4.6 Article

Experimental study on the intrinsic dissociation rate of methane hydrate

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CHEMICAL ENGINEERING SCIENCE
卷 282, 期 -, 页码 -

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PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ces.2023.119278

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Methane hydrate; Dissociation; Intrinsic kinetics; Rate constant; Activation energy

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This work developed a new method to directly measure the intrinsic dissociation rate of gas hydrate and modified the driving force in the dissociation model. The results demonstrate that the new model can accurately describe the effect of temperature on the hydrate decomposition rate.
This work developed a new method that can efficiently separate gas-liquid-hydrate mixture and obtain solid gas hydrate, making it possible to measure the intrinsic dissociation rate of gas hydrate directly. The results demonstrate that the classical Kim's model can reflect the relationship between driving force and hydrate dissociation rate when at same temperature, but can't accurately reveal the effect of temperature on hydrate decomposition rate when under the same driving force. In Kim's model, the driving force of hydrate dissociation was expressed as the difference between equilibrium fugacity (feq) and the fugacity of guest molecules in gas phase (fg). A new hydrate dissociation model was established in this work, and the driving force of hydrate dissociation was modified into (feq-fg)/feq, which has a higher universality than feq-fg. The intrinsic rate constant and activation energy of methane hydrate decomposition were determined to be 18905.35 mol/(m2 center dot s) and 22.149 kJ/mol, respectively.

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