Development of new method for D/H ratio measurements for volatile hydrocarbons of crude oils using solid phase micro-extraction (SPME) coupled to gas chromatography isotope ratio mass spectrometry (GC-IRMS)
Development of new method for D/H ratio measurements for volatile hydrocarbons of crude oils using solid phase micro-extraction (SPME) coupled to gas chromatography isotope ratio mass spectrometry (GC-IRMS)
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使用固相微萃取 (SPME) 结合气相色谱同位素比质谱 (GC-IRMS) 开发原油挥发性碳氢化合物 D/H 比测量新方法
DOI：
10.1016/j.marpetgeo.2017.01.008
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发表时间：
2018
影响因子：
4.2
通讯作者：
Zuodong Wang
中科院分区：
文献类型：
--
作者：
Zhongping Li;Liwu Li;Lantian Xing;Yan Liu;Mingjie Zhang;Xibin Wang;Chunhui Cao;Zuodong Wang
在化合物特异性同位素分析（CSIA）中，一个主要的挑战是有效的样品处理和分离足够量的分析物以准确测量同位素比。原油中正常水平烃类的氢同位素比值（D/H）已成功地用作油-油、油气对比的同位素示踪剂，但对于小尺寸烃类（C6单键C15）的研究进展甚微。本文提出了一种新的样品处理方法，实现了对这些特殊化合物的D/H比分析。该方法可以被表征为一个有效的方法，其特点是固相微萃取（SPME）耦合GC-IRMS（气相色谱-同位素比值质谱）。在这项研究中，CAR/DVB/PDMS纤维进行了评估，并作为吸收材料，和操作条件，包括提取时间，（0.1 min-150 min）和浸提温度（-30 °C-140 °C），这可能会影响吸附量，进行了仔细的评估，并且发现吸附产率不仅随操作条件而且随分子大小而显著变化。此外，还讨论了氢同位素分馏对D/H比值的影响，发现在萃取过程中未观察到氢同位素分馏，SPME-GC/IRMS得到的D/H比值与EA-IRMS结果吻合较好。值得注意的是，两种方法之间的差异通常在0.8‰至4.2‰的预期不确定度内，表明该方法对于挥发性烃富集和D/H测量是高效的。为验证所建立方法的有效性，对一个典型原油样品进行了分析，D/H比值结果显示出相当大的变化，足以区分不同的化合物，表明所建立的方法非常适合痕量烃富集，是迄今为止D/H分析最有效、最可靠的手段。
In compound-specific isotope analysis (CSIA), one major challenge is the effective sample treatment and the isolation of sufficient amount of analytes for accurate measurements for isotope ratios. The hydrogen isotope ratio (D/H) of normal level hydrocarbons in crude oils has been successfully used as an isotopic tracer in oil-oil and oil-gas correlations, but little progress so far has been made for small size hydrocarbons (C6single bondC15). In this paper, we presented a novel method for sample treatment and achieved the D/H ratio analysis for these particular compounds. The method can be characterized as an efficient approach featured by SPME (solid phase micro-extraction) coupled to GC-IRMS (gas chromatography-isotope ratio mass spectrometry). In this investigation, the CAR/DVB/PDMS fiber was evaluated and used as the absorptive material, and the operating conditions, including the extraction time (0.1 min–150 min) and the extraction temperature (−30 °C–140 °C), which may affect the adsorption amount, were carefully evaluated, and it was found that the adsorption yields varied considerably not only with the operating conditions but also with the molecular size. In addition, the possible hydrogen isotopic fractionation, which may exert strong influence on D/H ratios, were also discussed, it was found that the hydrogen isotopic fractionation were not observed in the extraction process, and the D/H ratios obtained via SPME-GC/IRMS were in good agreement with the EA-IRMS. Notably, the difference between the two approaches was generally within the expected uncertainties from 0.8‰ to 4.2‰, indicating the method is high efficient for volatile hydrocarbon enrichments and the D/H measurements. To assess the validity of the established method, one typical crude oil sample was analyzed, and the D/H ratio results displayed considerable large variation, enough to distinguished between different compounds, showing the established method is well suited for trace hydrocarbon enrichment, and provides so far the most efficient and reliable means for D/H analysis.
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影响因子：
3.4
作者：
Yi Wang;Y. Huang
通讯作者：
Yi Wang;Y. Huang
影响因子：
2.8
作者：
A. Rushdi;P. Clark;A. Mix;V. Ersek;V. Ersek;B. Simoneit;B. Simoneit;Hai Cheng;R. Edwards
通讯作者：
A. Rushdi;P. Clark;A. Mix;V. Ersek;V. Ersek;B. Simoneit;B. Simoneit;Hai Cheng;R. Edwards
DOI：
10.1016/j.chroma.2013.10.065
发表时间：
2013-12
期刊：
Journal of chromatography. A
影响因子：
--
作者：
Jing Fan;Z. Dong;M. Qi;R. Fu;L. Qu
通讯作者：
Jing Fan;Z. Dong;M. Qi;R. Fu;L. Qu
化石燃料燃烧残留物中正烷烃的化合物特定氢同位素组成
影响因子：
5
作者：
Bai Huiling;Peng Lin;Li Zhongping;Liu Xiaofeng;Song Chongfang;Mu Ling
通讯作者：
Mu Ling
DOI：
10.1016/j.chroma.2014.10.089
发表时间：
2014-12
期刊：
Journal of chromatography. A
影响因子：
--
作者：
Zhongping Li;Xibin Wang;Liwu Li;Mingjie Zhang;Mingxin Tao;Lan-tian Xing;Chunhui Cao;Yanqing Xia-Yanqing-X
通讯作者：
Zhongping Li;Xibin Wang;Liwu Li;Mingjie Zhang;Mingxin Tao;Lan-tian Xing;Chunhui Cao;Yanqing Xia-Yanqing-X