Proposing Crystallographic Theory to Deparameterize Hydrate Phase Description: Physical Insights and Validation

This work offers to resolve a crucial issue that has persisted for the last 60 years concerning the highly parametric equilibrium description of clathrate structures. Molecular (guest−guest and guest−host) interactions dominate the clathrate stability. The crystallographic theory is used for the stochastic estimation of these interactions contributing to lattice stability, which, in turn, governs the hydrate phase equilibrium. This innovative phenomenological approach formulates a pathway to deparameterize the hydrate phase model, and thereby, it avoids the traditional practice of parameter reduction of the existing statistical thermodynamic models followed by their parameter estimation that yields infinite sets of solution. This parameter-free formulation streamlines the elucidation of hydrate systems with great flexibility, and it is widely tested (total 48 systems) for single to multiple guests, pure to salt (single and multiple salts) water, and sI to sII hydrates. This novel approach to clathrate crystallography offers enormous new research possibilities and potential applications.