期刊
CHEMICAL GEOLOGY
卷 541, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.chemgeo.2020.119571
关键词
Intramolecular isotope; Carbon isotopes; Butane isomers; Hydrocarbons; Natural gas
资金
- JSPS [17H06105, P17725]
- U.S. Department of Energy Geosciences program [DE-SC0016271]
- MEXT, Japan [15K17774, 18K18782, 23224013]
- Kiban S
- Grants-in-Aid for Scientific Research [18K18782, 17H06105, 15K17774] Funding Source: KAKEN
A single-step method allowing the measurement of C-13 intramolecular distribution of butane isomers (n- and i-butane) from natural gas samples was developed. The method builds up on the one that has been developed for propane, using on-line pyrolysis followed by isotope analysis of the pyrolytic fragments. The isotopic filiation between n-butane and its pyrolytic fragments was elucidated using samples spiked with C-13 on terminal positions. The isotopic filiation for i-butane could not be shown experimentally due to the lack of commercially available enriched i-butane. We thus used a recent model named Reaction Mechanism Generator (RMG) to assess the origin of the fragments arising from i-butane pyrolysis. Butanes from natural gas samples from the Carnarvon Basin (Australia) and the Arkoma Basin (USA) were analyzed. The results are consistent with a model for thermogenic natural gas generation and suggest that combined intramolecular isotope composition of propane and n-butane can be related to the gas maturity. In addition, the method allows the detection and shed light on the mechanism of n-butane and i-butane biodegradation in natural gas reservoirs.
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