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Aromatic Hydrocarbons from the Middle Jurassic Fossil Wood of the Polish Jura

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Aromatic Hydrocarbons from the Middle Jurassic Fossil Wood of the Polish Jura 82 Contemporary Trends in Geoscience vol . 2 DOI: 10.2478/ctg-2014-0012 Justyna Smolarek1, Leszek Marynowski1 Aromatic hydrocarbons from the Middle Jurassic 1Faculty of Earth Sciences, University of Silesia, fossil wood of the Polish Jura Bedzinska 60, 41-200 Sosnowiec. E-mail: [email protected], [email protected] Key words: Abstract fossil wood, Middle Jurassic, organic Aromatic hydrocarbons are present in the for the majority of the samples are in the matter, biomarkers, aromatic fossil wood samples in relatively small range of 0.1 to 0.5, which results in the high- hydrocarbons, GC-MS amounts. In almost all of the tested sam- ly variable values of Rc (converted value of ples the dominating aromatic hydrocarbon vitrinite reflectance) ranging from 0.45 to is perylene and its methyl and dimethyl de- 0.70%. Such values suggest that MPI1 param- rivatives. The most important biomarkers eter is not useful as maturity parameter in present in the aromatic fraction are dehy- case of Middle Jurassic ore-bearing clays, droabietane, siomonellite and retene, com- even if measured strictly on terrestrial or- pounds characteristic for conifers. The dis- ganic matter (OM). As a result of weather- tribution of discussed compounds is highly ing processes (oxidation) the distribution of variable due to such early diagenetic pro- aromatic hydrocarbons changes. In the ox- cesses affecting the wood as oxidation and idized samples the amount of aromatic hy- the activity of microorganisms. MPI1 pa- drocarbons, both polycyclic as well as aro- rameter values (methylphenanthrene index) matic biomarkers decreases. Contemporary trends in Geoscience vol . 2 83 Introduction Polycyclic aromatic hydrocarbons (PAHs) in the sediment may be caused by micro- are generated in sedimentary rocks by the bial activity in the early stages of diagen- complex natural processes including aroma- esis and subsequent transformation dur- tization of the steroids, tricyclic diterpenoids ing thermal processes, with the additional or pentacyclic triterpentenoids (e.g. Radke, influence of pressure and mineral matrix 1987). They may also formed as a result of as a catalyst (Radke, 1987). Structural re- bacteria activity (Wakeham et al., 1980) and lationship between the natural precursors due to the influence of temperature on OM and aromatic hydrocarbons derived from in the presence of sulfur and/or clay min- sedimentary organic matter is not always erals (Eglinon, Murphy, 1969). Tissot et al. clear. Natural products during diagenetic (1971) and Radke (1987) found that a small processes may, in some cases, significantly percentage of aromatic hydrocarbons gen- change the structure of the precursors lead- erated from kerogen is formed from natu- ing to alkylation (substitution of hydrogen ral precursors without significant structur- an alkyl radical), dealkylation (cleavage of al changes. According to the fact that the the hydrocarbon-containing side chain), organisms do not biosynthesize aromatic isomerization or disruption of alicyclic sys- structures in large quantities, the presence tems (Radke, 1987). Here we are presenting of PAHs in crude oil and sediments should the composition of aromatic hydrocarbons be the result of complex chemical transfor- found in the immature fossil wood from mation of natural products, characterized the Middle Jurassic ore-bearing sediments, by naphthenic or olefinic structure (Hase, showing source, distribution and diagenet- Hites, 1976). This transformation runing ic transformations of PAHs. Materials Samples of the Middle Jurassic fossil wood (Gut – Kałamaga 2000). were taken from the ore-bearing clays of Due to the degree of mineralization wood the Polish Jura area. Eighteen fossil wood can be divided into: pieces were sampled from the active clay • non-mineralized wood fragments (xylite pits which are located in Czestochowa re- type) and gelified wood (jet type), gion: Gnaszyn Wienerberger, Sowa, Anna • wood fragments partly mineralized, and near to that city between Grodzisko and • wood fragments completely mineralized. Wreczyca Wielka (Grodzisko). Due to the degree of oxidation the follow- Middle Jurassic fossil wood from ing wood types can be distinguished: Czestochowa region is character- • not-oxidized wood fragments, ized by variable preservation and the • partly oxidized wood fragments, type and degree of mineralization • completely oxidized wood fragments. Methods Instrumental geochemical analysis and polar fractions were eluted and sepa- TOC rated with DCM. The aliphatic fractions of The total organic carbon (TOC) and total samples were further analysed in details sulfur (TS) content were determined us- by gas chromatography–mass spectrome- ing Eltra Elemental Analyser model CS530. try (GC–MS). Extraction and separation GC–MS Samples were Soxhlet-extracted with di- The GC–MS analyses were performed with chloromethane (DCM) for 48 h in cellulose an Agilent 6890 Series Gas Chromatograph thimbles. Extracts were further separated interfaced to an Agilent 5973 Network using silica gel TLC plates (Merck, 20 x 20 Mass Selective Detector and Agilent 7683 x 0.25 cm). Prior to separation, these plates Series Injector (Agilent Technologies, Palo were activated at 120ºC for 1 h. Plates were Alto, CA). then loaded with the DCM extracts and de- The detailed description of GC-MS method veloped with n-hexane. Aliphatic, aromatic was made by e.g. Marynowski & Zatoń, (2010). 84 Contemporary Trends in Geoscience vol . 2 Results Aromatic hydrocarbons are present in the The very important biomarkers present in tested samples in relatively small amounts, the aromatic fraction are dehydroabietane, generally not exceeding 40% of all HCs and siomonellite and retene. The main precur- in most cases ranging between 10 to 25%. sors of these compounds in the wood samples Examples of PAHs distribution typical for are most probable ferruginol and sugiol (e.g. the most investigated samples are shown in Bechtel et al., 2007) - biomolecules characteris- Figures 2, 3, 4. In almost all of the wood sam- tic for resinous plant of the genus Cupressaceae, ples the dominating aromatic hydrocarbon Podocarpaceae and Araucariaceae which are is perylene and its methyl and dimethyl de- present in polar fraction of the wood (Otto rivatives (Fig. 3; see also Marynowski et al., and Wilde, 2001; Otto and Simoneit, 2001; 2013). The similar situation was reported from Marynowski et al. 2007b). The distribution of many Miocene brown coals (Fabiańska, 2007). discussed compounds is highly variable (Fig. According to our new data, perylene is a prod- 2 &. 5, Table 1). Only in one sample (SOW JS7) uct of wood degradation by wood degrading dehydroabietane dominates accounting for fungi during decay and transportation of the over 60% of the discoursed biomarkers (Fig. wood (Marynowski et al., 2013; see also Grice 5). In samples SOW JS1 and SOW JS4 domi- et al., 2009; Itoh et al., 2012). In some sam- nant compound is retene whereas dehydro- ples simonellit or retene are the main domi- abietane accounts for less than 6% (Table 1). nant or the second predominant compounds Interestingly, wood samples are derived from a (Fig. 4). Other quantitatively important un- very similar stratigraphic intervals, facies and identified aromatic compounds include the deposits, as well as characterized by the same structures with the following molecular ion: level of thermal maturity (Marynowski et al. M+ = 256 (U1), M+ = 394 (U2), M+ = 376 (U3) 2007a). Thus, the cause of the distribution di- (Fig.3) and M+ = 364 (U1), M+ = 394 (U2), versity of discussed aromatic biomarkers are M+ = 376 (U3) and M+ = 364 (U4) (Fig.4). probably early diagenetic processes affecting Other quantitatively important aromatic the wood, such as oxidation and the activity compounds are: of microorganisms. In case of samples with • cadalene, low diagenetic changes, cadalene, dehydro- • phenanthrene, abietane and/or siomonellite are dominat- • dehydroabietane, ed (GN JS2, GN JS4, GN JS6, SOW JS2, SOW • simonellite, JS6, SOW JS7 SOW JS10, SOW JS13, GRO JS). • pyrene, Whereas, the samples with high diagenetic Fig. 1. The most common aromat- • retene, changes contain mainly retene (SOW JS1, SOW ic hydrocarbons identified in the ex- • methylpyrenes, JS4). On the triangular diagram (Fig. 5), the amined fossil wood samples. • indeno[1,2,3-cd]pyrene, large differences in the content of these aro- • benzo[ghi]perylene (Figs. 1 – 4). matic biomarkers and the lack of any trends suggests influence of early diagenetic process, between which degradation of the wood by mi- croorganisms seems to be the most plausible. Retene and siomonellite could be also derived from the aromatization of α-phyllocladane (Otto and Simoneit, 2001). Phyllocladane was detected only in a few samples of the wood from the Czestochowa region (Marynowski et al. 2008; 2011). There is possible that diversity of dehydroabietane, retene and siomonellite distribution are also associated with different precursors, which were present in each wood species in variable concentrations. MPI1 parameter values (methylphenanthrene index) for the majority of the samples ranged from 0.1 to 0.5. These values calculated to vit- rinite reflectance (Rc) are in the range of 0.45% to 0.70% (Table 1). Actual measured Contemporary trends in Geoscience vol . 2 Justyna Smolarek, Leszek Marynowski 85 Aromatic hydrocarbons from the Middle Jurassic fossil wood of the Polish Jura 3-MP 2-MP 9-MP 1-MP MPI1 Rc Sim[%] Ret[%] Deh[%] Samples [%] [%] [%] [%] [%] m/z 237 m/z 219 m/z 255 Sowa clay-pit
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