title: Nonequilibrium adiabatic molecular dynamics simulations of methane clathrate hydrate decomposition.
abstract: Nonequilibrium, constant energy, constant volume (NVE) molecular dynamics simulations are used to study the decomposition of methane clathrate hydrate in contact with water. Under adiabatic conditions, the rate of methane clathrate decomposition is affected by heat and mass transfer arising from the breakup of the clathrate hydrate framework and release of the methane gas at the solid-liquid interface and diffusion of methane through water. We observe that temperature gradients are established between the clathrate and solution phases as a result of the endothermic clathrate decomposition process and this factor must be considered when modeling the decomposition process. Additionally we observe that clathrate decomposition does not occur gradually with breakup of individual cages, but rather in a concerted fashion with rows of structure I cages parallel to the interface decomposing simultaneously. Due to the concerted breakup of layers of the hydrate, large amounts of methane gas are released near the surface which can form bubbles that will greatly affect the rate of mass transfer near the surface of the clathrate phase. The effects of these phenomena on the rate of methane hydrate decomposition are determined and implications on hydrate dissociation in natural methane hydrate reservoirs are discussed.
authors.affiliation: Department of Chemistry, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada. saman.alavi@nrc-cnrc.gc.ca
authors.forename: Saman
authors.initials: S
authors.lastname: Alavi
authors.forename: J A
authors.initials: JA
authors.lastname: Ripmeester
mesh_terms: D008697:Methane / Q000737:chemistry*; D056004:Molecular Dynamics Simulation; D013499:Surface Properties; D014867:Water / Q000737:chemistry*
chemical_list: D014867:Water; D008697:Methane