The effect of natural sand grains and associated mineral changes on methane hydrate formation

The highest gas hydrate saturations and possible energy resource targets are bound to sandy sediments. However, investigations regarding the influence of natural sand particles on gas hydrate formation are rare and almost missing with regards to the particle size effect of different grain size ranges of sand on the gas hydrate kinetics. Comparative investigations commonly use arbitrary sized sands and clay minerals. In addition, sand grains are often represented using glass beads or pure quartz grains instead of natural samples where additional effects from mineral compositions and coatings might occur. However, understanding the kinetics of hydrate formation in sand forms yet another foundation for a successful scale-up model of the production of natural gas hydrate reservoirs, where reformation of hydrates may occur under non-equilibrium conditions.

We investigated the particle size effect of sand on methane hydrate formation kinetics using five different grain size ranges of Ottawa sand, a rather pure quartz sand. Conditions of the static and small-volume experiments were far within the methane hydrate stability (7 MPa/1°C). Pressure and temperature recording as well as microscopic and Raman spectroscopic observations could verify methane hydrate formation and growth.

For the chosen experimental setup there is a strong particle size effect on the kinetics of gas hydrate formation. A high concentration of the finest range (< 125µm) has led to an explicitly faster hydrate formation compared to coarser sand or a small fraction of fine particles diluted in coarse sand grains. This is in contrast to the decrease of thermodynamic driving forces in the presence of fine sized particles given equilibrium conditions. The promoting kinetic effect of the mineral surface properties might be related to the impact of the surface area as well as crystal structures, and/or electrical charge since small fractions of natural sands commonly encounter different mineral compositions compared to the coarser, quartz rich sand fraction. Therefore, additional investigations focus on the influence of the different minerals on the hydrate formation process.