Molecular perspectives of interfacial properties of the hydrogen+water mixture in contact with silica or kerogen

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Interfacial behaviours in multiphase systems containing H2 are crucial to underground H2 storage but are not well understood. Molecular dynamics simulations were carried out to investigate interfacial properties of the H2+H2O and H2+H2O+silica/kerogen systems over a broad range of temperatures (298 - 523 K) and pressures (1 - 160 MPa). The combination of the H2 model with the INTERFACE force field and TIP4P/2005 H2O model can accurately predict the experimental interfacial tensions (IFTs) of the H2+H2O mixture. The IFTs from simulations are also in accordance with predictions from density gradient theory combined with the PC-SAFT equation of state. In general, the IFT decreases with pressure and temperature. However, at relatively high temperatures and pressures, the IFTs increase with pressure. The opposite pressure influence on IFTs can be explained by the inversion of the sign of the relative adsorption of H2. The H2 enrichment in the interfacial regions was identified in density distributions. Meanwhile, the behaviours of contact angles (CAs) in the H2+H2O+silica system are noticeably different from those in the H2+H2O+kerogen system. The H2O CAs for the H2+H2O+silica and H2+H2O+kerogen systems increase with pressure and decrease with temperature. However, the influence of temperature and pressure on these CAs is less pronounced for the H2+H2O+silica system at low temperatures. The behaviours of CAs were understood based on the variations of IFTs in the H2+H2O system (fluid-fluid interaction) and adhesion tensions (fluid-solid interaction). Furthermore, the analysis of the atomic density distributions indicates that the presence of H2 in between the H2O and the silica/kerogen is almost negligible. Nevertheless, the adsorption of H2O on the silica outside the H2O is strong, while less H2O adsorption is seen on the kerogen.