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Chapter 4: Paleoplant Communities in New Zealand Coal Swamps As Revealed by Terpenoid Hydrocarbons

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Chapter 4: Paleoplant Communities in New Zealand Coal Swamps As Revealed by Terpenoid Hydrocarbons CHAPTER 4: PALEOPLANT COMMUNITIES IN NEW ZEALAND COAL SWAMPS AS REVEALED BY TERPENOID HYDROCARBONS Both results presented in the previous chapter and in the publications of KILLOPS ET AL. (1995; 2003), WESTON ET AL. (1988; 1989), WOOLHOUSE ET AL. (1992), BLUNT ET AL. (1988), ALEXANDER ET AL. (1983B), NOBLE ET AL. (1985) have demonstrated that the organic matter of New Zealand coals consists of mostly higher land-plant material with additional bacterial biomass. In order to build a more detailed insight into the occurrences of angiosperms and gymnosperms surrounding the coal swamps, this chapter presents results on the composition and occurrences of sesquiterpanes and sesterterpanes, diterpanes and triterpanes. The relative contribution of angiosperms and gymnosperms has been evaluated by the ratio of diterpenoids to non-hopanoid triterpenoids biomarkers in the aliphatic and aromatic fractions as established by BECHTEL ET AL. (2002). This ratio was then modified and denoted as di-/ (di- plus triterpenoids) ratio that is defined as the concentration of saturated plus aromatic diterpenoids divided by the sum concentration of diterpenoids plus angiosperm-derived triterpenoids (BECHTEL ET AL., 2005). Recently, the angiosperm-gymnosperm aromatic ratio (AGAR), that is the proportion of aromatic diterpenoids in the sum of aromatic di- plus triterpenoids, has been established to investigate the plant communities in the Mallik site, a gas hydrate production research well in Mackenzie Delte, Canada by HABERER ET AL. (2006). It means that either both the aliphatic and aromatic biomarkers or only the aromatic ones were considered to estimate the relative contribution of angiosperms and gymnosperms into organic matter. The plant communities of the New Zealand coals in this study were observed using both di-/ (di-plus triterpenoids) and AGAR ratios. 90 4.1 SESQUI- AND SESTERTERPENOID HYDROCARBONS Aliphatic sesquiterpenoid hydrocarbons The identification of aliphatic sesquiterpanes in this study was mostly based on the published mass spectra of PHILP (1985), which shows that they include mostly C14- C16 bicyclic sesquiterpanes [S1, S2, S7; FIGURE 4-1; TABLE 4-1]. Their appearances are indicative of higher plants contributing to the organic matter of the studied coals. Furthermore, 4α(H)- and 4ß(H)- eudesmane [S3, S4; FIGURE 4-1 TABLE 4-1] were also detected: ALEXANDER ET AL. (1983B) have shown that these compounds were found in sediments with a significant contribution of terrigenous source material and undoubtedly reflect their higher plant origins. The content of total higher plant sesquiterpanes was calculated, and shown to fall in the range from 2 to 25 µg/g TOC (TABLE 4-2). There were some samples with a high abundance of sesquiterpanes, e.g. G001989, G001990, G002585, G002587 (West Coast Basin) and G001994 (Taranaki Basin). One specific sample (G002611, Eastern Southland) had a particularly high concentration of C15 bicyclic compounds (c.a. 40 µg/gTOC), this being the only detectable sesquiterpane. Additionally, 8α(H)- and 8ß(H)-drimanes [S5-S6; FIGURE 4-1; TABLE 4-1] were found, possibly associated with a microbial contribution in New Zealand coals. In this regard, ALEXANDER ET AL. (1983B) reported that 8ß(H)-drimane was found both in all sixteen worldwide crude oils. These oils range from Cambrian to Tertiary and represent a wide-varying types, and bitumen extracts from drill-hole cuttings of wells in Carnarvon and Canning basins (W. Australia; varying in age from Ordovician to Early Cretaceous and spanning a wide range of maturity levels) whereas the 8α(H)-drimane was present in undetectable amounts. The widespread geological and geographical occurrence of 8ß(H)-drimane suggests its ubiquitous source. Additionally, this compound was also found in Cambrian-Ordovician samples, where land plant input was absent, rules out the possibility of its being derived from higher plant precursors. Because of that, the authors concluded that 8ß(H)-drimane is most likely of microbial origin. The microbial degradation of higher terpenes such as hopanes, or from direct formation of a compound or compounds containing the bicyclic ring system was suggested as the possible precursor of these compounds. Even so, it does not exclude the possible origin from land plants for 8α(H)- and 8ß(H)-drimanes that are also found in young sediments, like the investigated samples are (C.F. PHILP, 1994). In fact, ALEXANDER ET AL. (1984) have also shown 91 ISD 100 D9 G002590-West Coast Rank(Sr) = 7.4 Late Eocene 75 D6 50 D13 25 S8 S7 D1 S6 { D2 D3 S2 S1 0 30 35 40 45 50 55 60 65 70 D9 100 G001990- West Coast Rank(Sr) = 10.8 Relative Abundance Relative Late Cretaceous 75 50 ISD 25 D2 20 C n- 0 30 35 40 45 50 55 60 65 70 75 Time (min) Figure 4-1: GC/MS chromatograms (m/z 123) of representative aliphatic fractions of samples G002590 (upper) and G001990 (below) originated from West Coast basin. Compound names are listed in Table 4-1. Table 4-1: The sesqui- and sesterterpenoid hydrocarbon biomarkers found in aliphatic and aromatic fractions from extractabl e organic matters of New Zealand coals Peak N0 Aliphatic Compounds Formular Mol. W. References (m/z 123) S C bicyclic sesquiterpane C H 194 1 14 14 26 Philp, 1985 S2 C15 bicyclic sesquiterpane C15H28 208 S3 4α(H)-eudesmane C15H28 208 S 4ß(H)-eudesmane C H 208 4 15 28 Alexander et al., 1983b S5 8α(H)-drimane C15H28 208 S6 8ß(H)-drimane C15H28 208 S C bicyclic sesquiterpane C H 222 7 16 16 30 Philp, 1985 S8 Des-A-lupane C24H42 330 Peak N0 Aromatic Compounds Formular Mol. W References S9 5,6,7,8-tetrahydrocadalene C15H22 202 Wang & Simoneit, 1991; S10 Calamene C15H22 202 Weston et al., 1989; Philp, 1985 S11 Cadalene C15H18 198 92 Table 4-2: The concentrations of aliphatic and aromatic sesqui-, sester-, di- and triterpenoid hydrocarbon biomarkers (µg/g TOC) originated from micro-organisms, higher land plants (gymnosperms, angiosperms, or not specific). The relative contribution of gymnosperms and angiosperms are shown. Higher land plant Gymnosperms/ Microorganisms Gymnosperms Angiosperms (not specific) Angiosperms Samples Rank(Sr) Ali.Sesq. Aro.Tri. Hopanoids Ali.Sesq. Aro.Sesq. Ali.Sest. Ali.Di. Aro.Di. Ali.Tri. Aro.Tri. AGAR di/(di+tri) G001985 0 -- 37.7 166.32 -- -- -- 1.0 -- -- 37.7 -- 0.03 G001988 0 -- 49.2 119.25 -- -- -- 4.8 -- -- 49.2 -- 0.09 G001979 0.1 -- 382.8 330.94 -- -- -- 0.6 -- -- 382.8 -- 0.00 G001987 0.4 -- 78.9 288.17 -- -- -- 2.1 0.5 -- 78.5 0.01 0.03 G001986 0.6 -- 50.8 200.54 -- -- -- -- -- -- 50.8 -- -- G001976 1.6 -- 864.9 84.77 -- -- -- 4.8 4.6 -- 860.4 0.01 0.01 G001978 3 -- 696.7 112.87 -- -- -- 87.6 28.8 -- 667.9 0.04 0.15 G001975 3.4 -- 740.4 180.75 -- -- -- 99.8 43.0 7.3 697.4 0.06 0.17 G001983 4.7 -- 615.2 19.12 -- -- -- 20.6 40.6 27.7 574.6 0.07 0.09 G001977 5.4 -- 615.3 16.58 -- -- -- 54.1 36.0 44.7 579.3 0.06 0.13 G001982 5.6 -- 90.2 60.63 -- -- -- -- 7.7 33.9 82.5 0.09 0.06 G001984 6.1 0.7 465.7 22.20 0.5 -- -- 4.8 30.4 37.8 435.3 0.07 0.07 G001981 6.6 -- 719.8 31.22 -- -- -- 29.9 55.2 11.2 664.7 0.08 0.11 G001992 6.9 -- 182.4 30.39 -- -- -- 5.0 -- 7.7 182.4 -- 0.03 G001980 7 0.3 333.3 52.89 2.1 -- -- 17.4 51.2 35.4 282.1 0.15 0.18 G001989 11.6 -- 115.4 157.70 22.7 -- -- 18.1 28.4 -- 87.0 0.25 0.35 G001990 10.8 -- 155.0 94.38 13.7 -- -- 260.4 -- -- 155.0 -- 0.63 G001993 10.1 1.9 79.9 68.17 10.4 -- -- 19.3 21.3 -- 58.6 0.27 0.41 G001995 7.4 -- 249.8 28.68 -- 3.2 -- 7.7 38.8 -- 207.9 0.16 0.18 G001996 8.3 1.3 266.0 71.97 4.4 -- -- 10.5 69.7 -- 196.3 0.26 0.29 G001997 7.8 -- 211.5 39.03 2.7 -- -- 10.3 42.0 7.0 169.6 0.20 0.23 G001991 11.8 2.5 47.9 144.70 16.6 -- -- 1.6 -- -- 47.9 -- 0.03 G001994 9.5 1.0 431.2 81.62 5.0 -- -- 12.4 55.8 -- 375.4 0.13 0.15 93 Table 4-2 (continue) Higher land plant Gymnosperms/ Microorganisms Gymnosperms Angiosperms (not specific) Angiosperms Samples Rank(Sr) Ali.Sesq. Aro.Tri. Hopanoids Ali.Sesq. Aro.Sesq. Ali.Sest. Ali.Di. Aro.Di. Ali.Tri. Aro.Tri. AGAR di/(di+tri) G002610 1.6 -- 1801.9 42.51 4.5 2.3 1.0 4.2 66.8 5.6 1732.7 0.04 0.04 G002611 1.7 -- 267.4 23.77 40.6 2.5 1.4 4.3 44.7 4.3 220.1 0.17 0.18 G002595 2.2 -- 1026.4 281.77 -- 7.0 0.9 2.6 19.5 -- 999.9 0.02 0.02 G002600 2.3 -- 2131.8 87.97 -- 9.9 -- -- 64.1 -- 2057.8 0.03 0.03 G002596 2.5 -- 2372.5 409.04 -- -- -- -- 619.9 -- 1752.6 0.26 0.26 G002570 5.3 -- 925.6 102.69 -- -- 1.3 20.7 30.4 70.6 895.2 0.03 0.05 G002580 5.6 0.7 1475.8 61.40 3.0 3.5 1.4 11.7 43.1 74.3 1429.1 0.03 0.04 G002573 5.7 -- 959.8 115.52 -- -- 1.9 18.1 39.8 179.2 920.0 0.04 0.05 G002582 6.4 -- 1467.0 58.77 4.0 -- 2.0 3.6 138.7 80.7 1328.3 0.09 0.09 G002590 7.4 0.8 703.0 44.68 2.0 -- 2.1 27.3 208.0 14.1 495.1 0.30 0.32 G002606 7.5 -- 222.3 64.41 -- -- -- 155.7 51.3 -- 171.0 0.23 0.55 G002604 8.0 -- 960.4 83.00 -- 4.3 -- 4943.7 476.9 -- 479.2 0.50 0.92 G002592 10.3 -- 520.1 205.59 -- -- -- 2874.4 186.8 -- 333.3 0.36 0.90 G002587 10.5 3.9 78.2 167.08 26.3 -- 2.9 11.1 21.8 -- 56.4 0.28 0.37 G002585 10.6 3.0 114.2 97.96 20.3 -- -- 7.2 22.6 -- 91.6 0.20 0.25 Note: Ali.Sesq.
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