加拿大油砂沥青中极性化合物的电喷雾——高分辨质谱研究

刘鹏; 黎茂稳; 孙永革; 蒋启贵; 陶国亮; 曹婷婷

doi:10.11781/sysydz201401089

加拿大油砂沥青中极性化合物的电喷雾——高分辨质谱研究

doi: 10.11781/sysydz201401089

刘鹏^1,2,3,
黎茂稳^2,3,
孙永革¹,
蒋启贵^2,3,
陶国亮^2,3,
曹婷婷^2,3

1.
浙江大学地球科学系, 杭州 310027
2. 中国石油化工集团公司油气成藏重点实验室, 江苏无锡 214126
3. 中国石油化工股份有限公司石油勘探开发研究院无锡石油地质研究所, 江苏无锡 214126

基金项目: 国家重点基础研究发展计划（973计划）（2012CB214801）；中国石化科技部项目（P11062）；中国博士后科学基金资助项目（2012M520550）及中国石化油气成藏重点实验室基金资助。

详细信息

作者简介:
刘鹏（1980-），男，博士后，从事油气地球化学研究工作。E-mail：liupeng_1207@163.com。

中图分类号: TE135.6
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出版历程
- 收稿日期: 2013-02-22
- 修回日期: 2013-12-02
- 刊出日期: 2014-01-28

Molecular characterization of polar species in Canadian oil sand bitumens by electrospray ionization and high resolution mass spectrometry

1.
Department of Earth Science, Zhejiang University, Hangzhou, Zhejiang 310027, China
2. SINOPEC Key Laboratory of Petroleum Accumulation Mechanisms, Wuxi, Jiangsu 214126, China
3. Wuxi Research Institute of Petroleum Geology, SINOPEC, Wuxi, Jiangsu 214126, China

摘要

摘要: 目前，生物降解作用对饱和烃生物标志物、芳香烃生物标志物参数以及小分子含氮化合物参数影响的研究较多，而对大分子极性化合物组成影响的研究较少。采用负离子电喷雾—傅立叶变换离子回旋共振质谱（ESI FT-ICR MS）分析不同降解级别的加拿大油砂沥青中酸性及非碱性氮化合物分子组成，结果表明，加拿大油砂沥青中杂原子化合物组成非常复杂，共鉴定出10种不同杂原子类型（N₁、N₁O₁、N₁O₂、N₁S₁、O₁、O₁S₁、O₂、O₂S₁、O₃、O₄）的化合物，其中以O₂类化合物为主。随着生物降解程度的加深，N₁、N₁O₁及O₁类化合物的相对丰度逐渐降低，而O₂及O₂S₁类化合物的相对丰度显现出逐渐增加的趋势；高分辨质谱分析在石油大分子杂原子化合物研究方面所独有的优势，为石油地球化学研究提供了新的思路。
- 油砂沥青 /
- 生物降解 /
- 极性化合物 /
- 环烷酸 /
- 电喷雾—傅立叶变换离子回旋共振质谱 /
- 加拿大
Abstract: At present, biodegradation effect on saturated hydrocarbon biomarkers, aromatic biomarker parameters and low molecular weight nitrogen compounds and their parameters is mostly studied, with less attention paid to the research of high molecular weight polar compounds. Four genetically related Canadian oil sand bitumens with various biodegradation levels have been analyzed by negative-ion electrospray ionization (ESI) and Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS). The results show that the neutral nitrogen and acidic heteroatom compounds in the oil sand bitumens include N₁,N₁O₁,N₁O₂,N₁S,O₁,O₁S₁,O₂,O₂S₁,O₃ and O₄ heteroatom classes, among which the O₂ class species are most abundant. With increasing biodegradation, the relative abundances of N₁,N₁O₁ and O₁ class species decrease slightly, while the relative abundances of O₂ and O₂S₁ class species increase slightly. The advantage of high resolution mass spectrometry for analyzing high molecular weight polar compounds in crude oil indicates great potential for developing new petroleum geochemistry techniques.
- oil sand /
- biodegradation /
- polar compound /
- naphthenic acid /
- ESI and FT-ICR MS /
- Canada

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参考文献(19)

[1]	王振齐, 卢鸿, 于赤灵, 等.济阳坳陷郑家—王庄油田生物降解稠油成熟度及油源研究[J].江汉石油学院学报, 2004, 26(2):1-6. Wang Zhenqi, Lu Hong, Yu Chiling, et al.Maturity and oil source of biodegradation viscous crude in Zhengjia-Wangzhuang oilfield of Jiyang depression[J].Journal of Jianghan Petroleum Institute, 2004, 26(2):1-6.
[2]	Larter S, Wilhelms A, Head I, et al.The controls on the composition of biodegraded oils in the deep subsurface:part 1:biodegradation rates in petroleum reservoirs[J].Organic Geochemistry, 2003, 34(4):601-613.
[3]	李秀鹏, 于洁.准噶尔盆地乌夏断裂带稠油类型及成因机理[J].断块油气田, 2012, 19(2):182-186. Li Xiupeng, Yu Jie.Classification and genetic mechanism of heavy oil in Wuerhe-Xiazijie fault belt, Junggar Basin[J].Fault-Block Oil and Gas Field, 2012, 19(2):182-186.
[4]	马安来, 张水昌, 张大江, 等.生物降解原油地球化学研究新进展[J].地球科学进展, 2005, 20(4):449-454. Ma Anlai, Zhang Shuichang, Zhang Dajiang, et al.The advances in the geochemistry of the biodegraded oil[J].Advance in Earth Sciences, 2005, 20(4):449-454.
[5]	彼得斯 K E, 沃尔特斯 C C, 莫尔多万 J M.生物标志化合物指南[M].2版.张水昌, 李振西, 等译.北京:石油工业出版社, 2011:189. Peters K E, Walters C C, Moldowan J M.The Biomarker Guide[M].2nd ed.Zhang Shuichang, Li Zhengxi, et al, eds.Beijing:Petroleum Industry Press, 2011:189.
[6]	Jenisch-Anton A, Adam P, Michaelis W, et al.Molecular evidence for biodegradation of geomacromolecules[J].Geochimica et Cosmochimica Acta, 2000, 64(20):3525-3537.
[7]	倪春华, 包建平, 顾忆.生物降解作用对芳烃生物标志物参数的影响研究[J].石油实验地质, 2008, 30(4):386-389. Ni Chunhua, Bao Jianping, Gu Yi.Study of biodegradation effect on aromatic biomarker parameters[J].Petroleum Geology & Experiment, 2008, 30(4):386-389.
[8]	史权, 赵锁奇, 徐春明, 等.傅立叶变换离子回旋共振质谱仪在石油组成分析中的应用[J].质谱学报, 2008, 29(6): 367-378. Shi Quan, Zhao Suoqi, Xu Chunming, et al.Fourier transform ion cyclotron resonance mass spectrometry and its application in petroleum analysis[J].Journal of Chinese Mass Spectrometry Society, 2008, 29(6):367-378.
[9]	Hughey C A, Rodgers R P, Marshall A G, et al.Acidic and neutral polar NSO compounds in Smackover oils of different thermal maturity revealed by electrospray high field Fourier transform ion cyclotron resonance mass spectrometry[J].Organic Geochemistry, 2004, 35(7):863-880.
[10]	Kim S, Stanford L A, Rodgers R P, et al.Microbial alteration of the acidic and neutral polar NSO compounds revealed by Fourier transform ion cyclotron resonance mass spectrometry[J].Organic Geochemistry, 2005, 36(8):1117-1134.
[11]	Liao Yuhong, Quan Shi, Hsu C S, et al.Distribution of acids and nitrogen-containing compounds in biodegraded oils of the Liaohe Basin by negative ion ESI FT-ICR MS[J].Organic Geochemistry, 2012, 47:51-65.
[12]	Li Maowen, Cheng Dingsheng, Pan Xiaohua, et al.Characterization of petroleum acids using combined FT-IR, FT-ICR-MS and GC-MS: Implications for the origin of high acidity oils in the Muglad Basin, Sudan[J].Organic Geochemistry, 2010, 41(9):959-965.
[13]	窦立荣, 黎茂稳.高酸值油藏的形成与分布[M].北京:地质出版社, 2010. Dou Lirong, Li Maowen.Origin and distribution of high acidity oils[M].Beijing:Geological Publishing House, 2010.
[14]	Kendrick E A.Mass Scale Based on CH₂=14.0000 for High Resolution Mass Spectrometry of Organic Compounds[J].Analytical Chemistry, 1963, 35(13):2146-2154.
[15]	Hughey C A, Hendrickson C L, Rodgers R P, et al.Kendrick Mass Defect Spectrum:A Compact Visual Analysis for Ultrahigh-Resolution Broadband Mass Spectra[J].Analytical Chemistry, 2001, 73(19):4676-4681.
[16]	Liu P, Xu C, Shi Q, et al.Characterization of Sulfide Compounds in Petroleum:Selective Oxidation Followed by Positive-Ion Electrospray Fourier Transform Ion Cyclotron Resonance Mass Spectrometry[J].Analytical Chemistry, 2010, 82(15):6601-6606.
[17]	Shi Quan, Pan Na, Long Haiyan, et al.Characterization of Middle-Temperature Gasification Coal Tar.Part 3:Molecular Composition of Acidic Compounds[J].Energy Fuels 2013, 27(1):108-117.
[18]	Peters K E, Walters C C, Moldowan J M.The biomarker guide, biomarkers and isotopes in petroleum exploration and earth history[M].2nd ed.Cambridge University press, New York, 2005.
[19]	Huang Haiping, Bowler B F, Zhang Zhanwen. et al.Influence of biodegradation on carbazole and benzocarbazole distributions in oil columns from the Liaohe basin, NE China[J].Organic Geochemistry, 2003, 34(7):951-969.