions of eastern Heilongjiang and their significance in tectonics, and coal and oil accumulation in northeast China

    Palaeogeography, Palaeoclimatology, Palaeoecology

    (2008)
  • T.G. Song

    Inversion styles in Songliao Basin (northeast china) and estimation of the degree of inversion

    Tectonophysics

    (1997)
  • M.L. Tuttle et al.

    Sedimentary sulfur geochemistry of the Paleogene Green River Formation, western USA: implications for interpreting depositional and diagenetic processes in saline alkaline lakes

    Geochimica et Cosmochimica Acta

    (1993)
  • X.Q. Wan et al.

    Late Cretaceous stratigraphy, Songliao Basin, NE China: SK1 cores, Palaeogeography, Palaeoclimatology

    Palaeoecology

    (2013)
  • P.K. Wang et al.

    Pyrite morphology in the first member of the Late Cretaceous Qingshankou Formation, Songliao Basin, Northeast China

    Palaeogeography, Palaeoclimatology, Palaeoecology

    (2013)
  • T. Watanabe et al.

    Biological and environmental changes in Lake Baikal during the late Quaternary inferred from carbon, nitrogen and sulfur isotopes

    Earth and Planetary Science Letters

    (2004)
  • R.T. Wilkin et al.

    Variations in pyrite texture, sulfur isotope composition, and iron systematics in the Black Sea: evidence for Late Pleistocene to Holocene excursions of the O2–H2S redox transition

    Geochimica et Cosmochimica Acta

    (2001)
  • R.T. Wilkin et al.

    Pyrite formation by reactions of iron monosulfides with dissolved inorganic and organic sulfur species

    Geochimica et Cosmochimica Acta

    (1996)
  • R.T. Wilkin et al.

    Formation processes of framboidal pyrite

    Geochimica et Cosmochimica Acta

    (1997)
  • R.T. Wilkin et al.

    The size distribution of framboidal pyrite in modern sediments: an indicator of redox conditions

    Geochimica et Cosmochimica Acta

    (1996)
  • R.T. Wilkin et al.

    History of water-column anoxia in the Black Sea indicated by pyrite framboid size distributions

    Earth and Planetary Science Letters

    (1997)
  • M. Yücel et al.

    Sulfur speciation in the upper Black Sea sediments

    Chemical Geology

    (2010)
  • Y.S. Zhou et al.

    Numerical simulation of the thermal maturation, oil generation and migration in the Songliao Basin, Northeastern China

    Marine and Petroleum Geology

    (1999)
  • D.D. Adams et al.

    Volcanic triggering of a biogeochemical cascade during Oceanic Anoxic Event 2

    Nature Geoscience

    (2010)
  • A. Bein et al.

    Sulphur diagenesis in freshwater lignites (Hula Basin, Israel): implication for S–C relationships in organic sediments

    Journal of the Geological Society of London

    (1988)
  • R.A. Berner et al.

    C/S method for distinguishing freshwater from marine sedimentary rocks

    Geology

    (1984)
  • J. Bloch et al.

    Sulfide diagenesis and sedimentation in the Albian Harmon Member, Western Canada

    Journal of Sedimentary Petrology

    (1992)
  • D.E. Canfield

    Biogeochemistry of sulfur isotopes

    Reviews in Mineralogy and Geochemistry

    (2001)
  • D.E. Canfield et al.

    Late Proterozoic rise in atmospheric oxygen concentration inferred from phylogenetic and sulphur-isotope studies

    Nature

    (1996)
  • D.E. Canfield et al.

    The production of 34S-depleted sulfide during bacterial disproportionation of elemental sulfur

    Science

    (1994)
  • D.E. Canfield et al.

    High isotope fractionations during sulfate reduction in a low-sulfate euxinic ocean analog

    Geology

    (2010)
  • N.F. Caroca et al.

    Sulfate control of phosphorus availability in lakes

    Hydrobiologia

    (1993)
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