Simulation of the THF hydrate–water interfacial free energy from computer simulation

In this work, the tetrahydrofuran (THF) hydrate-water interfacial free energy is determined at 500\,bar, at one point of the univariant two-phase coexistence line of the THF hydrate, by molecular dynamics simulation. The Mold Integration-Host methodology, an extension of the original Mold Integration technique to deal with hydrate-fluid interfaces, is used to calculate the interfacial energy. Water is described using the well-known TIP4P/Ice model and THF is described using a rigid version of the TraPPE model. We have recently used the combination of these two models to accurately describe the univariant two-phase dissociation line of the THF hydrate, in a wide range of pressures, from computer simulation [J. Chem. Phys. 160, 164718 (2024)]. The THF hydrate-water interfacial free energy predicted in this work is compared with the only experimental data available in the literature. The value obtained, 27(2)\,mJ/m², is in excellent agreement with the experimental data taken from the literature, 24(8)\,mJ/m². To the best of our knowledge, this is the first time that the THF hydrate-water interfacial free energy is predicted from computer simulation. This work confirms that the Mold Integration technique can be used with confidence to predict solid-fluid interfaces of complex structures, including hydrates that exhibit sI and sII crystallographic structures.