Abstract
We have devised an experimental method for calculating isotopic mass balances for the 12C and 13C in the pyrolysis products from a type II kerogen during artificial maturation in a closed system. The method also enables a study of the isotopic evolution of cracking products versus kerogen transformation ratios. The type II kerogen (Paris Basin) was at the onset of catagenesis. Pyrolysis was carried out in a confined closed system under isothermal conditions, at several temperatures (275–350 °C) and times at a constant pressure of 10 Mpa. Under these conditions, the kerogen transformation ratios covered a range from 1% to 87%. Pyrolysis effluents were separated into hydrocarbon gases (C 1–C 5), non-hydrocarbon gases (CO, CO 2, H 2, H 2S), C 6–C 14 products soluble in pentane (C 6–C 14 saturated, C 6–C 14 aromatics), C 14+ products soluble in pentane (C 14+ saturated, C 14+ aromatics, resins 1), C 14+ products soluble in dichloromethane (asphaltenes and resins 2) and residue insoluble in dichloromethane. Validation of mass and atomic carbon balances plus δ 13C measurements was checked carefully in order to obtain accurate isotopic mass balances. Mass balances on pyrolysis products were higher than 97.7% of the initial kerogen amount. The δ 13C fractionation observed between different pyrolysis products reached 18‰, but only 2‰ between different C 14+ fractions within the range of pyrolysis conditions.
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