Determination of kinetic parameters and simulation of early CO2 production from the Boom Clay kerogen under low thermal stress

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Determination of kinetic parameters and simulation of early CO2 production from the Boom Clay kerogen under low thermal stress. / De Cannière, Pierre; Deniau, I.; Behar, F.; Largeau, C.; Beaucaire, C.; Pitsch, H.; Van Geet, Maarten (Peer reviewer).

In: Applied Geochemistry, Vol. 20, 2005, p. 2097-2107.

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De Cannière, Pierre ; Deniau, I. ; Behar, F. ; Largeau, C. ; Beaucaire, C. ; Pitsch, H. ; Van Geet, Maarten. / Determination of kinetic parameters and simulation of early CO2 production from the Boom Clay kerogen under low thermal stress. In: Applied Geochemistry. 2005 ; Vol. 20. pp. 2097-2107.

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@article{4c88acee95734199b18c7dfec55d5cbb,
title = "Determination of kinetic parameters and simulation of early CO2 production from the Boom Clay kerogen under low thermal stress",
abstract = "The main purpose of the present study is to evaluate the nature and amount of gaseous compounds that would be generated from the Boom Clay kerogen due to the foreseen thermal stress associated with the geological disposal of high activity nuclear waste. To this end, pyrolysis experiments were carried out on this low maturity, O-rich kerogen with focus on mild conditions, including Rock–Eval and closed pyrolyses using a wide range of temperature/time conditions. The residual kerogen recovered after the closed pyrolyses was re-examined by Rock–Eval and elemental analyses and the components of the gas fractions were identified and quantified by gas chromatography. These experiments showed substantial production of CO2 (corresponding to ca. 1/5 of the total O content of the kerogen) under mild thermal stress. The kinetic parameters (frequency factor and distribution of activation energy) of this early production of CO2 were determined and used to simulate the possible consequences for the deep disposal of highly radioactive waste. Extrapolation to thermal stresses, corresponding to 80 and 100 °C over 1 ka, indicated that this production of CO2 might influence the geochemistry and perhaps therefore the effectiveness of the geological barrier. For example, unless diffusion out of the heated zone counterbalances the effect of CO2 generation, significant acidification and large changes in bicarbonate concentration may take place, in the interstitial water of the clay, at a time scale of only tens to a few hundred years.",
keywords = "PCO2, early CO2 production, Boom Clay, kerogen, thermal stress, kinetic, organic matter, HLW, spent fuel",
author = "{De Canni{\`e}re}, Pierre and I. Deniau and F. Behar and C. Largeau and C. Beaucaire and H. Pitsch and {Van Geet}, Maarten",
note = "Score = 10",
year = "2005",
doi = "10.1016/j.apgeochem.2005.07.006",
language = "English",
volume = "20",
pages = "2097--2107",
journal = "Applied Geochemistry",
issn = "0883-2927",
publisher = "Elsevier",

}

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TY - JOUR

T1 - Determination of kinetic parameters and simulation of early CO2 production from the Boom Clay kerogen under low thermal stress

AU - De Cannière, Pierre

AU - Deniau, I.

AU - Behar, F.

AU - Largeau, C.

AU - Beaucaire, C.

AU - Pitsch, H.

A2 - Van Geet, Maarten

N1 - Score = 10

PY - 2005

Y1 - 2005

N2 - The main purpose of the present study is to evaluate the nature and amount of gaseous compounds that would be generated from the Boom Clay kerogen due to the foreseen thermal stress associated with the geological disposal of high activity nuclear waste. To this end, pyrolysis experiments were carried out on this low maturity, O-rich kerogen with focus on mild conditions, including Rock–Eval and closed pyrolyses using a wide range of temperature/time conditions. The residual kerogen recovered after the closed pyrolyses was re-examined by Rock–Eval and elemental analyses and the components of the gas fractions were identified and quantified by gas chromatography. These experiments showed substantial production of CO2 (corresponding to ca. 1/5 of the total O content of the kerogen) under mild thermal stress. The kinetic parameters (frequency factor and distribution of activation energy) of this early production of CO2 were determined and used to simulate the possible consequences for the deep disposal of highly radioactive waste. Extrapolation to thermal stresses, corresponding to 80 and 100 °C over 1 ka, indicated that this production of CO2 might influence the geochemistry and perhaps therefore the effectiveness of the geological barrier. For example, unless diffusion out of the heated zone counterbalances the effect of CO2 generation, significant acidification and large changes in bicarbonate concentration may take place, in the interstitial water of the clay, at a time scale of only tens to a few hundred years.

AB - The main purpose of the present study is to evaluate the nature and amount of gaseous compounds that would be generated from the Boom Clay kerogen due to the foreseen thermal stress associated with the geological disposal of high activity nuclear waste. To this end, pyrolysis experiments were carried out on this low maturity, O-rich kerogen with focus on mild conditions, including Rock–Eval and closed pyrolyses using a wide range of temperature/time conditions. The residual kerogen recovered after the closed pyrolyses was re-examined by Rock–Eval and elemental analyses and the components of the gas fractions were identified and quantified by gas chromatography. These experiments showed substantial production of CO2 (corresponding to ca. 1/5 of the total O content of the kerogen) under mild thermal stress. The kinetic parameters (frequency factor and distribution of activation energy) of this early production of CO2 were determined and used to simulate the possible consequences for the deep disposal of highly radioactive waste. Extrapolation to thermal stresses, corresponding to 80 and 100 °C over 1 ka, indicated that this production of CO2 might influence the geochemistry and perhaps therefore the effectiveness of the geological barrier. For example, unless diffusion out of the heated zone counterbalances the effect of CO2 generation, significant acidification and large changes in bicarbonate concentration may take place, in the interstitial water of the clay, at a time scale of only tens to a few hundred years.

KW - PCO2

KW - early CO2 production

KW - Boom Clay

KW - kerogen

KW - thermal stress

KW - kinetic

KW - organic matter

KW - HLW

KW - spent fuel

UR - http://ecm.sckcen.be/OTCS/llisapi.dll/open/ezp_27324

UR - http://knowledgecentre.sckcen.be/so2/bibref/3009

U2 - 10.1016/j.apgeochem.2005.07.006

DO - 10.1016/j.apgeochem.2005.07.006

M3 - Article

VL - 20

SP - 2097

EP - 2107

JO - Applied Geochemistry

JF - Applied Geochemistry

SN - 0883-2927

ER -

ID: 188929