Temperature-Controlled\nGas Hydrate Nucleation in the\nHeterogeneous Environment

Nucleation of multicomponent systems is a pervasive phenomenon\nin nature and is pertinent to a diverse array of scientific and industrial\nchallenges. The nucleation mechanisms of immiscible multicomponent\nsystems remain unclear. Here, gas hydrate is employed as a model system\nto study the nucleation of multicomponent systems. The effect of gas/liquid\nand solid/liquid interfaces on hydrate nucleation is examined through\nmolecular dynamics simulations. The results demonstrate that gas hydrates\ntend to nucleate in the solution phase in the proximity of the gas/liquid\ninterface at lower temperatures, which is controlled by mass transfer.\nAs the temperature increases, the location of hydrate nucleation gradually\nshifts from the gas/liquid interface to the solid/liquid interface.\nWe anticipate that the nucleation free energy barrier dominates the\nhydrate nucleation process at these conditions, making the heterogeneous\nnucleation with a lower free energy barrier more probable. The findings\nprovide molecular insights into the mechanism and pathway underlying\ninterface-induced gas hydrate nucleation. These insights will inform\nthe development of the theory of gas hydrate nucleation, particularly\nin the context of heterogeneous nucleation.