Received date: 2015-12-15
Revised date: 2015-01-05
Online published: 2016-01-10
The carbon isotopic series of alkane gases could be divided into three types:(1)positive carbon isotopic series:δ13C values increase with increasing carbon numbers among the C1-C4 alkanes,which is a typical characteristic for primary alkane gases;(2)negative carbon isotopic series:δ13C values decrease with increasing carbon numbers among the C1-C4 alkanes;(3)partial carbon isotopic reversal,which has no increasing or decreasing relationship between the δ13C values and carbon numbers.Negative carbon isotopic series could be further subdivided into primary and secondary origins.The former is a typical characteristic of abiogenic gases while the later is resulted from the secondary alteration imposed on biogenic gases,which is commonly observed in over-mature shale gas or coal-derived gas.Previous works have proposed several possible explanations for negative carbon isotopic series of secondary origins such as secondary cracking,diffusion,the Rayleigh fractionation of ethane and propane through redox reaction with the participation of transition metal and water at 250-300℃.After a comparative study,the authors found that negative carbon isotopic series of secondary origin for both shale gas and coal-derived gas appeared in the area where source rocks(shales)are at over-mature stage while it was not observed in the area where source rocks(shales)are only at mature-high mature stage.As a result,extremely high maturity(＞200℃)is the main controlling factor for negative carbon isotopic series of secondary origin.Within this maturity interval,secondary cracking,diffusion and Rayleigh fractionation of ethane and propane could happen separately or together.
Dai Jin-xing，Ni Yun-yan，Huang Shi-peng，Gong De-yu，Liu Dan，Feng Zi-qi，Peng Wei-long，Han Wen-xue . Origins of secondary negative carbon isotopic series in natural gas[J]. Natural Gas Geoscience, 2016 , 27(1) : 1 -7 . DOI: 10.11764/j.issn.1672-1926.2016.01.0001
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