原油中金刚烷化合物的高效分析方法

张万峰; 童婷; 李东浩; 代威; 国朋飞; 何生; 朱书奎

doi:10.11781/sysydz201506796

原油中金刚烷化合物的高效分析方法

doi: 10.11781/sysydz201506796

张万峰^1,2,3,
童婷^1,2,
李东浩⁴,
代威^1,2,
国朋飞¹,
何生¹,
朱书奎^1,2, ,

1.
中国地质大学(武汉)构造与油气资源教育部重点实验室, 武汉 430074
2. 中国地质大学(武汉)生物地质与环境地质国家重点实验室, 武汉 430074
3. 中国科学院广州地球化学研究所同位素地球化学国家重点实验室, 广州 510640
4. 延边大学长白山生物资源与功能分子教育部重点实验室, 吉林延吉 133002

基金项目: 国家自然科学基金项目(21077039)和高等学校学科创新引智计划(B14031)资助。

详细信息

作者简介:
张万峰(1990—),男,工程师,从事有机地球化学和稀有气体同位素地球化学研究。E-mail:wfzhang@gig.ac.cn

通讯作者:
朱书奎(1972—),男,教授,从事有机地球化学和环境地球化学方向的研究。E-mail:shukuizhu@126.com

中图分类号: TE222.1
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- 被引次数: 0
出版历程
- 收稿日期: 2014-10-08
- 修回日期: 2015-09-12
- 刊出日期: 2015-11-28

A novel method for the determination of diamondoids in crude oils

Zhang Wanfeng^1,2,3,
Tong Ting^1,2,
Li Donghao⁴,
Dai Wei^1,2,
Guo Pengfei¹,
He Sheng¹,
Zhu Shukui^{1,2
, ,}

1.
Key Laboratory of Tectonics and Petroleum Resources of Ministry of Education, China University of Geosciences, Wuhan, Hubei 430074, China
2. State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan, Hubei 430074, China
3. State Key Laboratory of Isotope Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Geosciences, Guangzhou, Guangdong 510640, China
4. Key Laboratory of Nature Resource of the Changbai Mountain and Functional Molecular of Ministry of Education, Yanbian University, Yanji, Jilin 133002, China

摘要

摘要: 应用一种新型高效的预处理装置——气流吹扫-注射器微萃取仪(GP-MSE),对原油样品进行预处理,并利用全二维气相色谱-飞行时间质谱对样品中金刚烷化合物进行了定性定量分析。结果表明,GP-MSE与传统柱层析法相比,具有快速、操作简便、回收率高、重现性好等优点。单金刚烷、双金刚烷的相对标准偏差分别为1.57%和2.63%,能有效对原油样品进行净化和富集;与直接进样相比,相对偏差均小于9%,相关系数均大于0.997。
- 注射器微萃取 /
- 全二维气相色谱-飞行时间质谱 /
- 金刚烷化合物 /
- 地球化学参数 /
- 原油 /
- 珠江口盆地
Abstract: A novel device, termed as gas purge microsyringe extraction (GP-MSE), has been developed and applied to the preparation of different kinds of oil samples, including condensates, light and normal oils for the first time.Oils from the Pearl River Mouth Basin were firstly extracted by GP-MSE and then qualitatively and quantitatively analyzed by comprehensive two-dimensional gas chromatography with time-of-flight mass spectrometry (GC×GC-TOFMS).The proposed method has many advantages over traditional column chromatography, such as simple and fast steps, satisfactory recoveries, and lower consumption of solvents and samples.The relative standard deviations (RSD%) of adamantane and diamantane are 1.57% and 2.63%, respectively.Crude oil samples are purified and enriched effectively. The relative deviation is less than 9%, and the correlation coefficient is over 0.997.

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参考文献(24)

[1]	Huang B J,Xiao X M,Cai D S,et al.Oil families and their source rocks in the Weixinan Sub-basin,Beibuwan Basin,South China Sea[J].Organic Geochemistry,2011,42(2):134-145.
[2]	Wang Z D,Yang C,Hollebone B,et al.Forensic fingerprinting of diamondoids for correlation and differentiation of spilled oil and petroleum products[J].Environmental Science & Technology,2006,40(18):5636-5646.
[3]	Zhang S C,Huang H P,Xiao Z Y,et al.Geochemistry of Palaeozoic marine petroleum from the Tarim Basin,NW China.Part 2:Maturity assessment[J].Organic Geochemistry,2005,36(8):1215-1225.
[4]	崔景伟,王铁冠,胡健,等.塔里木盆地和田河气田轻质油成熟度判定及其油源意义[J].石油与天然气地质,2013,34(1):27-36. Cui Jingwei,Wang Tieguan,Hu Jian,et al.Maturity of light oil and its significance inindicating oil source in Hetianhe gas field,Tarim Basin[J].Oil & Gas Geology,2013,34(1):27-36.
[5]	Li J G,PhilpP,Cui M Z.Methyl diamantane index (MDI) as a maturity parameter for Lower Palaeozoic carbonate rocks at high maturity and overmaturity[J].Organic Geochemistry,2000,31(4):267-272.
[6]	Schulz L K,Wilhelms A,Rein E,et al.Application of diamondoids to distinguish source rock facies[J].Organic Geochemistry,2001,32(3):365-375.
[7]	Wei Z B,Moldowan J M,Zhang S C,et al.Diamondoid hydrocarbons as a molecular proxy for thermal maturity and oil cracking:Geochemical models from hydrous pyrolysis[J].Organic Geochemistry,2007,38(2):227-249.
[8]	Dahl J E,Liu S G,Carlson R M K.Isolation and structure of higher diamondoids,nanometer-sized diamond molecules[J].Science,2003,299(5603):96-99.
[9]	Dahl J E,Moldowan J M,Peters K E,et al.Diamondoid hydrocarbons as indicators of natural oil cracking[J].Nature,1999,399(6731):54-57.
[10]	Fang C C,Xiong Y Q,Liang Q Y,et al.Variation in abundance and distribution of diamondoids during oil cracking[J].Organic Geochemistry,2012,47:1-8.
[11]	Li S F,Hu S Z,Cao J,et al.Diamondoid characterization in condensate by comprehensive two-dimensional gas chromatography with time-of-flight mass spectrometry:the Junggar basin of Northwest China[J].International Journal of Molecular Sciences,2012,13(9):11399-11410.
[12]	Liang Q Y,Xiong Y Q,Fang C C,et al.Quantitative analysis of diamondoids in crude oils using gas chromatography-triple quadrupole mass spectrometry[J].Organic Geochemistry,2012,43:83-91.
[13]	Wang G L,Shi S B,Wang P R,et al.Analysis of diamondoids in crude oils using comprehensive two-dimensional gas chromatog-raphy/time-of-flight mass spectrometry[J].Fuel,2013,107:706-714.
[14]	马安来,金之钧,朱翠山,等.塔河油田原油中金刚烷化合物绝对定量分析[J].石油学报,2009,30(2):214-218. Ma Anlai,Jin Zhijun,Zhu Cuishan,et al.Quantitative analysis on absolute concentration of diamondoids in oils from Tahe Oilfield[J].Acta Petrolei Sinica,2009,30(2):214-218.
[15]	Grice K,Alexander R,Kagi R I.Diamondoid hydrocarbon ratios as indicators of biodegradation in Australian crude oils[J].Organic Geochemistry,2000,31(1):67-73.
[16]	Chen J H,Fu J M,Sheng G Y,et al.Diamondoid hydrocarbon ratios:Novel maturity indices for highly mature crude oils[J].Organic Geochemistry,1996,25(3/4):179-190.
[17]	Silva R C,Silva R S F,de Castro E V R,et al.Extended diamondoid assessment in crude oil using comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry[J].Fuel,2013,112:125-133.
[18]	Wei Z B,Moldowan J M,Jarvie D M,et al.The fate of diamondoids in coals and sedimentary rocks[J].Geology,2006,34(12):1013-1016.
[19]	Bastow T P,Van Aarssen B G K,Lang D.Rapid small-scale separation of saturate,aromatic and polar components in petroleum[J].Organic Geochemistry,2007,38(8):1235-1250.
[20]	Qiu J X,Wu C M,Fang Y Y,et al.Derivatization and liquid chromatography-UV-tandem mass spectrometric analysis of perfluorinated carboxylic acids[J].Journal of Chromatography A,2012,1235:132-140.
[21]	Yang C,Piao X F,Qiu J X,et al.Gas purge microsyringe extraction for quantitative direct gas chromatographic-mass spectrometric analysis of volatile and semivolatile chemicals[J].Journal of Chromatography A,2011,1218(12):1549-1555.
[22]	Zhu S K,Zhang W F,Dai W,et al.A simple model for separation prediction of comprehensive two-dimensional gas chromatography and its applications in petroleum analysis[J].Analy-tical Methods,2014,6(8):2608-2620.
[23]	梁前勇,熊永强,房忱琛,等.两种测定原油中金刚烷类化合物方法的对比研究[J].地球化学,2012,41(5):433-441. Liang Qianyong,Xiong Yongqiang,Fang Chenchen,et al.Comparison of two methods for the determination of diamondoids in crude oils[J].Geochimica,2012,41(5):433-441.
[24]	Wingert W S.GC-MS analysis of diamondoid hydrocarbons in Smackover petroleums[J].Fuel,1992,71(1):37-43.