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Graptolites As Fossil Geo-Thermometers and Source Material Of

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Graptolites As Fossil Geo-Thermometers and Source Material Of 1 Graptolites as fossil geo-thermometers and source material of 2 hydrocarbons: an overview of four decades of progress 3 Qingyong Luoa, b, Goodarzi Fariborzc, Ningning Zhonga, b*, Ye Wanga, b, Nansheng Qiua, b, 4 Christian B. Skovstedd, Václav Suchýe, Niels Hemmingsen Schovsbof, Rafał Morgag, 5 Jingyue Haoa, b, Anji Liua, b, Jin Wua, b, Xu Mina, b, Weixun Caoa, b, Jia Wua, b 6 a State Key Laboratory of Petroleum Resources and Prospecting, China University of Petroleum, Beijing 102249, China; 7 b College of Geoscience, China University of Petroleum, Beijing 102249, China; 8 c FG &Partner Ltd, Research Group, 29 Hawkside Mews NW., Calgary, Alberta, Canada; 9 d Department of Palaeobiology, Swedish Museum of Natural History, Box 50007, SE-104 05 Stockholm, Sweden; 10 e Nuclear Physics Institute, v. v. i.,Academy of Sciences of the Czech Republic, Na Truhlářce 39/64, 180 86 Prague 8, Czech 11 Republic; 12 f Geological Survey of Denmark and Greenland (GEUS), Øster Voldgade 10, DK-1350 Copenhagen K, Denmark; 13 g Silesian University of Technology, Faculty of Mining, Safety Engineering and Industrial Automation, Institute of Applied 14 Geology, Akademicka 2, 44-100 Gliwice, Poland. 15 16 *Corresponding author at: State Key Laboratory of Petroleum Resources and Prospecting, China 17 University of Petroleum, Changping, Beijing, 102249, China. Tel.: +86 10 89734548. E-mail address: 18 [email protected]. 19 20 Abstract 21 The thermal maturity of Lower Paleozoic graptolite-bearing marine sediments, which host many 22 hydrocarbon deposits worldwide, has long been difficult to determine due to the absence of wood-derived 23 vitrinite particles for conventional vitrinite reflectance. In 1976, graptolite reflectance was introduced as 24 a new indicator for organic maturity of these deposits and has been used since in many regional studies. 25 The majority of these studies, however, were done on a limited sample set and a limited range of thermal 26 maturity, which resulted in a number of controversial views concerning the usefulness of graptolite 27 reflectance as an alternative paleothermal indicator and its correlation with vitrinite reflectance through 28 various proxies. In this paper, we review previous studies and combine those analyses with new data to 29 assess the physical and chemical characteristics of graptolite periderm with increasing thermal maturity. 30 We conclude that graptolite random reflectance (GRor) is a better parameter for the thermal maturity 31 assessment than graptolite maximum reflectance (GRomax) due to the better quality of available data and 32 time saving. Combining published data with results of our study of both natural and heat-treated 33 graptolites and vitrinite, we present a new correlation between GRor and equivalent vitrinite reflectance 34 (EqVRo), as EqVRo = 0.99GRor + 0.08. Chemical composition of graptolite periderm is similar to vitrinite; 35 graptolites are mainly kerogen Type II-III, are gas prone and have a substantial hydrocarbon potential. 36 Lower Paleozoic graptolite-bearing organic-rich sediments are important shale gas source rocks and 37 reservoirs globally and make a significant contribution to worldwide petroleum reserves. 38 Keywords: Optical characteristics; Graptolite reflectance; Chemical composition; Microstructure; 39 Wufeng–Longmaxi Formations; Alum Shale; Hot shale; Shale gas. 40 41 1. Introduction and previous studies 42 Lower Paleozoic graptolite-bearing rocks were mainly deposited in marine environments, and are 43 important source rocks globally, especially shale gas deposits in the Wufeng–Longmaxi (also known as 44 Wufeng–Lungmachi) sediments from China (Zou et al., 2010; Zou et al., 2012; Dai et al., 2014; Dai et 45 al., 2016; Luo et al., 2016; Zou et al., 2016; Luo et al., 2017; Luo et al., 2018). These organic matter 46 (OM)-rich facies were also identified as true or potential hydrocarbon source rocks in the Anadarko basin 47 in the USA (Wang and Philp, 1997), North Africa and Arabian Peninsula (Jones and Stump, 1999; Lüning 48 et al., 2000), Taurus region of Turkey (Varol et al., 2006), the Czech Republic (Suchý et al., 2002), and 49 the Siberian platform (Makarov and Bazhenova, 1981). More recently, such shales have been recognized 50 as potential targets for unconventional shale gas deposits in the Norwegian-Danish Basin (Schovsbo et al. 51 2011, 2014; Pool et al. 2012), and Baltic basin of Central Europe (Littke et al., 2011; Karcz et al., 2013; 52 Yang et al. 2017). 53 Vitrinite reflectance is a most commonly used indicator for the thermal maturity (Stach et al., 1982; 54 Taylor et al., 1998; Suárez-Ruiz et al., 2012; Hackley and Cardott, 2016). However, due to the lack of 55 vitrinite (coalified wood) in pre-Devonian rocks, the determination of thermal maturity of Lower 56 Paleozoic graptolite-bearing rocks is always a difficult topic and a hot debate for petroleum industry 57 (Goodarzi, 1984; Goodarzi, 1985a; Goodarzi and Norford, 1985, 1987; Bertrand and Heroux, 1987; 58 Bustin et al., 1989; Bertrand, 1990; Goodarzi et al., 1992a; Bertrand, 1993; Petersen et al., 2013; Luo et 59 al., 2016; Luo et al., 2017; Luo et al., 2018). Thus, the surrogate proxies, such as the reflectance of 60 zooclasts, vitrinite-like particles and solid bitumen, Tmax, and biomarkers, have been proposed to assess 61 organic maturity in Lower Paleozoic graptolite-bearing sediments (Teichmüller, 1978; Goodarzi and 62 Norford, 1987; Jacob, 1989; Schoenherr et al., 2007; Suárez-Ruiz et al., 2012; Schmidt et al., 2019). 63 Tmax may be unreliable due to low S2 in overmature sediments (Peters, 1986; Peters and Cassa, 1994). 64 The maturity-related biomarker ratios may be also influenced by depositional environments and biological 65 sources, which will increase the difficulty of data interpretation (Radke and Welte, 1983; Radke et al., 66 1986; Radke, 1988; George and Ahmed, 2002; Peters et al., 2005). In addition, the biomarker ratios may 67 be invalid to assess thermal maturity of overmature sediments (Peters et al., 2005). Graptolite-bearing 68 rocks often contain bitumen and other zooclasts (Teichmüller, 1978; Goodarzi and Norford, 1987; Jacob, 69 1989; Schoenherr et al., 2007; Suárez-Ruiz et al., 2012; Schmidt et al., 2019). The difficulty with using 70 of solid bitumen reflectance is due to large variation in most samples, and their origin, e.g., by thermal 71 cracking, biodegradation and deasphalting (George et al., 1994; Hwang et al., 1998; Mastalerz et al., 2018), 72 all of which increase difficulty in data interpretation (e.g., Gonçalves et al., 2014; Fink et al., 2016). The 73 origin of discrete vitrinite-like particles remains controversial, and possible explanations includes: 74 migrated bitumen, either indigenous or exogenous to the host rock (Bertrand and Heroux, 1987); 75 gelification of polysaccharides (Buchardt and Lewan, 1990); residues of algae after maturation (Wang et 76 al., 1994); biodegraded zooclasts that are the product of a reducing to strongly reducing environment 77 (Xiao et al., 1997); marine humification of planktonic and benthic organisms (Romankevich, 1984), the 78 so called “marine vitrinite group” (Zhong and Qin, 1995); and fragments of graptolites (Petersen et al., 79 2013). 80 Zooclasts have clear advantage in reflectance studies due to their specific biological sources 81 compared to that of solid bitumen and vitrinite-like particles, and thus their reflectance was naturally 82 regarded as having a superior potential as a thermal maturity proxy. In general, graptolites are more 83 common than other zooclasts (e.g., chitinozoans and scolecodonts) in Lower Paleozoic marine rocks, and 84 as a result, the nature of graptolite reflectance has been a “hot topic” for organic petrologists over several 85 decades (Kurylowicz et al., 1976; Teichmüller, 1978; Goodarzi, 1984, 1985a; Bertrand and Heroux, 1987; 86 Bertrand, 1990; Link et al., 1990; Cardott and Kidwai, 1991; Hoffknecht, 1991; Goodarzi et al., 1992b; 87 Malinconico, 1992; Tricker et al., 1992; Malinconico, 1993; Wang et al., 1993; Cole, 1994; Gentzis et al., 88 1996; Liu et al., 2001; Bertrand et al., 2003; Petersen et al., 2013; İnan et al., 2016; Lavoie et al., 2016; 89 Luo et al., 2016; Luo et al., 2017; Luo et al., 2018; Synnott et al., 2018; Wang et al., 2019a). 90 Graptolite reflectance is a useful proxy of thermal maturity (Goodarzi, 1984; Goodarzi and Norford, 91 1985), and has been used to assess eroded thicknesses when used in conjunction with reflectance of 92 bitumen and sedimentological and tectonic evidences (Goodarzi et al., 1992b; Gentzis et al., 1996). The 93 graptolite maximum reflectance (GRomax) or graptolite random reflectance (GRor) was adopted to estimate 94 thermal maturity in worldwide sediments (Goodarzi, 1984; Goodarzi and Norford, 1985; Goodarzi et al., 95 1985; Goodarzi and Norford, 1989; Goodarzi et al., 1992b; Malinconico, 1992, 1993; Rantitsch, 1995; 96 Gentzis et al., 1996; Bertrand et al., 2003; Petersen et al., 2013; İnan et al., 2016; Lavoie et al., 2016; Luo 97 et al., 2016; Luo et al., 2017; Luo et al., 2018). Some researchers have established correlations among 98 reflectances of graptolite and other zooclasts, pyrobitumen and vitrinite (Bertrand and Heroux, 1987; 99 Bertrand, 1990; Bertrand, 1993; Yang and Hesse, 1993; Bertrand and Malo, 2001; Bertrand et al., 2003), 100 and Conodont Alteration Index (CAI; Goodarzi and Norford, 1985; Hoffknecht, 1991; Gentzis et al., 101 1996). Moreover, the graptolite reflectance has also been successfully correlated with some inorganic 102 paleothermal indices, including the illite “crystallinity” index (e.g. Kemp et al., 1985; Oliver, 1988; 103 Hoffknecht, 1991; Rantitsch, 1995, 1997; Suchý et al., 2015), and metamorphic index minerals in pre- 104 greenschist meta-sedimentary rocks (e.g. Malinconico, 1992). Graptolite reflectance is commonly related 105 to the lithology, and it will be higher in shales than in limestones (Link et al., 1990). Redox conditions 106 may have an impact on graptolite reflectance, and higher reflectance was observed in graptolites deposited 107 under oxic environments in comparison with those from anoxic environments (Cole, 1994).
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