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379157 
Journal Article 
Reaction rate constant of methane clathrate formation 
Bergeron, S; Beltran, JG; Servio, P 
2010 
1 
Fuel
ISSN: 0016-2361
EISSN: 1873-7153 
89 
2 
294-301 
English 
WOS:000271295400005 
Particle size distribution measurements were performed during the growth stage of methane hydrate formation in a semi-batch stirred tank crystallizer. Experiments were carried out at temperatures between 275.1 and 279.2 K and pressures ranging from 3873 to 5593 kPa. The reaction rate constant of methane hydrate formation was determined using the model of Bergeron and Servio (AIChE J 2008; 54:2964). The experimental reaction rate constant was found to increase with temperature, following an Arrhenius-type relationship, from 8.3 x 10 super(-8) m/s to 6.15 x 10 super(-7) m/s over the 4 degree range investigated, resulting in an activation energy of 323 kJ/mol. An increase in pressure of approximately 600 kPa did not have any effect on the reaction rate constant. Population balances, based on the measured critical nuclei diameter and that predicted by homogeneous nucleation theory, were also used for comparison purposes. The initial number of hydrate particles was calculated using the mole fraction of methane in the bulk liquid phase and compared to that predicted by an energy balance. 
Article Subject Terms: Fuels; Methane; Particle size; Particulates; Temperature; hydrates