Chemical Engineering Communications, Vol.144, 51-64, 1996
Investigations into the nucleation behaviour of methane gas hydrates
Details on the design and construction of a high-pressure, temperature controlled sapphire cell are reported for the study of clathrate hydrate nucleation under pristine experimental conditions. Laser light scattering optics and detection equipment have been successfully integrated with the apparatus to monitor the development of the incipient phase and characterize the early stages of hydrate growth. Experiments on the scattering behaviour of the nucleation process have revealed that within the detection limit of the technique, the hydrate phase was not present in sufficient size or number prior to its catastrophic appearance. A series of investigations to identify nucleation process variables have verified the existence of an aqueous phase thermal history. In addition, the efficacy of perturbations on inducing hydrate formation has been established. These studies are consistent with literature on the formation of ice and the crystallization of inorganic salts and sugars. The data support an argument that the nucleation process is non-deterministic due to a probabilistic element within the nucleation mechanism.