南海北部油气缓释环境沉积物脂类化合物组成特征
|
摘要
认识沉积环境有机碳留存状况是阐述油气形成过程中有机碳早期成岩的关键内容。以南海珠江口盆地及其邻近海域为背景,通过研究表层沉积物中脂类化合物的形态组成,认识脂类有机碳的来源和留存状态,阐述特征脂类分子的早期成岩特征。结果表明,研究区域表层沉积物有机碳含量为0.22%～0.66%,有机碳稳定同位素分布在-20.88‰～-22.93‰之间,表现为显著的海源特征。沉积物中共检测出21种脂肪酸、6种脂肪醇、8种甾醇和植醇;总脂肪酸、脂肪醇、甾醇和植醇含量分别为12.57～40.27μg/g、5.35～8.98μg/g、0.15～3.75μg/g和0.01～3.99μg/g干重,总体表现为靠近珠江口和台湾海峡略高。脂类化合物的存在形态以游离态(FR)和碱性水解态(BH)为主,酸性水解态(AH)贡献较低;其中植醇和甾醇呈现显著的BH优势,植醇中未检出AH组分的贡献。脂类化合物主要来自于海洋现场生产,海洋微藻和细菌的相对贡献率分别为21.18%～33.78%和11.02%～15.64%,陆源高等植物贡献低于5%。来源于硫酸盐还原菌的支链脂肪酸在靠近珠江口海域高达1.79～2.62μg/g,占总脂肪酸的5.14%～6.50%,并与硫酸盐还原过程相关的古菌分布相一致。
Distribution and composition of organic carbon is the key to demonstrating the early diagenesis of organic carbon in the formation of oil and gas. Surface sediments were collected and analyzed to determine the content and form composition of lipid biomarkers in the estuary of the Pearl River Basin and adjacent areas in the South China Sea. The sources and occurrence of lipid compounds are also discussed. Results show that the organic carbon content range was 0.22%-0.66% in the sediment samples. The δ~(13)C was-20.88‰ to-22.93‰, which implies a marine source of organic carbon. In total, 21 fatty acids, 6 fatty alcohols, 8 sterols and phytol were detected in the sediments. The content of total fatty acids, fatty alcohols, sterols and phytol ranged from 12.57 to 40.27 μg/g, 5.35-8.98 μg/g, 0.15-3.75 μg/g and 0.01-3.99 μg/g dry weight, respectively. The higher contents were located at the stations closest to the Pearl River estuary and Taiwan Strait. Lipid compounds mainly existed as free(FR) and base hydrolytic(BH) forms, with very little in acidic hydrolytic(AH) form. Phytol and sterols dominated BH components, but AH phytol was not detected. Lipid compounds primarily originate from marine microalgae and bacteria, with a small contribution from higher plants. The specific fatty acids produced by marine microalgae and bacteria contributed 21.18%-33.78% and 11.02%-15.64% to total fatty acids, respectively. The content of branched chain fatty acids(possibly derived from sulfate-reducing bacteria) was higher, at 1.79-2.62 μg/g dry weight, and accounted for 5.14%-6.50% of total fatty acids in sediments closest to the Pearl River estuary. These consisted of archaea microbes, implying sulfate reduction.
Distribution and composition of organic carbon is the key to demonstrating the early diagenesis of organic carbon in the formation of oil and gas. Surface sediments were collected and analyzed to determine the content and form composition of lipid biomarkers in the estuary of the Pearl River Basin and adjacent areas in the South China Sea. The sources and occurrence of lipid compounds are also discussed. Results show that the organic carbon content range was 0.22%-0.66% in the sediment samples. The δ~(13)C was-20.88‰ to-22.93‰, which implies a marine source of organic carbon. In total, 21 fatty acids, 6 fatty alcohols, 8 sterols and phytol were detected in the sediments. The content of total fatty acids, fatty alcohols, sterols and phytol ranged from 12.57 to 40.27 μg/g, 5.35-8.98 μg/g, 0.15-3.75 μg/g and 0.01-3.99 μg/g dry weight, respectively. The higher contents were located at the stations closest to the Pearl River estuary and Taiwan Strait. Lipid compounds mainly existed as free(FR) and base hydrolytic(BH) forms, with very little in acidic hydrolytic(AH) form. Phytol and sterols dominated BH components, but AH phytol was not detected. Lipid compounds primarily originate from marine microalgae and bacteria, with a small contribution from higher plants. The specific fatty acids produced by marine microalgae and bacteria contributed 21.18%-33.78% and 11.02%-15.64% to total fatty acids, respectively. The content of branched chain fatty acids(possibly derived from sulfate-reducing bacteria) was higher, at 1.79-2.62 μg/g dry weight, and accounted for 5.14%-6.50% of total fatty acids in sediments closest to the Pearl River estuary. These consisted of archaea microbes, implying sulfate reduction.
引文
[1] 苏广庆,罗又郎,邱传珠,等. 南海东北部沉积环境和沉积演化模式的初步研究[J]. 海洋学报,1987,9(3):335-343. [Su Guangqing, Luo Youlang, Qiu Chuanzhu, et al. Preliminary exploration of sedimentary environment and evolution model in the northeastern South China Sea[J]. Acta Oceanologica Sinica, 1987, 9(3): 335-343.]
[2] 陈芳,庄畅,周洋,等. 南海东北部陆坡天然气水合物钻探区生物地层与沉积速率[J]. 地球科学,2016,41(3):416-424. [Chen Fang, Zhuang Chang, Zhou Yang, et al. Calcareous nannofossils and foraminifera biostratigraphy on the northeastern slope of the South China Sea and variation in sedimentation rates[J]. Earth Science, 2016, 41(3): 416-424.]
[3] 于晓果,金肖兵,姚旭莹,等. 甲烷流体活动与沉积物中碳、氮同位素组成响应:南海东北部海洋IV号地区研究[J]. 海洋学研究,2013,31(3):1-7. [Yu Xiaoguo, Jin Xiaobing, Yao Xuying, et al. The stable isotopic composition of sediments in methane fluid flowing area, Haiyang IV, the northern part of South China Sea[J]. Journal of Marine Sciences, 2013, 31(3): 1-7.]
[4] 茅晟懿,朱小畏,孙永革,等. 南海北部神狐海域现代沉积物正构脂肪酸来源:加权平均碳同位素的建立与应用[J]. 海洋地质前沿,2014,30(8):1-15. [Mao Shengyi, Zhu Xiaowei, Sun Yongge, et al. Source of saturated fatty acids in modern sediments in Shenhu area, northern South China Sea and implications: application of n-weighted average carbon isotope[J]. Marine Geology Frontiers, 2014, 30(8): 1-15.]
[5] Thena T, Mohan K. Estimation of pore space methane hydrate in marine sediments of Cascadia margin[J]. Journal of Natural Gas Science and Engineering, 2016, 35: 956-963.
[6] 吴能友,邬黛黛,叶瑛,等. 南海东北部东沙海域沉积物烃类有机地球化学研究及其意义[J]. 南海地质研究,2007(1):1-14. [Wu Nengyou, Wu Daidai, Ye Ying, et al. Hydrocarbon geochemical study of sediments from Dongsha area, Northeast South China Sea and their significances[J]. Gresearch of Eological South China Sea, 2007(1): 1-14.]
[7] Haddad R I, Martens C S, Farrington J W. Quantifying early diagenesis of fatty acids in a rapidly accumulating coastal marine sediment[J]. Organic Geochemistry, 1992, 19(1/2/3): 205-216.
[8] 王江涛,杨庶,谭丽菊,等. 浙江南部近海沉积物柱状样中脂类生物标志物的组成及形态分布[J]. 海洋学报,2011,33(5):83-90. [Wang Jiangtao, Yang Shu, Tan Liju, et al. Composition and form distribution of lipids biomarkers in a sediment core from southern coastal area of Zhejiang province[J]. Acta Oceanologica Sinica, 2011, 33(5): 83-90.]
[9] Tissot B P, Pelet R, Ungerer P. Thermal history of sedimentary basins, maturation indices, and kinetics of oil and gas generation[J]. American Association of Petroleum Geologists Bulletin, 1987, 71(12): 1445-1466.
[10] Brinis A, Mejanelle L, Momzikoff A, et al. Phospholipid ester-linked fatty acids composition of size-fractionated particles at the top ocean surface[J]. Organic Geochemistry, 2004, 35(11/12): 1275-1287.
[11] Stefanova M, Disnar J R. Composition and early diagenesis of fatty acids in lacustrine sediments, lake Aydat (France)[J]. Organic Geochemistry, 2000, 31(1): 41-55.
[12] 段毅,崔明中,罗斌杰,等. 我国海洋沉降颗粒物质的有机地球化学研究:I. 有机质通量及烃类化合物和脂肪酸分布特征[J]. 中国科学(D辑):地球科学,1997,27(5):442-446. [Duan Yi, Cui Mingzhong, Luo Binjie et al. Organic geochemical studies of sinking particulate material in China sea area(I): organic matter fluxes and distributional features of hydrocarbon compounds and fatty acids[J]. Science China (Seri.D): Earth Sciences, 1997, 27(5): 442-446.]
[13] 曹梦莉,马倩倩,吴莹,等. 南海北部和海南岛附近海域表层沉积物中有机质的分布和降解状态的差异[J]. 海洋与湖沼,2017,48(2):258-265. [Cao Mengli, Ma Qianqian, Wu Ying, et al. Difference in organic matter distribution and degradation in surface sediment between northern South China Sea and Hainan Island[J]. Oceanologia et Limnologia Sinica, 2017, 48(2): 258-265.]
[14] 赵美训,赵晓晨,陈建芳,等. 南海表层沉积物生物标志物的分布特征及古生产力重建意义[J]. 热带海洋学报,2009,28(3):45-53. [Zhao Meixun, Zhao Xiaochen, Chen Jianfang, et al. Distribution of phytoplankton biomarkers in surface sediments from the South China Sea and its implication for paleoproductivity reconstruction[J]. Journal of Tropical Oceanography, 2009, 28(3): 45-53.]
[15] 彭溶. 应用脂类化合物研究北黄海沉积物有机碳的埋藏特征[D]. 青岛:中国海洋大学,2012. [Peng Rong. Sedimentary of organic carbon in the sediments of North Yellow Sea: Indicated by lipid compounds[D]. Qingdao: Ocean University of China, 2012.]
[16] Jia G D, Peng P A. Temporal and spatial variations in signatures of sedimented organic matter in Lingding Bay (Pearl estuary), southern China[J]. Marine Chemistry, 2003, 82(1/2): 47-54.
[17] Volkman J K. A review of sterol markers for marine and terrigenous organic matter[J]. Organic Geochemistry, 1986, 9(2): 83-99.
[18] Volkman J K, Jeffrey S W, Nichols P D, et al. Fatty acid and lipid composition of 10 species of microalgae used in mariculture[J]. Journal of Experimental Marine Biology and Ecology, 1989, 128(3): 219-240.
[19] Volkman J K. Sterols and other triterpenoids: source specificity and evolution of biosynthetic pathways[J]. Organic Geochemistry, 2005, 36(2): 139-159.
[20] Peng X Z, Zhang G, Mai B X, et al. Tracing anthropogenic contamination in the Pearl River estuarine and marine environment of South China Sea using sterols and other organic molecular markers[J]. Marine Pollution Bulletin, 2005, 50(8): 856-865.
[21] 黄良民,陈清朝,尹健强,等. 珠江口及邻近海域环境动态与基础生物结构初探[J]. 海洋环境科学,1997,16(3):1-7. [Huang Liangmin, Chen Qingchao, Yin Jianqiang, et al. Basic organism composition and environment status of the Zhujiang estuary and adjacent waters[J]. Marine Environmental Science, 1997, 16(3): 1-7.]
[22] 康建华,陈兴群,黄邦钦. 台湾海峡及其邻近海域表层水叶绿素a含量时空变化特征[J]. 台湾海峡,2010,29(1):34-41. [Kang Jianhua, Chen Xingqun, Huang Bangqin. Study on the spatial and temporal variation of surface chlorophyll a in Taiwan Strait and its adjacent waters[J]. Journal of Oceanography in Taiwan Strait, 2010, 29(1): 34-41.]
[23] 高寒凌. 黄渤海沉积物有机碳的运输和矿化特征研究[D]. 青岛:中国海洋大学,2016. [Gao Hanling. Study on the transport and mineralization of organic carbon in the Yellow Sea and Bohai Sea[D]. Qingdao: Ocean University of China, 2016.]
[24] 于文涛. 黄河三角洲潮间带有机碳的地球化学研究[D]. 青岛:中国海洋大学,2014. [Yu Wentao. The geochemical research of organic carbon in the intertidal zone of the Yellow River Delta[D]. Qingdao: Ocean University of China, 2014.]
[25] Ding H B, Sun M Y. Biochemical degradation of algal fatty acids in oxic and anoxic sediment-seawater interface systems: effects of structural association and relative roles of aerobic and anaerobic bacteria[J]. Marine Chemistry, 2005, 93(1): 1-19.
[26] 周鹏,李冬梅,刘广山,等. 南海东北部和南部海域表层沉积物生物硅研究[J]. 热带海洋学报,2010,29(4):40-47. [Zhou Peng, Li Dongmei, Liu Guangshan, et al. Biogenic silica in surface sediments of the northeastern and southern South China Sea[J]. Journal of Tropical Oceanography, 2010, 29(4): 40-47.]
[27] Londry K L, Jahnke L L, Marais D J D. Stable Carbon isotope ratios of lipid biomarkers of sulfate-reducing bacteria[J]. Applied and Environmental Microbiology, 2004, 70(2): 745-751.
[28] Taylor J, Parkes R J. Identifying different populations of sulphate-reducing bacteria within marine sediment systems, using fatty acid biomarkers[J]. Journal of General Microbiology, 1985, 131(3): 631-642.
[29] Boetius A, Ravenschlag K, Schubert C J, et al. A marine microbial consortium apparently mediating anaerobic oxidation of methane[J]. Nature, 2000, 407(6804): 623-626.
[30] 张国赏,吴文鹃,潘仁瑞. 气相色谱—质谱法检测细胞脂肪酸及其在细菌鉴定上的应用[J]. 合肥联合大学学报,2000,10(4):92-96. [Zhang Guoshang, Wu Wenjuan, Pan Renrui. Determination of fatty acids in cells by GC-MS and its application in bacterium identification[J] Journal of Hefei Union University, 2000, 10(4): 92-96.]
[31] 陈烨,张玉,甄毓,等. 南海东北部珠江口盆地沉积物中古菌群落垂向分布研究[J]. 海洋环境科学,2017,36(5):735-740. [Chen Ye, Zhang Yu, Zhen Yu, et al. Vertical profile of archaeal community in the sediments of Pearl River Mouth Basin in the northeastern South China Sea[J]. Marine Environmental Science, 2017, 36(5): 735-740.]
[2] 陈芳,庄畅,周洋,等. 南海东北部陆坡天然气水合物钻探区生物地层与沉积速率[J]. 地球科学,2016,41(3):416-424. [Chen Fang, Zhuang Chang, Zhou Yang, et al. Calcareous nannofossils and foraminifera biostratigraphy on the northeastern slope of the South China Sea and variation in sedimentation rates[J]. Earth Science, 2016, 41(3): 416-424.]
[3] 于晓果,金肖兵,姚旭莹,等. 甲烷流体活动与沉积物中碳、氮同位素组成响应:南海东北部海洋IV号地区研究[J]. 海洋学研究,2013,31(3):1-7. [Yu Xiaoguo, Jin Xiaobing, Yao Xuying, et al. The stable isotopic composition of sediments in methane fluid flowing area, Haiyang IV, the northern part of South China Sea[J]. Journal of Marine Sciences, 2013, 31(3): 1-7.]
[4] 茅晟懿,朱小畏,孙永革,等. 南海北部神狐海域现代沉积物正构脂肪酸来源:加权平均碳同位素的建立与应用[J]. 海洋地质前沿,2014,30(8):1-15. [Mao Shengyi, Zhu Xiaowei, Sun Yongge, et al. Source of saturated fatty acids in modern sediments in Shenhu area, northern South China Sea and implications: application of n-weighted average carbon isotope[J]. Marine Geology Frontiers, 2014, 30(8): 1-15.]
[5] Thena T, Mohan K. Estimation of pore space methane hydrate in marine sediments of Cascadia margin[J]. Journal of Natural Gas Science and Engineering, 2016, 35: 956-963.
[6] 吴能友,邬黛黛,叶瑛,等. 南海东北部东沙海域沉积物烃类有机地球化学研究及其意义[J]. 南海地质研究,2007(1):1-14. [Wu Nengyou, Wu Daidai, Ye Ying, et al. Hydrocarbon geochemical study of sediments from Dongsha area, Northeast South China Sea and their significances[J]. Gresearch of Eological South China Sea, 2007(1): 1-14.]
[7] Haddad R I, Martens C S, Farrington J W. Quantifying early diagenesis of fatty acids in a rapidly accumulating coastal marine sediment[J]. Organic Geochemistry, 1992, 19(1/2/3): 205-216.
[8] 王江涛,杨庶,谭丽菊,等. 浙江南部近海沉积物柱状样中脂类生物标志物的组成及形态分布[J]. 海洋学报,2011,33(5):83-90. [Wang Jiangtao, Yang Shu, Tan Liju, et al. Composition and form distribution of lipids biomarkers in a sediment core from southern coastal area of Zhejiang province[J]. Acta Oceanologica Sinica, 2011, 33(5): 83-90.]
[9] Tissot B P, Pelet R, Ungerer P. Thermal history of sedimentary basins, maturation indices, and kinetics of oil and gas generation[J]. American Association of Petroleum Geologists Bulletin, 1987, 71(12): 1445-1466.
[10] Brinis A, Mejanelle L, Momzikoff A, et al. Phospholipid ester-linked fatty acids composition of size-fractionated particles at the top ocean surface[J]. Organic Geochemistry, 2004, 35(11/12): 1275-1287.
[11] Stefanova M, Disnar J R. Composition and early diagenesis of fatty acids in lacustrine sediments, lake Aydat (France)[J]. Organic Geochemistry, 2000, 31(1): 41-55.
[12] 段毅,崔明中,罗斌杰,等. 我国海洋沉降颗粒物质的有机地球化学研究:I. 有机质通量及烃类化合物和脂肪酸分布特征[J]. 中国科学(D辑):地球科学,1997,27(5):442-446. [Duan Yi, Cui Mingzhong, Luo Binjie et al. Organic geochemical studies of sinking particulate material in China sea area(I): organic matter fluxes and distributional features of hydrocarbon compounds and fatty acids[J]. Science China (Seri.D): Earth Sciences, 1997, 27(5): 442-446.]
[13] 曹梦莉,马倩倩,吴莹,等. 南海北部和海南岛附近海域表层沉积物中有机质的分布和降解状态的差异[J]. 海洋与湖沼,2017,48(2):258-265. [Cao Mengli, Ma Qianqian, Wu Ying, et al. Difference in organic matter distribution and degradation in surface sediment between northern South China Sea and Hainan Island[J]. Oceanologia et Limnologia Sinica, 2017, 48(2): 258-265.]
[14] 赵美训,赵晓晨,陈建芳,等. 南海表层沉积物生物标志物的分布特征及古生产力重建意义[J]. 热带海洋学报,2009,28(3):45-53. [Zhao Meixun, Zhao Xiaochen, Chen Jianfang, et al. Distribution of phytoplankton biomarkers in surface sediments from the South China Sea and its implication for paleoproductivity reconstruction[J]. Journal of Tropical Oceanography, 2009, 28(3): 45-53.]
[15] 彭溶. 应用脂类化合物研究北黄海沉积物有机碳的埋藏特征[D]. 青岛:中国海洋大学,2012. [Peng Rong. Sedimentary of organic carbon in the sediments of North Yellow Sea: Indicated by lipid compounds[D]. Qingdao: Ocean University of China, 2012.]
[16] Jia G D, Peng P A. Temporal and spatial variations in signatures of sedimented organic matter in Lingding Bay (Pearl estuary), southern China[J]. Marine Chemistry, 2003, 82(1/2): 47-54.
[17] Volkman J K. A review of sterol markers for marine and terrigenous organic matter[J]. Organic Geochemistry, 1986, 9(2): 83-99.
[18] Volkman J K, Jeffrey S W, Nichols P D, et al. Fatty acid and lipid composition of 10 species of microalgae used in mariculture[J]. Journal of Experimental Marine Biology and Ecology, 1989, 128(3): 219-240.
[19] Volkman J K. Sterols and other triterpenoids: source specificity and evolution of biosynthetic pathways[J]. Organic Geochemistry, 2005, 36(2): 139-159.
[20] Peng X Z, Zhang G, Mai B X, et al. Tracing anthropogenic contamination in the Pearl River estuarine and marine environment of South China Sea using sterols and other organic molecular markers[J]. Marine Pollution Bulletin, 2005, 50(8): 856-865.
[21] 黄良民,陈清朝,尹健强,等. 珠江口及邻近海域环境动态与基础生物结构初探[J]. 海洋环境科学,1997,16(3):1-7. [Huang Liangmin, Chen Qingchao, Yin Jianqiang, et al. Basic organism composition and environment status of the Zhujiang estuary and adjacent waters[J]. Marine Environmental Science, 1997, 16(3): 1-7.]
[22] 康建华,陈兴群,黄邦钦. 台湾海峡及其邻近海域表层水叶绿素a含量时空变化特征[J]. 台湾海峡,2010,29(1):34-41. [Kang Jianhua, Chen Xingqun, Huang Bangqin. Study on the spatial and temporal variation of surface chlorophyll a in Taiwan Strait and its adjacent waters[J]. Journal of Oceanography in Taiwan Strait, 2010, 29(1): 34-41.]
[23] 高寒凌. 黄渤海沉积物有机碳的运输和矿化特征研究[D]. 青岛:中国海洋大学,2016. [Gao Hanling. Study on the transport and mineralization of organic carbon in the Yellow Sea and Bohai Sea[D]. Qingdao: Ocean University of China, 2016.]
[24] 于文涛. 黄河三角洲潮间带有机碳的地球化学研究[D]. 青岛:中国海洋大学,2014. [Yu Wentao. The geochemical research of organic carbon in the intertidal zone of the Yellow River Delta[D]. Qingdao: Ocean University of China, 2014.]
[25] Ding H B, Sun M Y. Biochemical degradation of algal fatty acids in oxic and anoxic sediment-seawater interface systems: effects of structural association and relative roles of aerobic and anaerobic bacteria[J]. Marine Chemistry, 2005, 93(1): 1-19.
[26] 周鹏,李冬梅,刘广山,等. 南海东北部和南部海域表层沉积物生物硅研究[J]. 热带海洋学报,2010,29(4):40-47. [Zhou Peng, Li Dongmei, Liu Guangshan, et al. Biogenic silica in surface sediments of the northeastern and southern South China Sea[J]. Journal of Tropical Oceanography, 2010, 29(4): 40-47.]
[27] Londry K L, Jahnke L L, Marais D J D. Stable Carbon isotope ratios of lipid biomarkers of sulfate-reducing bacteria[J]. Applied and Environmental Microbiology, 2004, 70(2): 745-751.
[28] Taylor J, Parkes R J. Identifying different populations of sulphate-reducing bacteria within marine sediment systems, using fatty acid biomarkers[J]. Journal of General Microbiology, 1985, 131(3): 631-642.
[29] Boetius A, Ravenschlag K, Schubert C J, et al. A marine microbial consortium apparently mediating anaerobic oxidation of methane[J]. Nature, 2000, 407(6804): 623-626.
[30] 张国赏,吴文鹃,潘仁瑞. 气相色谱—质谱法检测细胞脂肪酸及其在细菌鉴定上的应用[J]. 合肥联合大学学报,2000,10(4):92-96. [Zhang Guoshang, Wu Wenjuan, Pan Renrui. Determination of fatty acids in cells by GC-MS and its application in bacterium identification[J] Journal of Hefei Union University, 2000, 10(4): 92-96.]
[31] 陈烨,张玉,甄毓,等. 南海东北部珠江口盆地沉积物中古菌群落垂向分布研究[J]. 海洋环境科学,2017,36(5):735-740. [Chen Ye, Zhang Yu, Zhen Yu, et al. Vertical profile of archaeal community in the sediments of Pearl River Mouth Basin in the northeastern South China Sea[J]. Marine Environmental Science, 2017, 36(5): 735-740.]