The accurate prediction
of hydrate film thickness is critical for
addressing the hydrate-related issues in the fields of environment
and energy resource, including the disposal of greenhouse gases into
the ocean, evaluating the rising lifetime of bubble plumes in deepwater,
and flow assurance problems in subsea pipelines. However, the microscopic
mass-transfer mechanism in the existing hydrate film growth models
has not been thoroughly studied, especially in the pore updating inside
the hydrate film. In this work, an integrated mechanistic model of
hydrate film growth at the gas–liquid interface is developed.
Multiple mass-transfer behaviors that potentially control the thickening
growth of hydrate film are considered: (i) gas diffusion and water
permeation through the hydrate film; (ii) substance dissipation along
the hydrate pore channels; and (iii) gas transfer between the water/hydrate
interface and the surrounding fluid. In the new model, a characteristic
parameter is introduced to evaluate the pore updating efficiency,
which is determined by correlating with the published experimental
data. Based on the numerical solution of unsteady convection diffusion
equation, the gas concentration distribution in the flowing water
around the hydrate film is obtained, and the mass transfer coefficients
at different flow velocities are estimated correspondingly. Using
the proposed model, the dynamic evolution rules of hydrate film growth
at two specific conditions are investigated. The model predictions
for hydrate film steady-state thickness show a good agreement with
the measured results from the literature. Further, a sensitivity analysis
on the growing thickness of hydrate film is performed with various
influencing factors, which involves system subcooling, water flow
velocity, and dissolved gas concentration in liquid water. Eventually,
a case study for the scenario of the spatial and temporal changes
in film thickness on a rising methane bubble in Monterey Bay Canyon
is carried out. This work provides new insights into the interphase
mass-transfer characteristics for hydrate dynamic growth and can serve
as a useful reference for predicting the hydrate film thickness.