Unraveling the Role of Natural Sediments in sII Mixed Gas Hydrate Formation: An Experimental Study.

Considering the ever-increasing interests in natural gas hydrates, a better and more precise knowledge of how host sediments interact with hydrates and affect the formation process is crucial. Yet less is reported for the effects of sediments on structure II hydrate formation with complex guest compositions. In this study, experimental simulations were performed based on the natural reservoir in Qilian Mountain permafrost in China (QMP) due to its unique properties.

Influence of Gas Supply Changes on the Formation Process of Complex Mixed Gas Hydrates.

Natural gas hydrate occurrences contain predominantly methane; however, there are increasing reports of complex mixed gas hydrates and coexisting hydrate phases. Changes in the feed gas composition due to the preferred incorporation of certain components into the hydrate phase and an inadequate gas supply is often assumed to be the cause of coexisting hydrate phases. This could also be the case for the gas hydrate system in Qilian Mountain permafrost (QMP), which is mainly controlled by pores and fractures with complex gas compositions.

A new high-pressure cell for systematic in situ investigations of micro-scale processes in gas hydrates using confocal micro-Raman spectroscopy.

Natural gas hydrates are ice-like solids composed of gas and water molecules. They are found worldwide at all continental margins as well as in permafrost regions. Depending on the source of the enclathrated gas molecules, natural gas hydrates may occur as coexisting phases with different structures containing predominantly CH, but also a variety of hydrocarbons, CO or HS.

"Ester"-A new ring-shear-apparatus for hydrate-bearing sediments.

We developed a new thermostated ring-shear-apparatus for investigation on hydrate- or ice-bearing sediments. A fluid inlet at the bottom of the static part of the cell and a fluid outlet at the top of the rotating half-cell allow exchanging and pressurizing the pore fluid in the sample cell to a certain value below the pressure providing the normal load that is applied hydraulically via a seal disk using a syringe pump. The volume change in the sample can be derived from the volume received or injected by the pump.

Gas hydrates in sustainable chemistry.

Gas hydrates have received considerable attention due to their important role in flow assurance for the oil and gas industry, their extensive natural occurrence on Earth and extraterrestrial planets, and their significant applications in sustainable technologies including but not limited to gas and energy storage, gas separation, and water desalination. Given not only their inherent structural flexibility depending on the type of guest gas molecules and formation conditions, but also the synthetic effects of a wide range of chemical additives on their properties, these variabilities could be exploited to optimise the role of gas hydrates. This includes increasing their industrial applications, understanding and utilising their role in Nature, identifying potential methods for safely extracting natural gases stored in naturally occurring hydrates within the Earth, and for developing green technologies.

A cylindrical electrical resistivity tomography array for three-dimensional monitoring of hydrate formation and dissociation.

The LArge Reservoir Simulator (LARS) was developed to investigate various processes during gas hydrate formation and dissociation under simulated in situ conditions of relatively high pressure and low temperature (close to natural conditions). To monitor the spatial hydrate distribution during hydrate formation and the mobility of the free gas phase generated during hydrate dissociation, a cylindrical Electrical Resistivity Tomography (ERT) array was implemented into LARS. The ERT contains 375 electrodes, arranged in 25 circular rings featuring 15 electrodes each.

Cage occupancy and structural changes during hydrate formation from initial stages to resulting hydrate phase.

Hydrate formation processes and kinetics are still not sufficiently understood on a molecular level based on experimental data. In particular, the cavity formation and occupancy during the initial formation and growth processes of mixed gas hydrates are rarely investigated. In this study, we present the results of our time-depending Raman spectroscopic measurements during the formation of hydrates from ice and gases or gas mixtures such as CH4, CH4-CO2, CH4-H2S, CH4-C3H8, CH4-iso-C4H10, and CH4-neo-C5H12 at constant pressure and temperature conditions and constant composition of the feed gas phase.

The influence of SO2 and NO2 impurities on CO2 gas hydrate formation and stability.

The sequestration of industrially emitted CO(2) in gas hydrate reservoirs has been recently discussed as an option to reduce atmospheric greenhouse gas. This CO(2) contains, despite much effort to clean it, traces of impurities such as SO(2) and NO(2) . Here, we present results of a pilot study on CO(2) hydrates contaminated with 1% SO(2) or 1% NO(2) and show the impact on hydrate formation and stability.

A high-pressure cell for kinetic studies on gas hydrates by powder x-ray diffraction.

A new high-pressure-low-temperature cell was developed for in situ observations of gas hydrates by powder x-ray diffraction. The experimental setup allows investigating hydrate formation and dissociation as well as transformation processes between different hydrate crystal structures as a function of pressure, temperature, and feed gas composition. Due to a continuous gas flow, the composition of the gas phase is kept constant during the whole experiment.

Dissociation enthalpies of synthesized multicomponent gas hydrates with respect to the guest composition and cage occupancy.

This study presents the influences of additional guest molecules such as C2H6, C3H8, and CO2 on methane hydrates regarding their thermal behavior. For this purpose, the onset temperatures of decomposition as well as the enthalpies of dissociation were determined for synthesized multicomponent gas hydrates in the range of 173-290 K at atmospheric pressure using a Calvet heat-flow calorimeter. Furthermore, the structures and the compositions of the hydrates were obtained using X-ray diffraction and Raman spectroscopy as well as hydrate prediction program calculations.

Phase transitions in mixed gas hydrates: experimental observations versus calculated data.

This paper presents the phase behavior of multicomponent gas hydrate systems formed from primarily methane with small amounts of ethane and propane. Experimental conditions were typically in a pressure range between 1 and 6 MPa, and the temperature range was between 260 and 290 K. These multicomponent systems have been investigated using a variety of techniques including microscopic observations, Raman spectroscopy, and X-ray diffraction.