Improved kinetic modeling of the early generation of CO2 from the Boom Clay kerogen. Implications for simulation of CO2 production upon disposal of high activity nuclear waste

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Improved kinetic modeling of the early generation of CO2 from the Boom Clay kerogen. Implications for simulation of CO2 production upon disposal of high activity nuclear waste. / Lorant, François; Largeau, Claude; Behar, Françoise; De Cannière, Pierre.

In: Organic Geochemistry, Vol. 39, No. 9, 06.2008, p. 1294-1301.

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@article{4870ce0058e946caaf639cc3ca458422,
title = "Improved kinetic modeling of the early generation of CO2 from the Boom Clay kerogen. Implications for simulation of CO2 production upon disposal of high activity nuclear waste",
abstract = "A new kinetic model accounting for the generation of “early” CO2 from kerogen within the Boom Clay Formation was developed and calibrated using a large set of experimental pyrolysis data. The model also was constrained by the present day temperature of the clay where no CO2 generation is assumed. The kinetic scheme involved three competitive reactions characterized by relatively low activation energies, i.e., Ea <35 kcal/mol (146.5 kJ/mol) with an associated gas potential of ca. 49 mg of CO2 per gram of organic carbon. Focusing on the fastest reaction specifically, this study showed that the earliest stage of CO2 formation is associated with the thermal decomposition of moieties containing activated carboxylic acid functions present in the thermolabile fraction of the kerogen. Considering the temperature elevation within the Boom Clay Formation that would be imposed by high-level nuclear waste, the kinetic model predicts that (i) CO2 release would start about 1 year after disposal, and might reach the limits of the clay layer after about 100 years and (ii) for each meter length of gallery, the absolute cumulative mass of CO2 generated in a radius of 50 m around the gallery might reach ca. 3 tons.",
keywords = "Boom Clay, kerogen, organic matter, carbon dioxide, CO2, pCO2, decarboxylation, kinetics, pyrolysis, thermolysis, thermal stress, heat perturbation, HLW, nuclear waste",
author = "Fran{\cc}ois Lorant and Claude Largeau and Fran{\cc}oise Behar and {De Canni{\`e}re}, Pierre",
note = "Score = 10",
year = "2008",
month = "6",
doi = "10.1016/j.orggeochem.2008.05.008",
language = "English",
volume = "39",
pages = "1294--1301",
journal = "Organic Geochemistry",
issn = "0146-6380",
publisher = "Elsevier",
number = "9",

}

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TY - JOUR

T1 - Improved kinetic modeling of the early generation of CO2 from the Boom Clay kerogen. Implications for simulation of CO2 production upon disposal of high activity nuclear waste

AU - Lorant, François

AU - Largeau, Claude

AU - Behar, Françoise

AU - De Cannière, Pierre

N1 - Score = 10

PY - 2008/6

Y1 - 2008/6

N2 - A new kinetic model accounting for the generation of “early” CO2 from kerogen within the Boom Clay Formation was developed and calibrated using a large set of experimental pyrolysis data. The model also was constrained by the present day temperature of the clay where no CO2 generation is assumed. The kinetic scheme involved three competitive reactions characterized by relatively low activation energies, i.e., Ea <35 kcal/mol (146.5 kJ/mol) with an associated gas potential of ca. 49 mg of CO2 per gram of organic carbon. Focusing on the fastest reaction specifically, this study showed that the earliest stage of CO2 formation is associated with the thermal decomposition of moieties containing activated carboxylic acid functions present in the thermolabile fraction of the kerogen. Considering the temperature elevation within the Boom Clay Formation that would be imposed by high-level nuclear waste, the kinetic model predicts that (i) CO2 release would start about 1 year after disposal, and might reach the limits of the clay layer after about 100 years and (ii) for each meter length of gallery, the absolute cumulative mass of CO2 generated in a radius of 50 m around the gallery might reach ca. 3 tons.

AB - A new kinetic model accounting for the generation of “early” CO2 from kerogen within the Boom Clay Formation was developed and calibrated using a large set of experimental pyrolysis data. The model also was constrained by the present day temperature of the clay where no CO2 generation is assumed. The kinetic scheme involved three competitive reactions characterized by relatively low activation energies, i.e., Ea <35 kcal/mol (146.5 kJ/mol) with an associated gas potential of ca. 49 mg of CO2 per gram of organic carbon. Focusing on the fastest reaction specifically, this study showed that the earliest stage of CO2 formation is associated with the thermal decomposition of moieties containing activated carboxylic acid functions present in the thermolabile fraction of the kerogen. Considering the temperature elevation within the Boom Clay Formation that would be imposed by high-level nuclear waste, the kinetic model predicts that (i) CO2 release would start about 1 year after disposal, and might reach the limits of the clay layer after about 100 years and (ii) for each meter length of gallery, the absolute cumulative mass of CO2 generated in a radius of 50 m around the gallery might reach ca. 3 tons.

KW - Boom Clay

KW - kerogen

KW - organic matter

KW - carbon dioxide

KW - CO2

KW - pCO2

KW - decarboxylation

KW - kinetics

KW - pyrolysis

KW - thermolysis

KW - thermal stress

KW - heat perturbation

KW - HLW

KW - nuclear waste

UR - http://ecm.sckcen.be/OTCS/llisapi.dll/open/ezp_90540

UR - http://knowledgecentre.sckcen.be/so2/bibref/5077

U2 - 10.1016/j.orggeochem.2008.05.008

DO - 10.1016/j.orggeochem.2008.05.008

M3 - Article

VL - 39

SP - 1294

EP - 1301

JO - Organic Geochemistry

JF - Organic Geochemistry

SN - 0146-6380

IS - 9

ER -

ID: 63407