Probable fungal origin of perylene in Late Cretaceous to Paleogene terrestrial sedimentary rocks of northeastern Japan as indicated from stable carbon isotopes
Introduction
Perylene is a typical polyaromatic hydrocarbon (PAH) that occurs in many sediments. Although numerous studies have sought to clarify its origin, both its precursors and formation mechanism remain uncertain. Previous investigations have agreed that it can be formed from combustion of OM and fossil fuels in a similar manner to other PAHs. However, unlike anthropogenic PAHs, it generally increases in abundance with depth (Orr and Grady, 1967, Aizenshtat, 1973, Ishiwatari et al., 1980, Wakeham et al., 1980, Gschwend et al., 1983, Silliman et al., 1998, Silliman et al., 2000, Grice et al., 2009), leading researchers to infer that it forms within the rock mass. This conclusion has, in turn, led to the proposition that it forms through diagenetic alteration of natural precursors under anaerobic conditions (Aizenshtat, 1973, Orr and Grady, 1967, Hites et al., 1977, Garrigues et al., 1988, Silliman et al., 1998). Possible precursors include perylene quinones derived from black pigments in plants (Thomson, 1976), insects (Cameron et al., 1964), fungi (Hardil et al., 1989, Hashimoto et al., 1994) and crinoids (De Riccardis et al., 1991). Although such precursors are largely terrestrial in origin, it is still not apparent whether perylene is generated in terrestrial or aquatic environments.
There are numerous reports of the existence of perylene in terrestrial sediments (Taguchi et al., 1970, Aizenshtat, 1973, Ishiwatari et al., 1980, Hites et al., 1980, White and Lee, 1980, Garrigues et al., 1988, Jiang et al., 2000, Grice et al., 2009), but it has also been found in marine sediments (Orr and Grady, 1967, Aizenshtat, 1973, Wakeham et al., 1979, Hites et al., 1980, Louda and Baker, 1984, Venkatesan, 1988). In the latter cases, diatoms have been proposed as the source (Hites et al., 1980, Venkatesan, 1988), despite an absence of data showing the presence of perylene-related compounds in diatoms.
In this paper we report the distribution and stable carbon isotope ratio (δ13C) of perylene in terrestrial sediments of varying lithology and depositional environments in the MITI Sanriku-oki borehole of northeastern Japan. Our objective was to ascertain if natural precursors of perylene could be identified.
Section snippets
Samples and geological setting
The MITI Sanriku-oki borehole is on the Pacific side of northeastern Japan (40°40′N,142°17′E) in a water depth of 857 m (Fig. 1), close to Leg 57, Sites 438 and 439 of the Deep Sea Drilling Project (DSDP; DSDP Scientific Party, 1980). It penetrates 3.64 km of Late Cretaceous to Early Miocene sediments to a depth of 4500 m below sea level (mbsl). Downhole petrophysical log data, along with the results of seismic profiling have been summarized by the Japan National Oil Corporation (JNOC, 2000) and
Occurrence of perylene in Late Cretaceous to Paleogene sedimentary rocks
Analysis of the aromatic fraction of samples from the MITI Sanriku-oki borehole shows the presence of perylene in sediments of Late Cretaceous to mid-Eocene age from Units A–C. It occurs in all of them in much greater abundance than PAHs formed by combustion, such as pyrene, benzo[a]anthracenes, benzofluoranthenes, benzopyrenes and phenanthrenes (Fig. 2 and Table 1).
The Late Cretaceous to Paleogene sediments were deposited in shallow-terrestrial and marine environments. Continental environments
Conclusions
Perylene occurs in sediments from the MITI Sanriku-oki borehole and increases in concentration with depth among the intervals deposited in reducing environments and rich in terrestrial OM. This is consistent with previous suggestions that it is a diagenetic product of terrestrial OM, with anoxic conditions favoring its formation and/or preservation. Examination of the carbon isotope ratios of perylene and associated gymnosperm and angiosperm biomarkers shows perylene to be enriched in 13C
Acknowledgements
We thank the Japan Oil, Gas and Metals National Corporation (JOGMEC) for providing samples and for permission to publish. Thanks are also due to D. Dawson and an anonymous reviewer for comments which improved the manuscript. The research was partially supported by a Grant-in-Aid for Scientific Research (No. 18204045) from the Ministry of Education, Culture, Sports, Science and Technology of Japan.
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